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Guo C, Yu C, Zhang Y, Li Y, Wan J, Wang L, Pan J. Boosting micropollutants removal over bimetallic Fe-Mo catalyst via peracetic acid activation: Mo doping enhanced generation of reactive oxygen species. JOURNAL OF HAZARDOUS MATERIALS 2025; 491:138013. [PMID: 40122006 DOI: 10.1016/j.jhazmat.2025.138013] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/30/2024] [Revised: 03/07/2025] [Accepted: 03/18/2025] [Indexed: 03/25/2025]
Abstract
Herein, a range of bimetallic Fe-Mo catalysts (FexMoy@C) were successfully synthesized to explore the effect of Mo doping on the activity of Fe-based catalyst (Fe@C) for peracetic acid (PAA) activation. Mo doped during Fe@C preparation process introduced more low-valent metal species into Fe@C with the potential to promote PAA activation and Fe(III)/Fe(II) cycling. Compared to single Fe catalyst, Fe4Mo1@C exhibited outstanding performance in PAA activation for ultrafast degradation of bisphenol A (BPA), with the degradation rate of 0.88 min-1, which exceeded most reported heterogeneous catalysts. Mechanism results indicated that the Mo doping promoted the generation of reactive species and accelerated Fe(III)/Fe(II) conversion on the surface of Fe4Mo1@C to ensure the continuous PAA activation. Further analysis revealed that incorporated Mo not only promoted electron transfer and accelerated transform of Fe(III) to Fe(II), but also lowered the energy barrier for PAA activation. Moreover, the toxicity of BPA and its intermediates could be effectively reduced in Fe4Mo1@C/PAA system, guaranteeing the safety of treatment process. This study clarified the mechanism of Mo doping to enhance the Fe-based catalysts activity for organic micropollutant degradation, and the new insights obtained would further promote the application of bimetallic catalysts in PAA-based advanced oxidation processes.
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Affiliation(s)
- Congcong Guo
- College of Environment and Safety Engineering, Key Laboratory of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
| | - Chao Yu
- College of Environment and Safety Engineering, Key Laboratory of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
| | - Yiran Zhang
- College of Environment and Safety Engineering, Key Laboratory of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
| | - Yuyou Li
- College of Environment and Safety Engineering, Key Laboratory of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
| | - Jun Wan
- College of Environment and Safety Engineering, Key Laboratory of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
| | - Lei Wang
- College of Environment and Safety Engineering, Key Laboratory of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
| | - Jingwen Pan
- College of Environment and Safety Engineering, Key Laboratory of Eco-chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
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2
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Long L, Mao Y, Liu L, Chen Y, Shao Q, Liu Z, Xie P. Prolonged degradation of organic contaminants by Fe(II)/peracetic acid: Unraveling the roles of coexisting H 2O 2 and pH. JOURNAL OF HAZARDOUS MATERIALS 2025; 489:137567. [PMID: 39952124 DOI: 10.1016/j.jhazmat.2025.137567] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 10/29/2024] [Revised: 01/16/2025] [Accepted: 02/09/2025] [Indexed: 02/17/2025]
Abstract
The Fe(II)-activated peracetic acid (PAA) system is a promising advanced oxidation process for the removal of refractory organic pollutants. Although previous studies have reported its mechanism, highlighting the rapid generation of Fe(IV) and radicals (R-O•) within one second, the effects of coexisting H2O2 and pH remain unclear. In this study, we explored these factors in greater detail. In the initial fast stage, the Fe(IV) yield was found to be slightly influenced by water matrix, suggesting a superiority of Fe(II)/PAA in producing Fe(IV) under real water background. Moreover, our findings confirm that coexisting H2O2 is activated by the residual Fe(II) after PAA consumption, broadening the applicability for pollutants removal. The fast stage tends to degrade electron-rich pollutants, while the slow stage can degrade electron-deficient and electron-rich pollutants. During this process, in-situ formed Fe(III) exhibited negligible reactivity towards PAA or H2O2. As the pH increased from 3.0 to 7.0, the overall production of Fe(IV) and •OH drastically declined, reducing the system's oxidizing capacity. Density functional theory (DFT) calculations further suggest that deprotonation at higher pH levels theoretically hinders PAA decomposition by Fe(II). Using sulfamethoxazole (SMX) as a model pollutant, we observed that acidic conditions improved both pollutant removal efficiency and the formation of less toxic by-products. This study significantly advances the understanding of the decontamination mechanisms in the Fe(II)/PAA system.
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Affiliation(s)
- Liying Long
- School of Civil Engineering, Wuhan University, Wuhan 430072, China
| | - Yuxin Mao
- School of Civil Engineering, Wuhan University, Wuhan 430072, China
| | - Lu Liu
- School of Civil Engineering, Wuhan University, Wuhan 430072, China
| | - Yiqun Chen
- School of Civil Engineering, Wuhan University, Wuhan 430072, China.
| | - Qing Shao
- School of Civil Engineering, Wuhan University, Wuhan 430072, China
| | - Zizheng Liu
- School of Civil Engineering, Wuhan University, Wuhan 430072, China.
| | - Pengchao Xie
- School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
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3
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Tang Y, Jiang B, Zhu T, Sun Z. Novel CoFe-supported UiO-66-derived ZrO 2 for rapid activation of peracetic acid for sulfamethoxazole degradation. ENVIRONMENTAL RESEARCH 2025; 274:121329. [PMID: 40057109 DOI: 10.1016/j.envres.2025.121329] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 01/06/2025] [Revised: 03/05/2025] [Accepted: 03/05/2025] [Indexed: 03/15/2025]
Abstract
The leaching of toxic metals is still problematic for heterogeneous metal catalysts in activating peracetic acid (PAA). Herein, CoFe/U-ZrO2 was synthesized by loading CoFe onto the metal-organic framework (UiO-66) derived ZrO2 (U-ZrO2) for PAA activation. The high porosity and specific surface area of UiO-66 enable efficient embedding and uniform dispersion of CoFe particles into pore channels. The supported material effectively activates PAA and significantly reduces Co leaching. CoFe/U-ZrO2-PAA system shows a removal efficiency of sulfamethoxazole reaching 98.9% within 10 min with Co leaching concentrations as low as 0.005 mg/L (equivalent to 1.4% of CoFe-PAA system). Quenching experiments, probe experiments and electron paramagnetic resonance tests identify CH3C(O)OO· as the dominant radical species. The CoFe/U-ZrO2-PAA system maintains high activity in actual water bodies and can resist the interference of HPO42-, Cl-, SO42-, NO3- and humic acid except for the inhibitory effect of HCO3-. The system also displays good stability and high degradability to different pollutants, maintaining consistently outstanding degradation efficiency in the flow-through experiment. Overall, the environmentally friendly, good efficiency, and high stability of the CoFe/U-ZrO2-PAA system makes it potential for broad applications in wastewater treatment.
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Affiliation(s)
- Yanfei Tang
- Department of Environmental Engineering, Beijing University of Technology, Beijing, 100124, PR China; National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China
| | - Bingyu Jiang
- Department of Environmental Engineering, Beijing University of Technology, Beijing, 100124, PR China; National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China
| | - Tong Zhu
- Department of Environmental Engineering, Beijing University of Technology, Beijing, 100124, PR China; National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China
| | - Zhirong Sun
- Department of Environmental Engineering, Beijing University of Technology, Beijing, 100124, PR China; National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China.
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4
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Ren Y, Li J, Liu C, Zhang W, Lai B. Switchable surface Fe II/III sites for water/sediment remediation through enhanced selective oxidation and ROS regulation: Performance, mechanism and application. JOURNAL OF HAZARDOUS MATERIALS 2025; 485:136799. [PMID: 39675082 DOI: 10.1016/j.jhazmat.2024.136799] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 09/19/2024] [Revised: 11/15/2024] [Accepted: 12/04/2024] [Indexed: 12/17/2024]
Abstract
Selective oxidation relying on high-valent iron-oxo species (Fe(IV/V)) is a promising way of effective organic decontamination. However, Fe(IV/V) formation and further purposeful reinforcement production are commonly insufficient and unsustainable. Herein, cerium (Ce) modification strategy was adopted for efficient micropollutants removal through boosting Fe(IV/V) generation. Kinetic rate of sulfamethoxazole (SMX) removal through peracetic acid (PAA) activation by FeCe-O-CN is 4.1-fold of that without Ce doping. Ce modification lowered energy barrier of the key reaction pathway (*OH→*O) during Fe(IV/V) formation and accelerated the exposure of the surface FeII site for Fe(IV) production. Steady-state concentration of Fe(IV) and Fe(V) in FeCe-O-CN/PAA process is 2.5 × 10-8 and 9.7 × 10-11 M with its corresponding contribution to SMX removal as 64 % and 36 %. Not only intensified SMX removal, Ce modification significantly reduced the toxicity of transformation products. Furthermore, FeCe-O-CN/PAA system satisfies favorable decontaminant in long-term runs, anti-interference, and significantly alleviated bioaccumulation in plants. This study provides a new insight into the association between Ce modification and Fe(IV/V) generation in PAA activation and offered a feasible way for enhanced selective oxidation.
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Affiliation(s)
- Yi Ren
- State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, Sichuan 610065, China; College of Water Resource & Hydropower, Sichuan University, Chengdu 610065, China
| | - Jun Li
- State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, Sichuan 610065, China; College of Water Resource & Hydropower, Sichuan University, Chengdu 610065, China.
| | - Chao Liu
- State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, Sichuan 610065, China; College of Water Resource & Hydropower, Sichuan University, Chengdu 610065, China
| | - Weiming Zhang
- State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
| | - Bo Lai
- State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, Sichuan 610065, China; School of Architecture and Environment, Sichuan University, Chengdu 610065, China.
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5
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Zhuang W, Zhao X, Luo Q, Lv X, Zhang Z, Zhang L, Sui M. Task decomposition strategy based on machine learning for boosting performance and identifying mechanisms in heterogeneous activation of peracetic acid process. WATER RESEARCH 2024; 267:122521. [PMID: 39357159 DOI: 10.1016/j.watres.2024.122521] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 06/24/2024] [Revised: 08/25/2024] [Accepted: 09/24/2024] [Indexed: 10/04/2024]
Abstract
Heterogeneous activation of peracetic acid (PAA) process is a promising method for removing organic pollutants from water. Nevertheless, this process is constrained by several complex factors, such as the selection of catalysts, optimization of reaction conditions, and identification of mechanism. In this study, a task decomposition strategy was adopted by combining a catalyst and reaction condition optimization machine learning (CRCO-ML) model and a mechanism identification machine learning (MI-ML) model to address these issues. The Categorical Boosting (CatBoost) model was identified as the best-performing model for the dataset (1024 sets and 7122 data points) in this study, achieving an R2 of 0.92 and an RMSE of 1.28. Catalyst composition, PAA dosage, and catalyst dosage were identified as the three most important features through SHAP analysis in the CRCO-ML model. The HCO3- is considered the most influential water matrix affecting the k value. The errors between all reverse experiment results and the predictions of the CRCO-ML and MI-ML models were <10 % and 15 %, respectively. This interdisciplinary work provides novel insights into the design and application of the heterogeneous activation of PAA process, significantly contributing to the rapid development of this technology.
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Affiliation(s)
- Wei Zhuang
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
| | - Xiao Zhao
- Academy for Engineering and Technology, Fudan University, Shanghai 200000, China.
| | - Qianqian Luo
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
| | - Xinyuan Lv
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
| | - Zhilin Zhang
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
| | - Lihua Zhang
- Academy for Engineering and Technology, Fudan University, Shanghai 200000, China
| | - Minghao Sui
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
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6
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Wang YX, Liu XL, Li WQ, Wang YR, Li KW, Pan ZC, Mu Y. Boosting bioelectricity generation in bioelectrochemical systems with nitrogen-doped three-dimensional graphene aerogel anode. WATER RESEARCH 2024; 265:122244. [PMID: 39146657 DOI: 10.1016/j.watres.2024.122244] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 06/09/2024] [Revised: 07/26/2024] [Accepted: 08/08/2024] [Indexed: 08/17/2024]
Abstract
Bioelectricity generation by electrochemically active bacteria has become particularly appealing due to its vast potential in energy production, pollution treatment, and biosynthesis. However, developing high-performance anodes for bioelectricity generation remains a significant challenge. In this study, a highly efficient three-dimensional nitrogen-doped macroporous graphene aerogel anode with a nitrogen content of approximately 4.38 ± 0.50 at% was fabricated using hydrothermal method. The anode was successfully implemented in bioelectrochemical systems inoculated with Shewanella oneidensis MR-1, resulting in a significantly higher anodic current density (1.0 A/m2) compared to the control one. This enhancement was attributed to the greater biocapacity and improved extracellular electron transfer efficiency of the anode. Additionally, the N-doped aerogel anode demonstrated excellent performance in mixed-culture inoculated bioelectrochemical systems, achieving a high power density of 4.2 ± 0.2 W/m², one of the highest reported for three-dimensional carbon-based bioelectrochemical systems to date. Such improvements are likely due to the good biocompatibility of the N-doped aerogel anode, increased extracellular electron transfer efficiency at the bacteria/anode interface, and selectively enrichment of electroactive Geobacter soli within the NGA anode. Furthermore, based on gene-level Picrust2 prediction results, N-doping significantly upregulated the conductive pili-related genes of Geobacter in the three-dimensional anode, increasing the physical connection channels of bacteria, and thus strengthening the extracellular electron transfer process in Geobacter.
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Affiliation(s)
- Yi-Xuan Wang
- Key Laboratory of Environmental Remediation and Ecological Health, Ministry of Industry and Information Technology, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, Jiangsu 210094, PR China; CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei, Anhui 230026, China; Postdoctoral Research Station of Haitian Water Group Co., Ltd, Chengdu, Sichuan 610041, China
| | - Xiao-Li Liu
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei, Anhui 230026, China
| | - Wen-Qiang Li
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei, Anhui 230026, China
| | - Yi-Ran Wang
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei, Anhui 230026, China
| | - Ke-Wan Li
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei, Anhui 230026, China
| | - Zhi-Cheng Pan
- Postdoctoral Research Station of Haitian Water Group Co., Ltd, Chengdu, Sichuan 610041, China
| | - Yang Mu
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei, Anhui 230026, China.
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7
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Zou R, Yang W, Rezaei B, Tang K, Guo K, Zhang P, Keller SS, Andersen HR, Zhang Y. Activation of peracetic acid by electrodes using biogenic electrons: A novel energy- and catalyst-free process to eliminate pharmaceuticals. WATER RESEARCH 2024; 261:122065. [PMID: 39002421 DOI: 10.1016/j.watres.2024.122065] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 04/23/2024] [Revised: 06/22/2024] [Accepted: 07/08/2024] [Indexed: 07/15/2024]
Abstract
Peracetic acid (PAA) has received increasing attention as an alternative oxidant for wastewater treatment. However, existing processes for PAA activation to generate reactive species typically require external energy input (e.g., electrically and UV-mediated activation) or catalysts (e.g., Co2+), inevitably increasing treatment costs or introducing potential new contaminants that necessitate additional removal. In this work, we developed a catalyst-free, self-sustaining bioelectrochemical approach within a two-chamber bioelectrochemical system (BES), where a cathode electrode in-situ activates PAA using renewable biogenic electrons generated by anodic exoelectrogens (e.g., Geobacter) degrading biodegradable organic matter (e.g., acetic acid) in wastewater at the anode. This innovative BES-PAA technique achieved 98 % and 81 % removal of 2 µM sulfamethoxazole (SMX) in two hours at pH 2 (cation exchange membrane) and pH 6 (bipolar membrane) using 100 μM PAA without external voltage. Mechanistic studies, including radical quenching, molecular probe validation, electron spin resonance (ESR) experiments, and density functional theory (DFT) calculations, revealed that SMX degradation was driven by reactive species generated via biogenic electron-mediated OO cleavage of PAA, with CH3C(O)OO• contributing 68.1 %, •OH of 18.4 %, and CH3C(O)O• of 9.4 %, where initial formation of •OH and CH3C(O)O• rapidly reacts with PAA to produce CH3C(O)OO•. The presence of common water constituents such as anions (e.g., Cl-, NO3-, and H2PO4-) and humic acid (HA) significantly hinders SMX removal via the BES-PAA technique, whereas CO32- and HCO3- ions have a comparatively minor impact. Additionally, the study investigated the removal of various pharmaceuticals present in secondary treated municipal wastewater, attributing differences in removal efficiency to the selective action of CH3C(O)OO•. This research demonstrates a novel PAA activation method that is ecologically benign, inexpensive, and capable of overcoming catalyst deactivation and secondary pollution issues.
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Affiliation(s)
- Rusen Zou
- Department of Environmental & Ressource Engineering, Technical University of Denmark, DK-2800, Lyngby, Denmark
| | - Wenqiang Yang
- Department of Physics, Technical University of Denmark, Lyngby, DK 2800, Denmark
| | - Babak Rezaei
- National Centre for Nano Fabrication and Characterization, DTU Nanolab, Technical University of Denmark, 2800 Kgs., Lyngby, Denmark
| | - Kai Tang
- Department of Environmental & Ressource Engineering, Technical University of Denmark, DK-2800, Lyngby, Denmark
| | - Kuangxin Guo
- Department of Environmental & Ressource Engineering, Technical University of Denmark, DK-2800, Lyngby, Denmark
| | - Pingping Zhang
- School of Environment and Architecture, University of Shanghai for Science and Technology, Shanghai, 200093, PR China
| | - Stephan Sylvest Keller
- National Centre for Nano Fabrication and Characterization, DTU Nanolab, Technical University of Denmark, 2800 Kgs., Lyngby, Denmark
| | - Henrik Rasmus Andersen
- Department of Environmental & Ressource Engineering, Technical University of Denmark, DK-2800, Lyngby, Denmark
| | - Yifeng Zhang
- Department of Environmental & Ressource Engineering, Technical University of Denmark, DK-2800, Lyngby, Denmark.
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8
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Lu B, Fang Z, Tsang PE. Key role of Phyllanthus emblica L. fruit extract promotes ZVI/H 2O 2 process: rich titratable acid, suitable chelating ability, and antioxidant capacity. ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH INTERNATIONAL 2024; 31:55422-55436. [PMID: 39230818 DOI: 10.1007/s11356-024-34644-5] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Grants] [Track Full Text] [Subscribe] [Scholar Register] [Received: 09/25/2023] [Accepted: 08/02/2024] [Indexed: 09/05/2024]
Abstract
Phyllanthus emblica L. fruit extract (PFE) was introduced to improve ZVI/H2O2 technology, and the efficiency and mechanism of PFE promoting ZVI/H2O2 technology were explored. With the introduction of PFE, the Norfloxacin (NOR) removal rate and kobs of the process were improved by 41.17% and 5.08 times, respectively. In the ZVI/H2O2/PFE process, the degradation of NOR by the attack of ROS is the main pathway for decontamination and is dominated by the heterogeneous reaction on the catalyst surface. PFE contains 13.92 g/L titratable acid and has good complexing ability and antioxidant ability. The mechanism of PFE promoting ZVI/H2O2 technology was based on lowering the pH, complemented by chelation and antioxidant capacity. With the introduction of PFE, the utilization rate of the reagent was significantly increased (7.56 times for ZVI and 3.21 times for H2O2), the applicable pH range was widened (6-9) and the iron sludge was reduced (32.80%). Meanwhile, the concept of UPR is proposed for the first time. The result is the key role to the selection of green promoters in the ZVI/H2O2 process depends on the abundance of titratable acid, followed by a certain chelating ability and antioxidant capacity.
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Affiliation(s)
- Baizhou Lu
- School of Environment, South China Normal University, Guangzhou, 510006, China
- Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou, 510006, China
| | - Zhanqiang Fang
- School of Environment, South China Normal University, Guangzhou, 510006, China.
- Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou, 510006, China.
- Normal University (Qingyuan) Environmental Remediation Technology Co., Ltd, Qingyuan, 511500, China.
| | - Pokeung Eric Tsang
- Department of Science and Environmental Studies, The Education University of Hong Kong, Hong Kong, 00852, China
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Dong J, Dong H, Xiao J, Li L, Huang D, Zhao M. Enhanced Degradation of Micropollutants in a Peracetic Acid/Mn(II) System with EDDS: An Investigation of the Role of Mn Species. ENVIRONMENTAL SCIENCE & TECHNOLOGY 2024; 58:12179-12188. [PMID: 38913078 DOI: 10.1021/acs.est.4c00901] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Indexed: 06/25/2024]
Abstract
Extensive research has been conducted on the utilization of a metal-based catalyst to activate peracetic acid (PAA) for the degradation of micropollutants (MPs) in water. Mn(II) is a commonly employed catalyst for homogeneous advanced oxidation processes (AOPs), but its catalytic performance with PAA is poor. This study showed that the environmentally friendly chelator ethylenediamine-N,N'-disuccinic acid (EDDS) could greatly facilitate the activation of Mn(II) in PAA for complete atrazine (ATZ) degradation. In this process, the EDDS enhanced the catalytic activity of manganese (Mn) and prevented disproportionation of transient Mn species, thus facilitating the decay of PAA and mineralization of ATZ. By employing electron spin resonance detection, quenching and probe tests, and 18O isotope-tracing experiments, the significance of high-valent Mn-oxo species (Mn(V)) in the Mn(II)-EDDS/PAA system was revealed. In particular, the involvement of the Mn(III) species was essential for the formation of Mn(V). Mn(III) species, along with singlet oxygen (1O2) and acetyl(per)oxyl radicals (CH3C(O)O•/CH3C(O)OO•), also contributed partially to ATZ degradation. Mass spectrometry and density functional theory methods were used to study the transformation pathway and mechanism of ATZ. The toxicity assessment of the oxidative products indicated that the toxicity of ATZ decreased after the degradation reaction. Moreover, the system exhibited excellent interference resistance toward various anions and humid acid (HA), and it could selectively degrade multiple MPs.
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Affiliation(s)
- Jie Dong
- College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China
- Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha, Hunan 410082, China
| | - Haoran Dong
- College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China
- Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha, Hunan 410082, China
| | - Junyang Xiao
- College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China
- Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha, Hunan 410082, China
| | - Long Li
- College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China
- Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha, Hunan 410082, China
| | - Daofen Huang
- College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China
- Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha, Hunan 410082, China
| | - Mengxi Zhao
- College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China
- Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha, Hunan 410082, China
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10
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An L, Kong X, Jiang M, Li W, Lv Q, Hou X, Liu C, Su P, Ma J, Yang T. Photo-assisted natural chalcopyrite activated peracetic acid for efficient micropollutant degradation. WATER RESEARCH 2024; 257:121699. [PMID: 38713937 DOI: 10.1016/j.watres.2024.121699] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 12/17/2023] [Revised: 04/01/2024] [Accepted: 04/29/2024] [Indexed: 05/09/2024]
Abstract
The effective activation of natural chalcopyrite (CuFeS2) on peracetic acid (PAA) to remove organic micropollutants was studied under visible light irradiation. Results showed than an effective sulfamethoxazole (SMX) degradation (95.0 %) was achieved under visible light irradiation for 30 min at pH 7.0. Quenching experiments, electron spin resonance analysis, and LC/MS spectrum demonstrated that HO• and CH3C(O)OO• were the main reactive species for SMX degradation, accounting for 43.3 % and 56.7 % of the contributions, respectively. Combined with X-ray photoelectron spectroscopy analysis, the photoelectrons generated on CuFeS2 activated by visible light enhanced the Fe3+/Fe2+ and Cu2+/Cu+ cycles on the surface, thereby activating PAA to generate HO•/CH3C(O)OO•. The removal rate of SMX decreased with the increase in wavelengths, due to the formation of low energy photons at longer wavelengths. Besides, the optimal pH for degradation of SMX by CuFeS2/PAA/Vis-LED process was neutral, which was attributed to the increasing easily activated anionic form of PAA during the increase in pH and the depletion of Fe species at alkaline conditions. Cl-, HCO3-, and HA slightly inhibited SMX degradation because of reactive species being quenched and/or shielding effect. Furthermore, the degradation efficiency of different pollutants by CuFeS2/PAA/Vis-LED was also measured, and the removal efficiency was different owing to the selectivity of CH3C(O)OO•. Finally, the process exhibited good applicability in real waters. Overall, this study provides new insight into visible light-catalyzed activation of PAA and suggests on further exploration of the intrinsic activation mechanism of PAA.
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Affiliation(s)
- Linqian An
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China
| | - Xiujuan Kong
- Center of Water Resources and Environment, School of Civil Engineering, Sun Yat-Sen University, Guangzhou 510275, China
| | - Maoju Jiang
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China
| | - Wenqi Li
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China
| | - Qixiao Lv
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China
| | - Xiangyang Hou
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China
| | - Chenlong Liu
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China
| | - Peng Su
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China
| | - Jun Ma
- State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150090, China
| | - Tao Yang
- School of Environmental and Chemical Engineering, Wuyi University, Jiangmen 529020, Guangdong Province, China; Institute of Carbon Peaking and Carbon Neutralization, Wuyi University, Jiangmen 529020, Guangdong Province, China.
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11
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Ning R, Dong Y, Yang SR, Yang S, Zhou P, Xiong Z, Pan ZC, He CS, Lai B. Fe-N co-doped biochar derived from biomass waste triggers peracetic acid activation for efficient water decontamination. JOURNAL OF HAZARDOUS MATERIALS 2024; 470:134139. [PMID: 38555674 DOI: 10.1016/j.jhazmat.2024.134139] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 01/05/2024] [Revised: 03/04/2024] [Accepted: 03/24/2024] [Indexed: 04/02/2024]
Abstract
In this study, the porous carbon material (FeN-BC) with ultra-high catalytic activity was obtained from waste biomass through Fe-N co-doping. The prominent degradation rate (> 96.8%) of naproxen (NAP) was achieved over a wide pH range (pH 3.0-9.0) in FeN-BC/PAA system. Unlike previously reported iron-based peracetic acid (PAA) systems with •OH or RO• as the dominated reactive species, the degradation of contaminants was attributed to singlet oxygen (1O2) produced by organic radicals (RO•) decomposition, which was proved to be thermodynamically feasible and favorable by theoretical calculations. Combining the theoretical calculations, characteristic and experimental analysis, the synergistic effects of Fe and N were proposed and summarized as follows: i) promoted the formation of extensive defects and Fe0 species that facilitated electron transfer between FeN-BC and PAA and continuous Fe(II) generation; ii) modified the specific surface area (SSA) and the isoelectric point of FeN-BC in favor of PAA adsorption on the catalyst surface. This study provides a strategy for waste biomass reuse to construct a heterogeneous catalyst/PAA system for efficient water purification and reveals the synergistic effects of typical metal-heteroatom for PAA activation.
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Affiliation(s)
- Ruyan Ning
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Yudan Dong
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Shu-Run Yang
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Shuai Yang
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Peng Zhou
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Zhaokun Xiong
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Zhi-Cheng Pan
- State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China; Water Safety and Water Pollution Control Engineering Technology Research Center in Sichuan Province, Haitian Water Group, Chengdu 610041, China
| | - Chuan-Shu He
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
| | - Bo Lai
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
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12
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Zhou C, Sui M, Guo Y, Du S. Enhancing Fenton-like reaction through a multifunctional molybdenum disulfide film coating on nano zero valent iron surface (MoS 2@nZVI): Collaboration of radical and non-radical pathways. THE SCIENCE OF THE TOTAL ENVIRONMENT 2024; 920:170818. [PMID: 38342461 DOI: 10.1016/j.scitotenv.2024.170818] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 12/10/2023] [Revised: 01/17/2024] [Accepted: 02/06/2024] [Indexed: 02/13/2024]
Abstract
In this study, we synthesized nano zero-valent iron incorporated with a multifunctional molybdenum disulfide film (MoS2@nZVI). The material exhibited a 100.00 % removal efficiency for sulfamethoxazole (SMX) and achieved a kobs of 0.4485 min-1 within 10 min. The excellent degradation performance can be attributed to the incorporation of the MoS2 film, which facilitated Fe2+ regeneration. Simultaneously, the MoS2 film assisted in proton accumulation and electron transfer, thereby amplifying the efficiency of SMX degradation across a wide pH range. Comprehensive experimental examinations and characterizations confirmed the selectivity and stability of the MoS2@nZVI catalysts, encompassing both degradation efficiency and structural stability. Interestingly, the MoS2@nZVI/PMS system for SMX degradation significantly involved a non-radical mechanism (1O2), along with radicals (SO4·-, ·OH, and O2·-). The direct oxidation of PMS by Fe2+ not only facilitated the generation of ·OH and SO4·- but also actively engaged in a reaction with O2, leading to the production of O2·-. The primary pathway for 1O2 production was established through the interplay between Mo6+ and O2·-, in conjunction with the direct electron transfer (DET) mechanism between PMS and SMX. The contributions of these active species to SMX degradation occurred in the following precedence: SO4·- > 1O2 > ·OH > O2·-. Notably, the primary pathways for radicals and non-radicals were studied during separate reaction periods. This investigation proposed a promising approach for mitigating pharmaceutical pollutants using a transition metal sulfide-modified nZVI catalyst.
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Affiliation(s)
- Chundi Zhou
- State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, People's Republic of China
| | - Minghao Sui
- State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, People's Republic of China.
| | - Yali Guo
- State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, People's Republic of China
| | - Songhang Du
- State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, People's Republic of China
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13
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Sciscenko I, Vione D, Minella M. Infancy of peracetic acid activation by iron, a new Fenton-based process: A review. Heliyon 2024; 10:e27036. [PMID: 38495153 PMCID: PMC10943352 DOI: 10.1016/j.heliyon.2024.e27036] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Figures] [Journal Information] [Subscribe] [Scholar Register] [Received: 02/07/2024] [Revised: 02/22/2024] [Accepted: 02/22/2024] [Indexed: 03/19/2024] Open
Abstract
The exacerbated global water scarcity and stricter water directives are leading to an increment in the recycled water use, requiring the development of new cost-effective advanced water treatments to provide safe water to the population. In this sense, peracetic acid (PAA, CH3C(O)OOH) is an environmentally friendly disinfectant with the potential to challenge the dominance of chlorine in large wastewater treatment plants in the near future. PAA can be used as an alternative oxidant to H2O2 to carry out the Fenton reaction, and it has recently been proven as more effective than H2O2 towards emerging pollutants degradation at circumneutral pH values and in the presence of anions. PAA activation by homogeneous and heterogeneous iron-based materials generates - besides HO• and FeO2+ - more selective CH3C(O)O• and CH3C(O)OO• radicals, slightly scavenged by typical HO• quenchers (e.g., bicarbonates), which extends PAA use to complex water matrices. This is reflected in an exponential progress of iron-PAA publications during the last few years. Although some reviews of PAA general properties and uses in water treatment were recently published, there is no account on the research and environmental applications of PAA activation by Fe-based materials, in spite of its gratifying progress. In view of these statements, here we provide a holistic review of the types of iron-based PAA activation systems and analyse the diverse iron compounds employed to date (e.g., ferrous and ferric salts, ferrate(VI), spinel ferrites), the use of external ferric reducing/chelating agents (e.g., picolinic acid, l-cysteine, boron) and of UV-visible irradiation systems, analysing the mechanisms involved in each case. Comparison of PAA activation by iron vs. other transition metals (particularly cobalt) is also discussed. This work aims at providing a thorough understanding of the Fe/PAA-based processes, facilitating useful insights into its advantages and limitations, overlooked issues, and prospects, leading to its popularisation and know-how increment.
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Affiliation(s)
- Iván Sciscenko
- Departamento de Ingeniería Textil y Papelera, Universitat Politècnica de València, plaza Ferrándiz y Carbonell S/N, 03801, Alcoy, Spain
| | - Davide Vione
- Department of Chemistry, University of Turin, via Pietro Giuria 5, 10125, Turin, Italy
| | - Marco Minella
- Department of Chemistry, University of Turin, via Pietro Giuria 5, 10125, Turin, Italy
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14
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Cui T, Yan S, Ding Y, Lin S, Chen Q, Hou Y, Ding L, Wang H, Xu R. Chromium immobilization from wastewater via iron-modified hydrochar: Different iron fabricants and practicality assessment. ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY 2024; 274:116132. [PMID: 38471342 DOI: 10.1016/j.ecoenv.2024.116132] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/14/2023] [Revised: 02/06/2024] [Accepted: 02/18/2024] [Indexed: 03/14/2024]
Abstract
The recycling of industrial solid by-products such as red mud (RM) has become an urgent priority, due to their large quantities and lack of reutilization methods can lead to resource wastage. In this work, RM was employed to fabricate green hydrochar (HC) to prepare zero-valent iron (ZVI) modified carbonous materials, and conventional iron salts (IS, FeCl3) was applied as comparison, fabricated HC labeled as RM/HC and IS/HC, respectively. The physicochemical properties of these HC were comprehensively characterized. Further, hexavalent chromium (Cr(VI)) removal performance was assessed (375.66 and 337.19 mg/g for RM/HC and IS/HC, respectively). The influence of dosage and initial pH were evaluated, while isotherms, kinetics, and thermodynamics analysis were also conducted, to mimic the surface interactions. The stability and recyclability of adsorbents also verified, while the practical feasibility was assessed by bok choy-planting experiment. This work revealed that RM can be used as a high value and green fabricant for HC the effective removal of chromium contaminants from the wastewater.
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Affiliation(s)
- Ting Cui
- School of Energy and Environment Science, Yunnan Normal University, Kunming 650500, China
| | - Song Yan
- Agency on Rural Energy Management of Yunnan Province, Kunming 650500, China
| | - Yu Ding
- Rural Energy Workstation of Baoshan City, Baoshan 678000, China
| | - Shaopeng Lin
- Rural Energy Workstation of Baoshan City, Baoshan 678000, China
| | - Qiuliang Chen
- Rural Energy Workstation of Honghe City, Honghe 661000, China
| | - Ying Hou
- Agricultural Environmental Protection and Rural Energy Workstation of Luoping, Qvjing 655800, China
| | - Lin Ding
- National-Local Joint Engineering Research Center for Heavy Metal Pollutant Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, PR China
| | - Huabin Wang
- School of Energy and Environment Science, Yunnan Normal University, Kunming 650500, China; Agency on Rural Energy Management of Yunnan Province, Kunming 650500, China.
| | - Rui Xu
- School of Energy and Environment Science, Yunnan Normal University, Kunming 650500, China; Agency on Rural Energy Management of Yunnan Province, Kunming 650500, China.
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15
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Dai Y, Yang S, Wu L, Cao H, Chen L, Zhong Q, Xu C, He H, Qi C. Converting peracetic acid activation by Fe 3O 4 from nonradical to radical pathway via the incorporation of L-cysteine. JOURNAL OF HAZARDOUS MATERIALS 2024; 465:133303. [PMID: 38141297 DOI: 10.1016/j.jhazmat.2023.133303] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/01/2023] [Revised: 12/11/2023] [Accepted: 12/15/2023] [Indexed: 12/25/2023]
Abstract
Recently, peracetic acid (PAA) based Fenton (-like) processes have received much attention in water treatment. However, these processes are limited by the sluggish Fe(III)/Fe(II) redox circulation efficiency. In this study, L-cysteine (L-Cys), an environmentally friendly electron donor, was applied to enhance the Fe3O4/PAA process for the sulfamethoxazole (SMX) abatement. Surprisingly, the L-Cys incorporation was found not only to enhance the SMX degradation rate constant by 3.2 times but also to switch the Fe(IV) dominated nonradical pathway into the •OH dominated radical pathway. Experiment and theoretical calculation result elucidated -NH2, -SH, and -COOH of L-Cys can increase Fe solubilization by binding to the Fe sites of Fe3O4, while -SH of L-Cys can promote the reduction of bounded/dissolved Fe(III). Similar SMX conversion pathways driven by the Fe3O4/PAA process with or without L-Cys were revealed. Excessive L-Cys or PAA, high pH and the coexisting HCO3-/H2PO4- exhibit inhibitory effects on SMX degradation, while Cl- and humic acid barely affect the SMX removal. This work advances the knowledge of the enhanced mechanism insights of L-Cys toward heterogeneous Fenton (-like) processes and provides experimental data for the efficient treatment of sulfonamide antibiotics in the water treatment.
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Affiliation(s)
- Yinhao Dai
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China
| | - Shaogui Yang
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China; Suzhou Furong Environmental Engineering Co., Ltd, Suzhou 215500, PR China
| | - Leliang Wu
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China
| | - Hui Cao
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China
| | - Longjiong Chen
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China
| | - Qiang Zhong
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China
| | - Chenmin Xu
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China
| | - Huan He
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China
| | - Chengdu Qi
- School of Environment, Jiangsu Province Engineering Research Center of Environmental Risk Prevention and Emergency Response Technology, Jiangsu Engineering Lab of Water and Soil Eco-remediation, Nanjing Normal University, Nanjing 210023, PR China.
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16
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Lu B, Fang Z, Tsang PE. Effect and mechanism of norfloxacin removal by Eucalyptus leaf extract enhanced the ZVI/H 2O 2 process. THE SCIENCE OF THE TOTAL ENVIRONMENT 2024; 914:169820. [PMID: 38199363 DOI: 10.1016/j.scitotenv.2023.169820] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/07/2023] [Revised: 12/26/2023] [Accepted: 12/29/2023] [Indexed: 01/12/2024]
Abstract
The conventional ZVI/H2O2 technology suffers from poor reagent utilization, excess iron sludge generation, and strong low pH dependence. Therefore, eucalyptus leaf extract (ELE) was introduced to improve ZVI/H2O2 technology, and the efficacy and mechanism of ELE promoting ZVI/H2O2 technology were deeply explored. The results showed that the norfloxacin (NOR) removal and kobs of the ZVI/H2O2/ELE process were enhanced by 35.64 % and 3.27 times, respectively, compared to the ZVI/H2O2 process. In the ZVI/H2O2 process, the production of three reactive oxygen species (ROS: 1O2,·O2-,·OH) was effectively promoted by ELE so that the reaction efficacy was significantly enhanced. Moreover, the attack and degradation of pollutants by ROS was the main way to remove pollutants. With the introduction of ELE, the reactive sites on the catalyst appearance were increased to some extent, and the Fe(III)/Fe(II) cycle was improved. The analysis showed that ELE is rich in titratable acids and the ZVI/H2O2 technology is promoted mainly by lowering the pH of the process. In addition, the chelation of ELE and the reduction in pH by the ELE synergistically enhanced the ZVI/H2O2 technology, which significantly improved the reagent utilization (4.70 times for ZVI and 3.03 times for H2O2), broadened the pH range of the technology (6-9) and was able to effectively reduce the iron sludge contamination (30.33 %) of the process. Therefore, the study offers an important value to study eucalyptus leaves in micron-scale ZVI-Fenton technology.
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Affiliation(s)
- Baizhou Lu
- School of Environment, South China Normal University, Guangzhou 510006, China; Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou 510006, China
| | - Zhanqiang Fang
- School of Environment, South China Normal University, Guangzhou 510006, China; Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou 510006, China; Normal University (Qingyuan) Environmental Remediation Technology Co., Ltd, Qingyuan 511500, China.
| | - Pokeung Eric Tsang
- Department of Science and Environmental Studies, The Education University of Hong Kong, 00852, Hong Kong
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17
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Yu SY, Shi Y, He CS, Dong YD, Sun S, Ning RY, Xiong ZK, Zhou P, Zhang H, Lai B. Accelerated removal of naproxen in the iron-based peracetic acid activation system by chloride ions: Enhancement of reactive oxidative species via the formation of iron-chloride complexes. JOURNAL OF HAZARDOUS MATERIALS 2024; 462:132760. [PMID: 37839375 DOI: 10.1016/j.jhazmat.2023.132760] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 08/11/2023] [Revised: 09/17/2023] [Accepted: 10/09/2023] [Indexed: 10/17/2023]
Abstract
Iron-based PAA activation process is a promising advanced oxidation process for water decontamination which depends on Fe(II) as the main reactive site for PAA activation, resulting in various reactive oxidative species (ROSs) generation. For practical application, the impact of water matrix chloride ion (Cl-) on ROSs production and contaminants removal should be carefully considered. In this study, it's found that the introduction of Cl- (0.1-10 mM) could significantly enhance the reaction rate of the rapid stage (kobs1) up to 2.15 times at the initial pH of 4.25 in the Fe(II)/PAA system. Further studies demonstrated that the improved removal capacity of NAP resulted from Cl- induced R-O• generation as indicated by the exposure dose of R-O• increasing from 7.74 × 10-11 M•s to 1.44 × 10-10 M•s, rather than chlorine-containing radicals' generation. DFT calculation results suggested that the formed Fe(II)-Cl- complexes could easily activate PAA to generate more ROSs for NAP removal. Moreover, Fe(II)/PAA treatment can alleviate the biological toxicity of pollutants via both the Escherichia coli test and toxicity assessment. The obtained new knowledge manifested that Cl- can boost ROSs generation and conversion in iron-based PAA systems, providing guidance for the efficient decontamination of chlorine-containing sewage with PAA-based AOPs.
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Affiliation(s)
- Si-Ying Yu
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Yang Shi
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Chuan-Shu He
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
| | - Yu-Dan Dong
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Si Sun
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Ru-Yan Ning
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Zhao-Kun Xiong
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Peng Zhou
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Heng Zhang
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Bo Lai
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
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18
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Guo Y, Sui M, Liu S, Li T, Lv X, Yu M, Mo Y. Insight into cobalt substitution in LaFeO 3-based catalyst for enhanced activation of peracetic acid: Reactive species and catalytic mechanism. JOURNAL OF HAZARDOUS MATERIALS 2024; 461:132662. [PMID: 37801973 DOI: 10.1016/j.jhazmat.2023.132662] [Citation(s) in RCA: 6] [Impact Index Per Article: 6.0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 05/25/2023] [Revised: 07/28/2023] [Accepted: 09/26/2023] [Indexed: 10/08/2023]
Abstract
In this study, a hollow sphere-like Co-modified LaFeO3 perovskite catalyst (LFC73O) was developed for peracetic acid (PAA) activation to degrade sulfamethoxazole (SMX). Results indicated that the constructed heterogeneous system achieved a 99.7% abatement of SMX within 30 min, exhibiting preferable degradation performance. Chemical quenching experiments, probe experiments, and EPR techniques were adopted to elucidate the involved mechanism. It was revealed that the superior synergistic effect of electron transfer and oxygen defects in the LFC73O/PAA system enhanced the oxidation ability of PAA. The Co atoms doped into LaFeO3 as the main active site with the original Fe atoms as an auxiliary site exhibited high activity to mediate PAA activation via the Co(III)/Co(II) cycle, generating carbon-centered radicals (RO·) including CH3C(O)O· and CH3C(O)OO·. The oxygen vacancies induced by cobalt substitution also served as reaction sites, facilitating the dissociation of PAA and production of ROS. Furthermore, the degradation pathways were postulated by DFT calculation and intermediates identification, demonstrating that the electron-rich sites of SMX molecules such as amino group, aromatic ring, and S-N bond, were more susceptible to oxidation by reactive species. This study offers a novel perspective on developing catalysts with the coexistence of multiple active units for PAA activation in environmental remediation.
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Affiliation(s)
- Yali Guo
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China
| | - Minghao Sui
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, PR China.
| | - Shuan Liu
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China
| | - Tian Li
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, PR China
| | - Xinyuan Lv
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China
| | - Miao Yu
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China
| | - Yaojun Mo
- State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China
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19
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Chen XJ, Bai CW, Sun YJ, Huang XT, Zhang BB, Zhang YS, Yang Q, Wu JH, Chen F. pH-Driven Efficacy of the Ferrate(VI)-Peracetic Acid System in Swift Sulfonamide Antibiotic Degradation: A Deep Dive into Active Species Evolution and Mechanistic Insights. ENVIRONMENTAL SCIENCE & TECHNOLOGY 2023; 57:20206-20218. [PMID: 37965750 DOI: 10.1021/acs.est.3c06370] [Citation(s) in RCA: 15] [Impact Index Per Article: 7.5] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Indexed: 11/16/2023]
Abstract
In the realm of wastewater treatment, the power of ferrate (Fe(VI)) and peracetic acid (PAA) as oxidants stands out. But their combined might is where the enhancement truly lies. Their collaborative effect intensifies, but the underlying mechanics, especially across varying pH levels and pollutant types, still lurks in obscurity. Our study delved into the sophisticated oxidation interplay among Fe(VI)-PAA, Fe(VI)-H2O2, and standalone Fe(VI) systems. Notably, at a pH of 9.0, boasting a kinetic constant of ∼0.127 M-1·s-1, the Fe(VI)-PAA system annihilated the pollutant sulfamethoxazole, outpacing its counterparts by a staggering 48.73-fold when compared to the Fe(VI)-H2O2 system and 105.58-fold when using Fe(VI) individually. The behavior of active species─such as the dynamic •OH radicals and high-valent iron species (Fe(IV)/Fe(V))─shifted with pH variations, leading to distinct degradation pathways. Our detailed exploration pinpoints the behaviors of certain species across pH levels from 3.0 to 9.0. In more acidic environments, the •OH species proved indispensable for the system's reactivity. Conversely, as the pH inclined, degradation was increasingly steered by high-valent iron species. This intensive probe demystifies Fe(VI) interactions, deepening our understanding of the capabilities of the Fe(VI)-centered system and guiding us toward cleaner water solutions. Importantly, pH value, often underappreciated, holds the reins in organic wastewater decontamination. Embracing this key player is vital as we strategize for more expansive systems in upcoming ventures.
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Affiliation(s)
- Xin-Jia Chen
- Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China
| | - Chang-Wei Bai
- Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China
| | - Yi-Jiao Sun
- Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China
| | - Xin-Tong Huang
- Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China
| | - Bin-Bin Zhang
- Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China
| | - Yi-Shuo Zhang
- Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China
| | - Qi Yang
- College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
- Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, China
| | - Jing-Hang Wu
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei 230026, China
| | - Fei Chen
- Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing 400045, China
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Yang S, He Y, Hua Z, Xie Z, He CS, Xiong Z, Du Y, Liu Y, Xing G, Fang J, Mu Y, Lai B. pH-dependent bisphenol A transformation and iodine disinfection byproduct generation by peracetic acid: Kinetic and mechanistic explorations. WATER RESEARCH 2023; 246:120695. [PMID: 37812978 DOI: 10.1016/j.watres.2023.120695] [Citation(s) in RCA: 3] [Impact Index Per Article: 1.5] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 07/03/2023] [Revised: 09/06/2023] [Accepted: 10/03/2023] [Indexed: 10/11/2023]
Abstract
Peracetic acid (PAA) is regarded as an environmentally friendly oxidant because of its low formation of toxic byproducts. However, this study revealed the potential risk of generating disinfection byproducts (DBPs) when treating iodine-containing wastewater with PAA. The transformation efficiency of bisphenol A (BPA), a commonly detected phenolic contaminant and a surrogate for phenolic moieties in dissolved organic matter, by PAA increased rapidly in the presence of I-, which was primarily attributed to the formation of active iodine (HOI/I2) in the system. Kinetic model simulations demonstrated that the second-order rate constant between PAA and HOI was 54.0 M-1 s-1 at pH 7.0, which was lower than the generation rate of HOI via the reaction between PAA and I-. Therefore, HOI can combine with BPA to produce iodine disinfection byproducts (I-DBPs). The transformation of BPA and the generation of I-DBPs in the I-/PAA system were highly pH-dependent. Specifically, acidic conditions were more favorable for BPA degradation because of the higher reaction rates of BPA and HOI. More iodinated aromatic products were detected after 5 min of the reaction under acidic and neutral conditions, resulting in higher toxicity towards E. coli. After 12 h of the reaction, more adsorbable organic iodine (AOI) was generated at alkaline conditions because HOI was not able to efficiency transform to IO3-. The presence of H2O2 in the PAA solution played a role in the reaction with HOI, particularly under alkaline conditions. This study significantly advances the understanding of the role of I- in BPA oxidation by PAA and provides a warning to further evaluate the potential environmental risk during the treatment of iodine-bearing wastewater with PAA.
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Affiliation(s)
- Shurun Yang
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Yongli He
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Zhechao Hua
- Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China
| | - Zhihui Xie
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Chuan-Shu He
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
| | - Zhaokun Xiong
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Ye Du
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Yang Liu
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Guowei Xing
- College of Environment & Ecology, Xiamen University, Xiamen 361000, China
| | - Jingyun Fang
- Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China
| | - Yang Mu
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
| | - Bo Lai
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
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Wu J, Zou J, Lin J, Li S, Chen S, Liao X, Yang J, Yuan B, Ma J. Hydroxylamine enhanced the degradation of diclofenac in Cu(II)/peracetic acid system: Formation and contributions of CH 3C(O)O •, CH 3C(O)OO •, Cu(III) and •OH. JOURNAL OF HAZARDOUS MATERIALS 2023; 460:132461. [PMID: 37677972 DOI: 10.1016/j.jhazmat.2023.132461] [Citation(s) in RCA: 4] [Impact Index Per Article: 2.0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 06/28/2023] [Revised: 08/13/2023] [Accepted: 08/31/2023] [Indexed: 09/09/2023]
Abstract
The slow reduction of Cu(II) into Cu(I) through peracetic acid (PAA) heavily limited the widespread application of Cu(II)/PAA system. Herein, hydroxylamine (HA) was proposed to boost the oxidative capacity of Cu(II)/PAA system by facilitating the redox cycle of Cu(I)/Cu(II). HA/Cu(II)/PAA system was quite rapid in the removal of diclofenac within a broad pH range of 4.5-9.5, with a 10-fold increase in the removal rate of diclofenac compared with the Cu(II)/PAA system at an optimal initial pH of 8.5. Results of UV-Vis spectra, electron paramagnetic resonance, and alcohol quenching experiments demonstrated that CH3C(O)O•, CH3C(O)OO•, Cu(III), and •OH were involved in HA/Cu(II)/PAA system, while CH3C(O)OO• was verified as the predominant reactive species of diclofenac elimination. Different from previously reported Cu-catalyzed PAA processes, CH3C(O)OO• mainly generated from the reaction of PAA with Cu(III) rather than CH3C(O)O• and •OH. Four possible elimination pathways for diclofenac were proposed, and the acute toxicity of treated diclofenac solution with HA/Cu(II)/PAA system significantly decreased. Moreover, HA/Cu(II)/PAA system possessed a strong anti-interference ability towards the commonly existent water matrix. This research proposed an effective strategy to boost the oxidative capacity of Cu(II)/PAA system and might promote its potential application, especially in copper-contained wastewater.
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Affiliation(s)
- Jianying Wu
- Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China
| | - Jing Zou
- Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China.
| | - Jinbin Lin
- Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China; Key Laboratory for Thin Film and Microfabrication of the Ministry of Education, School of Environment, Shanghai Jiao Tong University, Shanghai 200240, PR China
| | - Sheng Li
- Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China
| | - Siying Chen
- Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China
| | - Xiaobin Liao
- Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China
| | - Jingxin Yang
- Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, PR China
| | - Baoling Yuan
- Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China; Key Laboratory of Songliao Aquatic Environment, Ministry of Education, Jilin Jianzhu University, Changchun 130118, PR China
| | - Jun Ma
- State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, Heilongjiang 150090, PR China
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Wu X, Wang X, Lynch I, Guo Z, Zhang P, Wu L, Ning P, Ren N. Exceptional photo-elimination of antibiotic by a novel Z-scheme heterojunction catalyst composed of nanoscale zero valent iron embedded with carbon quantum dots (CQDs)-black TiO 2. JOURNAL OF HAZARDOUS MATERIALS 2023; 460:132323. [PMID: 37666174 DOI: 10.1016/j.jhazmat.2023.132323] [Citation(s) in RCA: 7] [Impact Index Per Article: 3.5] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 05/30/2023] [Revised: 07/28/2023] [Accepted: 08/15/2023] [Indexed: 09/06/2023]
Abstract
Passivation of nanoscale zero valent iron (nZVI, Fe0) impaired its longevity while black TiO2 (b-TiO2) suffered from restricted optical properties. Using a facile approach, a novel Z-scheme heterojunction catalyst (Fe0@CQDs-TiO2(b)) of nZVI decorated with carbon quantum dots (CQDs) implanted into b-TiO2 was designed. Characterization results revealed the optical potential of the passivation coating of nZVI. The incorporation of CQDs stimulated the creation of active •OH during the dark reaction, and led to an accelerated mobility of photo-excited carriers of b-TiO2 and optimized its band gap (narrowing from 2.36 eV to 2.15 eV) during the light reaction. The photo-elimination capacity of metronidazole (MNZ) on Fe0@CQDs-TiO2(b) (99.36%) was 2.64, 8.25 and 1.34 fold beyond that on nZVI, b-TiO2 and Fe0@b-TiO2, respectively. The assembled material offered excellent adaptability to environmental substrates, in addition to being virtually unaffected by tap (95.62%) and river water (92.62%). The mechanism of MNZ degradation was elaborated, and the combination of density functional theory (DFT) calculations and LC-MS discerned 12 intermediates and 3 routes. Toxicity assessment of these products was conducted to ensure no inadvertent negative environmental impacts arose. This work proposed an original direction and mechanism for the application of passivation layers in nZVI-based materials for environmental restoration.
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Affiliation(s)
- Xi Wu
- Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China
| | - Xiangyu Wang
- Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China; School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UK.
| | - Iseult Lynch
- School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UK
| | - Zhiling Guo
- School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UK
| | - Peng Zhang
- School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UK
| | - Lisi Wu
- School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UK
| | - Ping Ning
- Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China.
| | - Nanqi Ren
- School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150090, China
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23
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Chen JQ, Zhou GN, Ding RR, Li Q, Zhao HQ, Mu Y. Ferrous ion enhanced Fenton-like degradation of emerging contaminants by sulfidated nanosized zero-valent iron with pH insensitivity. JOURNAL OF HAZARDOUS MATERIALS 2023; 459:132229. [PMID: 37549576 DOI: 10.1016/j.jhazmat.2023.132229] [Citation(s) in RCA: 4] [Impact Index Per Article: 2.0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 06/14/2023] [Revised: 07/29/2023] [Accepted: 08/03/2023] [Indexed: 08/09/2023]
Abstract
In this study, the performance and mechanism of the integrated sulfidated nanosized zero-valent iron and ferrous ions (S-nZVI/Fe2+) system for oxygen activation to remove emerging contaminants (ECs) were comprehensively explored. The S-nZVI/Fe2+ system exhibited a 2.4-8.2 times of increase in the pseudo-first order kinetic rate constant for the oxidative degradation of various ECs compared to the S-nZVI system under aerobic conditions, whereas negligible removal was observed in both nZVI and nZVI/Fe2+ systems. Moreover, remarkable EC mineralization efficiency and benign detoxification capacity were also demonstrated in the S-nZVI/Fe2+ system. We revealed that dosing Fe2+ promoted the corrosion of S-nZVI by maintaining an acidic solution pH, which was conducive to O2 activation by dissolved Fe2+ and surface-absorbed Fe(II) to produce •OH. Furthermore, the generation of H* was enhanced for the further reduction of Fe(III) and H2O2 to Fe(II) and •O2-, resulting in the improvement of consecutive single-electron O2 activation for •OH production. Additionally, bisphenol A (BPA) degradation by S-nZVI/Fe2+ was positively correlated with the S-nZVI dosage, with an optimum S/Fe molar ratio of 0.15. The Fenton-like degradation process by S-nZVI/Fe2+ was pH-insensitive, indicating its robust performance over a wide pH range. This study provides valuable insights for the practical implementation of nZVI-based technology in achieving high-efficiency removal of ECs from water.
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Affiliation(s)
- Jia-Qi Chen
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
| | - Guan-Nan Zhou
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China; State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic Pollution, China University of Geosciences, Wuhan 430078, China
| | - Rong-Rong Ding
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
| | - Qi Li
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
| | - Han-Qing Zhao
- College of Environment and Ecology, Chongqing University, Chongqing, China
| | - Yang Mu
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.
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24
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Zhou C, Sui M, Du S. Insights into the electron activation mechanisms at the micro level by nano zero-valent iron supported by molybdenum disulfide (nZVI@MD) from preparation to application. JOURNAL OF HAZARDOUS MATERIALS 2023; 458:131968. [PMID: 37429190 DOI: 10.1016/j.jhazmat.2023.131968] [Citation(s) in RCA: 3] [Impact Index Per Article: 1.5] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 05/03/2023] [Revised: 06/14/2023] [Accepted: 06/28/2023] [Indexed: 07/12/2023]
Abstract
Both molybdenum disulfide (MoS2) and nano zero-valent iron (nZVI) exhibit excellent adsorption abilities. However, the constrained conductivity of MoS2 and the lack of selectivity of nZVI for electron transfer still pose challenges. In this study, we designed a series of novel nano zero-valent iron supported by molybdenum disulfide composites (nZVI@MD) with multiple electron-rich active sites, including iron dopant replacement, iron atom intercalation and exposed Mo4+, for effective removal of Cr(VI). Results showed that preparation temperature and the amount of MoS2 added were identified as the two most significant factors affecting the reduction properties of nZVI@MD. Systematic experiments revealed that the nZVI@MD exhibited good anti-interference performance, stability and reusability due to its excellent electron selectivity. Characterization results exhibited that iron atoms replaced the sulfur vacancies in MoS2 and inserted into an intercalation of MoS2 during the preparation process. The mechanisms underlying the uptake of Cr(VI) by nZVI@MD can be proposed as follows: (i) electrostatic interactions, (ii) reduction reaction, and (iii) co-precipitation involving Fe-O-Cr. Furthermore, nZVI@MD exhibited excellent electron activity, hydrophilicity and oxidation resistance, confirmed by density functional theory (DFT) calculations. This work provided new strategies and mechanistic insights for the rational design of adsorbents.
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Affiliation(s)
- Chundi Zhou
- State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, People's Republic of China
| | - Minghao Sui
- State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, People's Republic of China.
| | - Songhang Du
- State Key Laboratory of Pollution Control and Resource Reuse, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai 200092, People's Republic of China
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25
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Xie ZH, He CS, Pei DN, Zheng YZ, Wu XY, Xiong Z, Du Y, Pan ZC, Yao G, Lai B. Efficient degradation of micropollutants in CoCaAl-LDO/peracetic acid (PAA) system: An organic radical dominant degradation process. JOURNAL OF HAZARDOUS MATERIALS 2023; 452:131286. [PMID: 37001209 DOI: 10.1016/j.jhazmat.2023.131286] [Citation(s) in RCA: 14] [Impact Index Per Article: 7.0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 01/06/2023] [Revised: 03/15/2023] [Accepted: 03/23/2023] [Indexed: 06/19/2023]
Abstract
As a novel strategy, peracetic acid (PAA) based advanced oxidation processes (AOPs) are being used in micropollutant elimination due to their high oxidation and low toxicity. In this study, Co2Ca1Al1-LDO as a kind of layered double oxides (LDOs) was successfully synthesized, and it is the first time to apply Co2Ca1Al1-LDO for activating PAA. The Co2Ca1Al1-LDO/PAA system showed excellent removal efficiencies for various micropollutants with removal ratios ranging from 90.4% to 100% and k values from 0.087 min-1 to 0.298 min-1. In the degradation period, various reactive oxygen species (ROS) are involved in the system, while organic radicals (R-O•) with a high concentration of 5.52 × 10-13 M are the dominant ROS in the contaminants degradation process. Compared to other ROS, R-O• had the largest contribution ratio (more than 85%) to pollutant degradation. Further analysis demonstrated that C1, C2, C3, C4, C5, C6 and N11 concentrated on the aniline group of SMX are the main attack sites based on the density functional theory (DFT) results, which is consistent with the degradation products. The toxicity of contaminants was obviously reduced after removing in this system. Furthermore, Co2Ca1Al1-LDO showed good reusability and stability, and Co2Ca1Al1-LDO/PAA system had excellent removal ability in actual water bodies containing inorganic anions, showing good application potential. Importantly, this study explored the feasibility of applying LDO catalysts in PAA-based AOPs for micropollutants elimination, providing new insights for subsequent research.
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Affiliation(s)
- Zhi-Hui Xie
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Chuan-Shu He
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
| | - Dan-Ni Pei
- Nanjing Institute of Testing and Measurement Technology, Nanjing 210049, China
| | - Yun-Zhe Zheng
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Xiao-Yu Wu
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Zhaokun Xiong
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Ye Du
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
| | - Zhi-Cheng Pan
- Water Safety and Water Pollution Control Engineering Technology Research Center in Sichuan Province, Haitian Water Group, China
| | - Gang Yao
- Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China; Institute of Environmental Engineering, RWTH Aachen University, Germany
| | - Bo Lai
- State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
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26
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Xu P, Wang L, Liu X, Xie S, Hou B. Vitamin C promoted refractory organic contaminant elimination in the zero-valent iron/peracetic acid system: Efficiency, mechanism and effects of various parameters. CHEMOSPHERE 2023; 326:138481. [PMID: 36958501 DOI: 10.1016/j.chemosphere.2023.138481] [Citation(s) in RCA: 2] [Impact Index Per Article: 1.0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/06/2022] [Revised: 02/28/2023] [Accepted: 03/20/2023] [Indexed: 06/18/2023]
Abstract
The conventional zero-valent iron/peracetic acid (ZVI/PAA) system is severely limited owing to the passivation of ZVI and the low recovery of Fe2+. In this study, a reducing agent, vitamin C (H2A), was used for the first time to enhance the ZVI/PAA system as a way to improve its degradation performance. Under optimal conditions, the removal efficiency of the H2A/ZVI/PAA system was 82.9%, while that of the H2A/PAA and ZVI/PAA systems were only 19.0% and 25.6%. Free radical quenching and electron paramagnetic experiments (EPR) confirmed that CH3C(O)O•, •OH and CH3C(O)OO• were the major active species for acid orange 7 (AO7) degradation with contributions of 9.7%, 75% and 14.4%, respectively. The degradation mechanism was proposed through UV-vis full-wavelength scanning and chemical oxygen demand (COD) experiments. The removal of AO7 was not affected in the presence of Cl-, SO42- and HCO3-, while inhibition occurred with humic acid. ZVI exhibited excellent catalytic properties and stability, and the removal efficiency of AO7 exceeded 70% after three cycles. Additionally, the H2A/ZVI/PAA system showed good ability to remove AO7 in well water, lake water, river water and reservoir water, and the elimination efficiency of MO, DCF and ACE also exceeded 70%. Overall, this study contributes new cognition for enhancing the ZVI/PAA system to degrade contaminants, which is expected to achieve a cleaner water environment.
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Affiliation(s)
- Peng Xu
- Hunan Engineering Research Center of Water Security Technology and Application, College of Civil Engineering, Hunan University, Changsha, 410082, PR China; Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Hunan University, Changsha, 410082, PR China.
| | - Lei Wang
- Hunan Engineering Research Center of Water Security Technology and Application, College of Civil Engineering, Hunan University, Changsha, 410082, PR China; Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Hunan University, Changsha, 410082, PR China
| | - Xin Liu
- Hunan Engineering Research Center of Water Security Technology and Application, College of Civil Engineering, Hunan University, Changsha, 410082, PR China; Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Hunan University, Changsha, 410082, PR China
| | - Shiqi Xie
- Hunan Engineering Research Center of Water Security Technology and Application, College of Civil Engineering, Hunan University, Changsha, 410082, PR China; Key Laboratory of Building Safety and Energy Efficiency, Ministry of Education, Hunan University, Changsha, 410082, PR China
| | - Baolin Hou
- School of Civil Engineering, Hunan University of Science and Technology, Xiangtan, 411201, China
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Thamilselvan A, Dang VD, Doong RA. Ni-Co bimetallic decorated dodecahedral ZIF as an efficient catalyst for photoelectrochemical degradation of sulfamethoxazole coupled with hydrogen production. THE SCIENCE OF THE TOTAL ENVIRONMENT 2023; 873:162208. [PMID: 36801406 DOI: 10.1016/j.scitotenv.2023.162208] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/02/2022] [Revised: 01/26/2023] [Accepted: 02/09/2023] [Indexed: 06/18/2023]
Abstract
In this work, a NiCo bimetallic ZIF (BMZIF) dodecahedron material has been synthesized by the precipitation approach and then used for simultaneously photoelectrocatalytic degradation of sulfamethoxazole (SMX) and hydrogen production. The combination of Ni/Co loading in ZIF structure increased the specific surface area 1484 (m2 g-1) and photocurrent density (0.4 mA cm-2), which can facilitate the good charge transfer efficiency. In presence of peroxymonosulfate (PMS, 0.1 mM), the complete degradation of SMX (10 mg L-1) was achieved at initial pH of 7 within 24 min, with the pseudo-first-order rate constants of 0.18 min-1 and TOC removal efficiency of 85 %. Radical scavenger experiments affirm that •OH radicals were the primary oxygen reactive species to drive the SMX degradation. Along with SMX degradation at the anode, the H2 production was observed at the cathode (140 μmol cm-2 h-1), which was 1.5 and 3 times higher than that of Co-ZIF and Ni-ZIF, respectively. The superior catalytic performance of BMZIF was assigned to the distinctive internal structure and synergistic effect between ZIF and Ni/Co bimetals, which improves light absorption and charge conduction efficiency. This study may provide insight into the new way to treat polluted water and simultaneously produce green energy using bimetallic ZIF in a PEC system.
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Affiliation(s)
- Annadurai Thamilselvan
- Institute of Analytical and Environmental Sciences, National Tsing Hua University, Hsinchu 30013, Taiwan
| | - Van Dien Dang
- Faculty of Biology and Environment, Ho Chi Minh City University of Food Industry, 140 Le Trong Tan, Tan Phu dist., Ho Chi Minh 700000, Viet Nam
| | - Ruey-An Doong
- Institute of Analytical and Environmental Sciences, National Tsing Hua University, Hsinchu 30013, Taiwan.
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28
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Zhang H, An Q, Su Y, Quan X, Chen S. Co 3O 4 with upshifted d-band center and enlarged specific surface area by single-atom Zr doping for enhanced PMS activation. JOURNAL OF HAZARDOUS MATERIALS 2023; 448:130987. [PMID: 36860058 DOI: 10.1016/j.jhazmat.2023.130987] [Citation(s) in RCA: 13] [Impact Index Per Article: 6.5] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/17/2022] [Revised: 02/06/2023] [Accepted: 02/08/2023] [Indexed: 06/18/2023]
Abstract
In this work, single-atom Zr doping is demonstrated to be an effective strategy to enhance the catalytic performance of Co3O4 toward peroxymonosulfate (PMS) by modulating electronic structure and enlarging specific surface simultaneously. The d-band center of Co sites upshifts owing to different electronegativity of Co and Zr in the bonds of Co-O-Zr confirmed by density functional theory calculations, leading to enhanced adsorption energy of PMS and strengthened electron transfer from Co(II) to PMS. The specific surface area of Zr-doped Co3O4 increases by 6 times due to the decrease of crystalline size. Consequently, the kinetic constant of phenol degradation with Zr-Co3O4 is 10 times higher than that with Co3O4 (0.31 vs. 0.029 min-1). The relative surface specific kinetic constant of Zr-Co3O4 for phenol degradation is still 2.29 times higher than that of Co3O4 (0.00660 vs. 0.00286 g m-2 min-1). In addition, the potential practical applicability of 8Zr-Co3O4 was also confirmed by practical wastewater treatment. This study provides deep insights into modifying electronic structure and enlarging specific surface area to enhance the catalytic performance.
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Affiliation(s)
- Hang Zhang
- Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, China, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
| | - Qi An
- Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, China, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
| | - Yan Su
- Key Laboratory of Materials Modification by Laser, Ion and Electron Beams, Ministry of Education, School of Physics, Dalian University of Technology, Dalian 116024, China
| | - Xie Quan
- Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, China, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
| | - Shuo Chen
- Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of Education, China, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.
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29
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Li Q, Wang M, Chen JQ, Liu X, Wang J, Mu Y. Vivianite-induced peroxymonosulfate activation for containment removal under dark conditions: Performance, mechanism and regeneration. WATER RESEARCH 2023; 233:119729. [PMID: 36801576 DOI: 10.1016/j.watres.2023.119729] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/21/2022] [Revised: 02/09/2023] [Accepted: 02/09/2023] [Indexed: 06/18/2023]
Abstract
The performance and intrinsic mechanism of vivianite, a natural mineral containing structural Fe(II), for peroxymonosulfate (PMS) activation and pollutant degradation under dark conditions were comprehensively explored in this study. It was found that vivianite was able to efficiently activate PMS to degrade various pharmaceutical pollutants under dark conditions, in which the corresponding reaction rate constant of ciprofloxacin (CIP) degradation was 47- and 32-fold higher than that of magnetite and siderite, respectively. SO4·-, ·OH, Fe(IV) and electron-transfer processes were found in the vivianite-PMS system, while SO4·- was the main contributor to CIP degradation. Moreover, mechanistic explorations revealed that the Fe site on the surface of vivianite could bind PMS in the form of a bridge position, and thus vivianite could rapidly activate absorbed PMS due to its strong electron-donating ability. Additionally, it was illustrated that the used vivianite could be efficiently regenerated by either chemical or biological reduction. This study may provide an alternative application of vivianite in addition to phosphorus recovery from wastewater.
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Affiliation(s)
- Qi Li
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
| | - Mingzhou Wang
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
| | - Jia-Qi Chen
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
| | - Xiaomeng Liu
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.
| | - Jing Wang
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
| | - Yang Mu
- CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.
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30
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Lu B, Fang Z, Tsang PE, Wu J. Effect and mechanism of norfloxacin removal by guava leaf extract in the ZVI/H 2O 2 system. CHEMOSPHERE 2023; 316:137801. [PMID: 36634715 DOI: 10.1016/j.chemosphere.2023.137801] [Citation(s) in RCA: 2] [Impact Index Per Article: 1.0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 11/07/2022] [Revised: 12/25/2022] [Accepted: 01/08/2023] [Indexed: 06/17/2023]
Abstract
To overcome the bottlenecks of the conventional zero-valent iron Fenton-like (ZVI/H2O2) process, such as low reagent utilization, low applicable pH, and iron sludge contamination, guava leaf extract (GLE) was used as a green promoter to enhance ZVI/H2O2 process in this study. Compared with the ZVI/H2O2 system, the removal rate and kobs of norfloxacin by the ZVI/H2O2/GLE system were increased by 33.76% and 2.19 times, respectively. The experimental investigation of the mechanism showed that the attack of reactive oxygen species was the main pathway for the removal of pollutants, and three types of reactive oxygen species (1O2, O2-,·OH) generations in the ZVI/H2O2/GLE system were effectively promoted by the introduction of GLE. The reactivity improvement was mainly due to the decrease of pH. At the same time, the chelation of iron ions by GLE promoted the Fe(III)/Fe(II) cycle on the catalyst surface was also a minor mechanism to improve the reactivity. This study provides a crucial reference for the practical application of guava leaf to promote the ZVI/H2O2 process in environmental pollution control.
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Affiliation(s)
- Baizhou Lu
- School of Environment, South China Normal University, Guangzhou, 510006, China; Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou, 510006, China
| | - Zhanqiang Fang
- School of Environment, South China Normal University, Guangzhou, 510006, China; Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou, 510006, China; Normal University (Qingyuan) Environmental Remediation Technology Co., Ltd., Qingyuan, 511500, China.
| | - Pokeung Eric Tsang
- Department of Science and Environmental Studies, The Education University of Hong Kong, 00852, Hong Kong, China
| | - Jinhua Wu
- School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China
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31
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Ohta N, Kobayashi M, Kawase Y. Removal of pharmaceutically active compounds (PhACs) by zero-valent iron: quantification of removal mechanisms consisting of degradation, adsorption and co-precipitation. ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH INTERNATIONAL 2023; 30:38819-38831. [PMID: 36586022 DOI: 10.1007/s11356-022-25047-5] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 10/24/2022] [Accepted: 12/25/2022] [Indexed: 06/17/2023]
Abstract
The removal mechanisms of carbamazepine (CBZ), which is one of pharmaceutically active compounds, using zero-valent iron (ZVI) were quantified by defining three fractions, namely "degradation", "adsorption", and "co-precipitation". The maximum total organic carbon (TOC) removal was obtained at pH 4. The results demonstrate that the adsorption on the ZVI surface is dominant in the TOC removal of CBZ for 4 ≤ pH ≤ 6 while the degradation by oxidative and reductive reactions is efficient exclusively for pH ≤ 3. TOC removal was not obtained for pH ≥ 8. The most dominant mechanism in the removal of CBZ by ZVI is the adsorption onto the iron oxides/hydroxides layer formed on ZVI surface rather than the degradation by oxidative and reductive reactions including Fenton and Fenton-like reactions for pH ≥ 4. A novel kinetic model for removal of CBZ by ZVI was developed to simulate the dynamic concentration profiles of CBZ, TOC, total Fe ions, and dissolved oxygen linked closely with each other and the contributions of degradation, adsorption, and co-precipitation in TOC removal of CBZ. Reasonable agreement between experimental data and model predictions suggests the applicability of the proposed kinetic model to quantitatively analyze the mechanisms of CBZ removal by ZVI.
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Affiliation(s)
- Naoki Ohta
- Research Center for Biochemical and Environmental Engineering, Department of Applied Chemistry, Toyo University, Kawagoe, Saitama, 350-8585, Japan
| | - Maki Kobayashi
- Research Center for Biochemical and Environmental Engineering, Department of Applied Chemistry, Toyo University, Kawagoe, Saitama, 350-8585, Japan
| | - Yoshinori Kawase
- Research Center for Biochemical and Environmental Engineering, Department of Applied Chemistry, Toyo University, Kawagoe, Saitama, 350-8585, Japan.
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32
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Geng M, Huang X, Shi B, Yu J, Wang C, Du Y, Wang Y. Enhancement of thioethers removal by pre-oxidation-coagulation: Effects of background organic matter. THE SCIENCE OF THE TOTAL ENVIRONMENT 2023; 857:159465. [PMID: 36257419 DOI: 10.1016/j.scitotenv.2022.159465] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 08/21/2022] [Revised: 10/10/2022] [Accepted: 10/12/2022] [Indexed: 06/16/2023]
Abstract
Swampy/septic odor caused by thioethers has become the main taste and odor (T&O) problem in drinking water of China. Improving its removal performance by commonly traditional water treatment process is significant. In our study, we have found that pre-oxidation could modify the background dissolved organic matter (DOM) properties and thus improve the coagulation performance of thioethers, increasing the coagulation removal rates by 1.5-3 times. Particularly, after pre-ozonation only protein-like substances remained, and thioethers removal was 1.5 times higher than that after pre-chlorination (only coagulation not including oxidation). Compared with humic acid (HA), the thioethers compounds removal efficiencies under bovine serum albumin (BSA) as background DOM was increased by 0.3-3 times. Through Freundlich model analysis, the binding strength of BSA (KF = 20.712, at 298 K) to dimethyl disulfide (DMDS) was enhanced by 60 % compared to HA (KF = 12.778, at 298 K). According to thermodynamic parameters, the binding effect between HA/BSA and thioethers compounds was mainly van der Waals forces and hydrogen bond. BSA with more amino structure and oxygen groups was more easily to adsorb DMDS through hydrogen bond and thus achieved better coagulation performance. Therefore, pre-ozonation combined with coagulation was suggested to be more suitable for thioethers compounds control.
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Affiliation(s)
- Mengze Geng
- Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China
| | - Xin Huang
- Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
| | - Baoyou Shi
- Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; University of Chinese Academy of Sciences, Beijing 100049, China
| | - Jianwei Yu
- Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; University of Chinese Academy of Sciences, Beijing 100049, China
| | - Chunmiao Wang
- Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
| | - Yuning Du
- Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
| | - Yili Wang
- Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, China.
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33
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Li Q, Wei G, Duan G, Zhang L, Li Z, Yan F. Valorization of ball-milled waste red mud into heterogeneous catalyst as effective peroxymonosulfate activator for tetracycline hydrochloride degradation. JOURNAL OF ENVIRONMENTAL MANAGEMENT 2022; 324:116301. [PMID: 36179468 DOI: 10.1016/j.jenvman.2022.116301] [Citation(s) in RCA: 6] [Impact Index Per Article: 2.0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 07/09/2022] [Revised: 08/25/2022] [Accepted: 09/14/2022] [Indexed: 06/16/2023]
Abstract
Red mud (RM), a kind of iron-rich industrial waste produced in the alumina production process, can be utilized as a potential iron-based material for the removal of refractory organic pollutants from wastewater in advanced oxidation processes (AOPs). In this work, high-iron RM (rich in iron) was activated in a ball mill and applied as an effective activator of peroxymonosulfate (PMS) for tetracycline hydrochloride (TC-HCl) degradation. Compared with that of unmilled RM (69.7%), the TC-HCl decomposition ratios of ball-milled RM (BM-RM) (72.2%-92.0%) were all improved in the presence of PMS. Systematic characterization suggested that ball milling could optimize the physicochemical properties of RM, such as increased surface area, increased oxygen vacancies, enhanced electrical conductivity, and increased exposure of Fe(II) sites, all of which could effectively improve RM for PMS activation to degrade TC-HCl. The quenching experiments and electron paramagnetic resonance technique revealed that 1O2 and SO4·- contributed dominantly to the TC-HCl degradation. Ultra performance liquid chromatography mass spectrometry analysis combined with density functional theory calculation revealed that the degradation pathways of TC-HCl were driven by hydroxylation, N-demethylation and dehydration in BM-RM/PMS system. Based on quantitative structure-activity relationship prediction using the Toxicity Estimation Software Tool software, the toxicity of almost all intermediates was significantly reduced. An obvious inhibition effect on TC-HCl was occurred in the presence of Cl-, whereas the presences of NO3- and SO42- had little effect. However, HCO3- improved TC-HCl removal efficiency. BM-RM had a wide working pH range (pH = 3-11) and showed good stability and reusability in use. Overall, this work not only offers a simple and promising approach to improve the catalytic activity of RM, but also opens new insights into the ball-milled RM as an effective PMS activator for wastewater treatment.
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Affiliation(s)
- Qingyong Li
- School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China; School of Environmental Science and Engineering, Guangdong University of Petrochemical Technology, Maoming, Guangdong, 525000, China
| | - Guangtao Wei
- School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China; Guangxi Key Laboratory of Processing for Non-ferrous Metallic and Featured Materials, Guangxi Zhuang Autonomous Region, Nanning, 530004, PR China.
| | - Guangxiang Duan
- School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China
| | - Linye Zhang
- School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China; Guangxi Key Laboratory of Bio-refinery, Guangxi Zhuang Autonomous Region, Nanning, 530007, PR China.
| | - Zhongmin Li
- School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China
| | - Feng Yan
- School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, PR China
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34
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Li S, Yang Y, Zheng H, Zheng Y, He CS, Lai B, Ma J, Nan J. Introduction of oxygen vacancy to manganese ferrite by Co substitution for enhanced peracetic acid activation and 1O 2 dominated tetracycline hydrochloride degradation under microwave irradiation. WATER RESEARCH 2022; 225:119176. [PMID: 36191527 DOI: 10.1016/j.watres.2022.119176] [Citation(s) in RCA: 42] [Impact Index Per Article: 14.0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Track Full Text] [Subscribe] [Scholar Register] [Received: 07/30/2022] [Revised: 09/19/2022] [Accepted: 09/26/2022] [Indexed: 06/16/2023]
Abstract
High microwave-response cobalt-substituted manganese ferrite (CMFO-0.5) was successfully synthesized as a heterogeneous catalyst for efficient peracetic acid (PAA) activation and tetracycline hydrochloride (TCH) degradation with singlet oxygen (1O2) as the dominated reactive oxidized species (ROS). The removal efficiency of TCH could reach 98.16% within 6 min under microwave irradiation when the CMFO-0.5 was added at 20 mg/L. It's found that the Co substitution could produce the oxygen vacancies (OVs), improve the microwave (MW) absorbing performance and enhance the internal electron transfer efficiency of materials. The phenomenon why 1O2 as the dominated ROS rather than hydroxyl radical (•OH) and organic radicals (R-O•) would be explained by the following aspects: the oxygen adsorbed on the OVs can accept the electron transformed from PAA to form superoxide radical (•O2-), which will disproportionate to form 1O2; the energy generated by the non-thermal effect of MW can dissociate PAA to generate peroxy-group for 1O2 generation. Furthermore, the possible TCH degradation pathways were proposed based on DFT theory calculations and product identification, and the toxicity predictions of the degradation products were also performed by the Ecological Structure-Activity Relationship Model (ECOSAR) software. Additionally, the decrease of acute toxicity of treated TCH, excellent stability and strong resistance towards water matrix fully demonstrate the superiority of the proposed system for practical application in wastewater treatment.
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Affiliation(s)
- Shuo Li
- College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar, 161006, China; Urban Water Resources Development and Northern National Engineering Research Center, Harbin, 150090, China; School of Environment, Harbin Institute of Technology, Harbin, 150090, China
| | - Yalun Yang
- College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar, 161006, China
| | - Heshan Zheng
- College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar, 161006, China
| | - Yongjie Zheng
- College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar, 161006, China
| | - Chuan-Shu He
- Department of Environmental Science and Engineering, School of Architecture and Environment, Sichuan University, Chengdu 610065, China.
| | - Bo Lai
- Department of Environmental Science and Engineering, School of Architecture and Environment, Sichuan University, Chengdu 610065, China.
| | - Jun Ma
- Urban Water Resources Development and Northern National Engineering Research Center, Harbin, 150090, China; School of Environment, Harbin Institute of Technology, Harbin, 150090, China
| | - Jun Nan
- Urban Water Resources Development and Northern National Engineering Research Center, Harbin, 150090, China; School of Environment, Harbin Institute of Technology, Harbin, 150090, China
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35
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Wang F, Duan H, Xu W, Sheng G, Sun Z, Chu H. Light-activated nanomaterials for tumor immunotherapy. Front Chem 2022; 10:1031811. [PMID: 36277335 PMCID: PMC9585221 DOI: 10.3389/fchem.2022.1031811] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Grants] [Track Full Text] [Download PDF] [Figures] [Journal Information] [Subscribe] [Scholar Register] [Received: 08/30/2022] [Accepted: 09/20/2022] [Indexed: 11/20/2022] Open
Abstract
Tumor immunotherapy mainly relies on activating the immune system to achieve antitumor treatment. However, the present tumor immunotherapy used in the clinic showed low treatment efficacy with high systematic toxicity. To overcome the shortcomings of traditional drugs for immunotherapy, a series of antitumor immunotherapies based on nanomaterials have been developed to enhance the body’s antitumor immune response and reduce systematic toxicity. Due to the noninvasiveness, remote controllability, and high temporal and spatial resolution of light, photocontrolled nanomaterials irradiated by excitation light have been widely used in drug delivery and photocontrolled switching. This review aims to highlight recent advances in antitumor immunotherapy based on photocontrolled nanomaterials. We emphasized the advantages of nanocomposites for antitumor immunotherapy and highlighted the latest progress of antitumor immunotherapy based on photoactivated nanomaterials. Finally, the challenges and future prospects of light-activated nanomaterials in antitumor immunity are discussed.
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Affiliation(s)
- Fang Wang
- Translational Medicine Center, Beijing Chest Hospital, Capital Medical University, Beijing, China
- Beijing Key Laboratory in Drug Resistant Tuberculosis Research, Beijing Tuberculosis and Thoracic Tumor Research Institute, Beijing, China
| | - Huijuan Duan
- Translational Medicine Center, Beijing Chest Hospital, Capital Medical University, Beijing, China
- Beijing Key Laboratory in Drug Resistant Tuberculosis Research, Beijing Tuberculosis and Thoracic Tumor Research Institute, Beijing, China
| | - Weizhe Xu
- Translational Medicine Center, Beijing Chest Hospital, Capital Medical University, Beijing, China
- Beijing Key Laboratory in Drug Resistant Tuberculosis Research, Beijing Tuberculosis and Thoracic Tumor Research Institute, Beijing, China
| | - Gang Sheng
- Translational Medicine Center, Beijing Chest Hospital, Capital Medical University, Beijing, China
- Beijing Key Laboratory in Drug Resistant Tuberculosis Research, Beijing Tuberculosis and Thoracic Tumor Research Institute, Beijing, China
| | - Zhaogang Sun
- Translational Medicine Center, Beijing Chest Hospital, Capital Medical University, Beijing, China
- Beijing Key Laboratory in Drug Resistant Tuberculosis Research, Beijing Tuberculosis and Thoracic Tumor Research Institute, Beijing, China
| | - Hongqian Chu
- Translational Medicine Center, Beijing Chest Hospital, Capital Medical University, Beijing, China
- Beijing Key Laboratory in Drug Resistant Tuberculosis Research, Beijing Tuberculosis and Thoracic Tumor Research Institute, Beijing, China
- *Correspondence: Hongqian Chu,
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