1
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Adly A, Galal MM, Matta ME. Catalytic degradation of norfloxacin using persulfate activation by Ni-Fe layered double hydroxide catalyst supported on activated carbon. Sci Rep 2025; 15:5132. [PMID: 39934292 DOI: 10.1038/s41598-025-89106-w] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Journal Information] [Subscribe] [Scholar Register] [Received: 11/16/2024] [Accepted: 02/03/2025] [Indexed: 02/13/2025] Open
Abstract
This study investigated the catalytic degradation of Norfloxacin (NOR), a persistent fluoroquinolone antibiotic, using a novel Ni-Fe Layered Double Hydroxide supported on Activated Carbon (NiFe-LDH@AC) as a catalyst. The composite was designed to activate persulfate (PDS) and generate sulfate radicals for NOR degradation in aqueous solutions. Characterization techniques such as XRD, SEM, EDS, TEM, FTIR, and BET confirmed the successful synthesis and structural integrity of the composite. The optimal degradation was achieved with a NiFe-LDH@AC ratio of 2:1, 0.3 g/L catalyst dosage, and 1 g/L PDS, resulting in 86% NOR removal efficiency within 60 min at neutral pH and ambient temperature for an initial concentration of 50 mg/L, and 100% removal for initial concentrations of 10 mg/L and 20 mg/L under the same conditions. The activation energy of the reaction was calculated as 58.27 kJ/mol. Radical scavenging experiments identified sulfate (SO₄˙⁻) and hydroxyl (•OH) radicals as the dominant reactive species, but the SO₄˙⁻ played a larger role. Furthermore, the catalyst exhibited good reusability, maintaining 75% degradation efficiency after four cycles, and showed minimal metal leaching. The study also proposed a mechanism for PDS activation using XPS analysis and suggested NOR degradation pathways through LC-ESI-MS/MS analysis. Moreover, the NiFe-LDH@AC/PDS system demonstrated 84% NOR degradation and 55% COD removal in real treated wastewater. Results demonstrated that the NiFe-LDH@AC composite effectively activated PDS, achieving high NOR removal efficiency, making it a promising sustainable material for wastewater treatment.
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Affiliation(s)
- Adel Adly
- Sanitary and Environmental Engineering Division, Faculty of Engineering, Cairo University, Giza, 12613, Egypt.
| | - Mona M Galal
- Sanitary and Environmental Engineering Division, Faculty of Engineering, Cairo University, Giza, 12613, Egypt
| | - Minerva E Matta
- Sanitary and Environmental Engineering Division, Faculty of Engineering, Cairo University, Giza, 12613, Egypt
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2
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Sambyal S, Sharma R, Mandyal P, Chauhan V, Priye A, Kumar M, Shandilya P. Nanocellulose-Supported Dual S-Scheme SnWO 4/Cu 2O/Ag 2WO 4 Heterojunction for Enhanced Photodegradation of Amoxicillin. ACS OMEGA 2025; 10:2472-2487. [PMID: 39895770 PMCID: PMC11780444 DOI: 10.1021/acsomega.4c05403] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Grants] [Track Full Text] [Download PDF] [Figures] [Subscribe] [Scholar Register] [Received: 06/28/2024] [Revised: 11/29/2024] [Accepted: 12/16/2024] [Indexed: 02/04/2025]
Abstract
A dual S-scheme nanocellulose-based SnWO4/Cu2O/Ag2WO4 (NC-SCA) heterojunction photocatalyst was synthesized via ultrasonication followed by a hydrothermal method for the efficient photodegradation of amoxicillin (AMX). Under UV-vis light irradiation, the NC-SCA photocatalyst exhibited an impressive 97.40% AMX degradation within 30 min, attributed to its improved optical absorption and superior charge migration. The characterization techniques, including XRD, FTIR, PL, and UV-vis spectroscopy, confirmed the successful integration of nanocellulose with SnWO4/Cu2O/Ag2WO4. XPS and ESR analyses provided insights into the S-scheme charge migration mechanism within the heterojunction. Further, the trapping experiments identified hydroxyl (•OH) and superoxide radicals as the primary reactive species. The photocatalyst displayed a specific surface area of 115.9 m2/g, offering a large active surface for photodegradation. Operational parameters such as the photocatalyst dosage, pH, and AMX concentration were systematically optimized. The NC-SCA photocatalyst exhibited high stability, retaining around 85% efficiency after seven cycles. This study presents an innovative strategy for designing high-performance photocatalysts addressing the limitations of conventional materials.
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Affiliation(s)
- Shabnam Sambyal
- School
of Advanced Chemical Sciences, Shoolini
University, Solan, HP 173229, India
| | - Rohit Sharma
- School
of Advanced Chemical Sciences, Shoolini
University, Solan, HP 173229, India
| | - Parteek Mandyal
- School
of Advanced Chemical Sciences, Shoolini
University, Solan, HP 173229, India
| | - Vinay Chauhan
- School
of Advanced Chemical Sciences, Shoolini
University, Solan, HP 173229, India
| | - Aashish Priye
- Department
of Chemical and Environmental Engineering, University of Cincinnati, Cincinnati, Ohio 45221, United States
| | - Manish Kumar
- Department
of Chemistry and Chemical Sciences, Central
University of Himachal Pradesh, Dharamshala, Shahpur, Kangra, HP 176206, India
| | - Pooja Shandilya
- Department
of Chemical and Environmental Engineering, University of Cincinnati, Cincinnati, Ohio 45221, United States
- Department
of Chemistry, MMEC, Maharishi Markandeshwar
(Deemed to be University), Mullana-Ambala, Haryana 133207, India
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3
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Kanwar B, Koli M, Singh SP. Antibiotic amoxicillin degradation by electrochemical oxidation process: effects of process parameters and degradation pathway at environmentally relevant concentrations. ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH INTERNATIONAL 2025; 32:575-586. [PMID: 39695035 DOI: 10.1007/s11356-024-35780-8] [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: 08/20/2024] [Accepted: 12/09/2024] [Indexed: 12/20/2024]
Abstract
Amoxicillin (AMX) is a common antibiotic used in both human and veterinary medicine in order to both cure and avoid bacterial infections. Traces of AMX have been found in ground and surface water, urban effluents, water, and wastewater treatment facilities due to its widespread use. The level of hazard and disposal of this class of micropollutants is the reason for concern. Advanced technology is required since conventional wastewater treatment plants are ineffective at eliminating these emerging contaminants. Electrochemical oxidation is a promising method of treating wastewater, which uses electrogenerated radicals to mineralize organic pollutants. This work investigated the detailed process mechanism for AMX degradation utilizing a low-cost, thin, flexible graphite sheet with lower AMX concentrations, initial pH value, voltage, electrolyte concentration, and wastewater matrix. The degradation of AMX by in situ generated hydroxyl radicals is a function of applied voltage and follows pseudo-first-order reaction kinetics. The removal efficiencies of AMX have been achieved up to 99% within 3 h. Moreover, intermediate by-products have been identified using liquid chromatography-mass spectrometry, and a plausible pathway has been proposed. This study could serve as a process reference for controlling AMX wastewater contamination via the electrochemical oxidation technique.
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Affiliation(s)
- Bhavana Kanwar
- Environmental Science and Engineering Department (ESED), Indian Institute of Technology Bombay, Mumbai, 400076, India
| | - Mitil Koli
- Environmental Science and Engineering Department (ESED), Indian Institute of Technology Bombay, Mumbai, 400076, India
| | - Swatantra P Singh
- Environmental Science and Engineering Department (ESED), Indian Institute of Technology Bombay, Mumbai, 400076, India.
- Centre for Research in Nanotechnology & Science (CRNTS), Indian Institute of Technology Bombay, Mumbai, 400076, India.
- Centre of Climate Studies, Indian Institute of Technology Bombay, Mumbai, 400076, India.
- Centre of Excellence On Membrane Technologies for Desalination, Brine Management, and Water Recycling (DesaltM), Indian Institute of Technology Bombay, Mumbai, 400076, India.
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4
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Sikorski Ł, Bęś A, Warmiński K, Truszkowski W, Kowal P. Utilizing Morphological and Physiological Parameters of Lemna minor for Assessing Tetracyclines' Removal. Molecules 2024; 29:3971. [PMID: 39203049 PMCID: PMC11356931 DOI: 10.3390/molecules29163971] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Grants] [Track Full Text] [Figures] [Journal Information] [Subscribe] [Scholar Register] [Received: 05/21/2024] [Revised: 06/15/2024] [Accepted: 08/20/2024] [Indexed: 09/03/2024] Open
Abstract
Antibiotics with significant environmental toxicity, e.g., tetracyclines (TCs), are often used in large quantities worldwide, with 50-80% of the applied dose ending up in the environment. This study aimed to investigate the effects of exposure to tetracycline hydrochloride (TC) and minocycline hydrochloride (MIN) on L. minor. Our research evaluated the phytotoxicity of the TCs by analyzing plant growth and biomass and evaluating assimilation pigment levels and fluorescence. The research was extended with the ability potential of duckweed as a tool for removing TCs from water/wastewater. The results demonstrated that both TCs influenced Ir, Iy, biomass, and photosynthetic efficiency. The uptake of TC and MIN by duckweed was proportional to the concentration in the growth medium. The TC was absorbed more readily, reaching up to 8.09 mg × g-1 of dry weight (DW) at the highest concentration (19.2 mg × L-1), while MIN reached 6.01 mg × g-1 of DW. As indicated, the consequences of the influence of TC on plants were slightly smaller, in comparison to MIN, while the plants could biosorb this drug, even at the lowest tested concentration. This study has shown that using plants for drug biosorption can be an effective standalone or complementary method for water and wastewater treatment.
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Affiliation(s)
- Łukasz Sikorski
- Department of Chemistry, Faculty of Agriculture and Forestry, University of Warmia and Mazury in Olsztyn, Pl. Łódzki 4, 10-727 Olsztyn, Poland; (A.B.); (K.W.)
| | - Agnieszka Bęś
- Department of Chemistry, Faculty of Agriculture and Forestry, University of Warmia and Mazury in Olsztyn, Pl. Łódzki 4, 10-727 Olsztyn, Poland; (A.B.); (K.W.)
| | - Kazimierz Warmiński
- Department of Chemistry, Faculty of Agriculture and Forestry, University of Warmia and Mazury in Olsztyn, Pl. Łódzki 4, 10-727 Olsztyn, Poland; (A.B.); (K.W.)
| | - Wojciech Truszkowski
- Department of Agrotechnology and Agribusiness, Faculty of Agriculture and Forestry, University of Warmia and Mazury in Olsztyn, M. Oczapowskiego 8, 10-719 Olsztyn, Poland;
| | - Przemysław Kowal
- Department of Sanitary Engineering, Faculty of Civil and Environmental Engineering, Gdansk University of Technology, Narutowicza 11/12, 80-233 Gdansk, Poland;
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5
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Wang Z, Zhang L, Su R, Yang L, Xiao F, Chen L, He P, Yang D, Zeng Y, Zhou Y, Wan Y, Tang B. PANI/GO and Sm co-modified Ti/PbO 2 dimensionally stable anode for highly efficient amoxicillin degradation: Performance assessment, impact parameters and degradation mechanism. JOURNAL OF ENVIRONMENTAL MANAGEMENT 2024; 364:121435. [PMID: 38889646 DOI: 10.1016/j.jenvman.2024.121435] [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: 02/09/2024] [Revised: 05/22/2024] [Accepted: 06/07/2024] [Indexed: 06/20/2024]
Abstract
The abuse and uncontrolled discharge of antibiotics present a severe threat to environment and human health, necessitating the development of efficient and sustainable treatment technology. In this work, we employ a facile one-step electrodeposition method to prepare polyaniline/graphite oxide (PANI/GO) and samarium (Sm) co-modified Ti/PbO2 (Ti/PbO2-PANI/GO-Sm) electrode for the degradation of amoxicillin (AMX). Compared with traditional Ti/PbO2 electrode, Ti/PbO2-PANI/GO-Sm electrode exhibits more excellent oxygen evolution potential (2.63 V) and longer service life (56 h). In degradation experiment, under optimized conditions (50 mg L-1 AMX, 20 mA cm-2, pH 3, 0.050 M Na2SO4, 25 °C), Ti/PbO2-PANI/GO-Sm electrode achieves remarkable removal efficiencies of 88.76% for AMX and 79.92% for chemical oxygen demand at 90 min. In addition, trapping experiment confirms that ·OH plays a major role in the degradation process. Based on theoretical calculation and liquid chromatography-mass spectrometer results, the heterocyclic portion of AMX molecule is more susceptible to ·OH attacks. Thus, this novel electrode offers a sustainable and efficient solution to address environmental challenges posed by antibiotic-contaminated wastewater.
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Affiliation(s)
- Zeyi Wang
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China
| | - Luyao Zhang
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China
| | - Rong Su
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China; School of Science, Xichang University, Xichang, 615000, PR China
| | - Lu Yang
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China
| | - Feng Xiao
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China
| | - Lichuan Chen
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China
| | - Ping He
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China; International Science and Technology Cooperation Laboratory of Micro-nanoparticle Application Research, Southwest University of Science and Technology, Mianyang, 621010, PR China.
| | - Dingming Yang
- School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, 621010, PR China.
| | - Yali Zeng
- Sichuan Mianyang 404 Hospital, Mianyang, 621000, PR China
| | - Yun Zhou
- Sichuan Mianyang 404 Hospital, Mianyang, 621000, PR China.
| | - Ying Wan
- School of Basic Medical Sciences, Southwest Medical University, Luzhou, 646000, PR China
| | - Bin Tang
- School of Basic Medical Sciences, Southwest Medical University, Luzhou, 646000, PR China.
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6
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Singh PP, Pandey G, Murti Y, Gairola J, Mahajan S, Kandhari H, Tivari S, Srivastava V. Light-driven photocatalysis as an effective tool for degradation of antibiotics. RSC Adv 2024; 14:20492-20515. [PMID: 38946773 PMCID: PMC11208907 DOI: 10.1039/d4ra03431g] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Track Full Text] [Download PDF] [Figures] [Journal Information] [Subscribe] [Scholar Register] [Received: 05/09/2024] [Accepted: 06/22/2024] [Indexed: 07/02/2024] Open
Abstract
Antibiotic contamination has become a severe issue and a dangerous concern to the environment because of large release of antibiotic effluent into terrestrial and aquatic ecosystems. To try and solve these issues, a plethora of research on antibiotic withdrawal has been carried out. Recently photocatalysis has received tremendous attention due to its ability to remove antibiotics from aqueous solutions in a cost-effective and environmentally friendly manner with few drawbacks compared to traditional photocatalysts. Considerable attention has been focused on developing advanced visible light-driven photocatalysts in order to address these problems. This review provides an overview of recent developments in the field of photocatalytic degradation of antibiotics, including the doping of metals and non-metals into ultraviolet light-driven photocatalysts, the formation of new semiconductor photocatalysts, the advancement of heterojunction photocatalysts, and the building of surface plasmon resonance-enhanced photocatalytic systems.
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Affiliation(s)
- Praveen P Singh
- Department of Chemistry, United College of Engineering & Research Prayagraj U.P.-211010 India
| | - Geetika Pandey
- Department of Physics, Faculty of Science, United University Prayagraj-211012 India
| | - Yogesh Murti
- Institute of Pharmaceutical Research, GLA University Mathura-281406 India
| | - Jagriti Gairola
- School of Pharmacy, Graphic Era Hill University Clement Town Dehradun 248002 Uttarakhand India
- Department of Allied Sciences, Graphic Era (Deemed to be University) Clement Town Dehradun 248002 Uttarakhand India
| | - Shriya Mahajan
- Centre of Research Impact and Outcome, Chitkara University Rajpura-140417 Punjab India
| | - Harsimrat Kandhari
- Chitkara Centre for Research and Development, Chitkara University Himachal Pradesh-174103 India
| | - Shraddha Tivari
- Department of Chemistry, CMP Degree College, University of Allahabad Prayagraj U.P.-211002 India
| | - Vishal Srivastava
- Department of Chemistry, CMP Degree College, University of Allahabad Prayagraj U.P.-211002 India
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7
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Qutob M, Alshehri S, Shakeel F, Alam P, Rafatullah M. An insight into the role of experimental parameters in advanced oxidation process applied for pharmaceutical degradation. ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH INTERNATIONAL 2024; 31:26452-26479. [PMID: 38546921 DOI: 10.1007/s11356-024-33040-3] [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: 12/12/2023] [Accepted: 03/18/2024] [Indexed: 05/04/2024]
Abstract
The advanced oxidation process (AOP) is an efficient method to treat recalcitrance pollutants such as pharmaceutical compounds. The essential physicochemical factors in AOP experiments significantly influence the efficiency, speed, cost, and safety of byproducts of the treatment process. In this review, we collected recent articles that investigated the elimination of pharmaceutical compounds by various AOP systems in a water medium, and then we provide an overview of AOP systems, the formation mechanisms of active radicals or reactive oxygen species (ROS), and their detection methods. Then, we discussed the role of the main physicochemical parameters (pH, chemical interference, temperature, catalyst, pollutant concentration, and oxidant concentration) in a critical way. We gained insight into the most frequent scenarios for the proper and improper physicochemical parameters for the degradation of pharmaceutical compounds. Also, we mentioned the main factors that restrict the application of AOP systems in a commercial way. We demonstrated that a proper adjustment of AOP experimental parameters resulted in promoting the treatment performance, decreasing the treatment cost and the treatment operation time, increasing the safeness of the system products, and improving the reaction stoichiometric efficiency. The outcomes of this review will be beneficial for future AOP applicants to improve the pharmaceutical compound treatment by providing a deeper understanding of the role of the parameters. In addition, the proper application of physicochemical parameters in AOP systems acts to track the sustainable development goals (SDGs).
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Affiliation(s)
- Mohammad Qutob
- Environmental Technology Division, School of Industrial Technology, Universiti Sains Malaysia, 11800, Penang, Malaysia
| | - Sultan Alshehri
- Department of Pharmaceutical Sciences, College of Pharmacy, AlMaarefa University, 13713, Diriyah, Riyadh, Saudi Arabia
| | - Faiyaz Shakeel
- Department of Pharmaceutics, College of Pharmacy, King Saud University, 11451, Riyadh, Saudi Arabia
| | - Prawez Alam
- Department of Pharmacognosy, College of Pharmacy, Prince Sattam Bin Abdulaziz University, 11942, Al-Kharj, Saudi Arabia
| | - Mohd Rafatullah
- Environmental Technology Division, School of Industrial Technology, Universiti Sains Malaysia, 11800, Penang, Malaysia.
- Renewable Biomass Transformation Cluster, School of Industrial Technology, Universiti Sains Malaysia, 11800, Penang, Malaysia.
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8
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Jiang T, Chai J, Wang Y, Du Q, Shi J, Xu Z. Enhanced photocatalytic reduction of Cr(VI) from aqueous solution using Fe 0/TiO 2-based polymeric nanocomposites. ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH INTERNATIONAL 2023; 30:110312-110323. [PMID: 37783998 DOI: 10.1007/s11356-023-30106-6] [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: 07/24/2023] [Accepted: 09/23/2023] [Indexed: 10/04/2023]
Abstract
The combination of zerovalent iron (Fe0) and titanium dioxide (TiO2) has been investigated as a promising method for environmental remediation. However, it is a challenge to prepare conveniently desirable Fe0/TiO2 nanocomposites with excellent efficiency and reusability. Here, a novel nanocomposite material, Fe0/TiO2@D201, was synthesized to enhance the removal of Cr(VI) from an aqueous system by impregnating Fe0 and TiO2 inside a commercial anion exchanger (D201). The proposed structure and Cr(VI) removal mechanism of Fe0/TiO2@D201 were confirmed using scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) analysis. Compared to the monometallic samples (Fe0-D201 and TiO2-D201), Fe0/TiO2@D201 showed outstanding Cr(VI) removal and the removal ratio reached up to 97.30% after 120 min of UV light irradiation. The removal of Cr(VI) by Fe0/TiO2@D201 remained high (91.70%) even after four cycles, indicating the stability of the nanocomposites toward Cr(VI) removal and their strong potential for practical applications. The addition of ethylenediaminetetraacetic acid (EDTA) positively affected the Cr(VI) reduction process, whereas the addition of Na2S2O8 negatively affected the Cr(VI) process. The XPS results revealed that the photocatalytic reduction of Cr(VI) by Fe0/TiO2@D201 involved the capture of photoexcited electrons and Fe0 reduction. A path for the photogenerated electrons engaging in the reduction reaction to improve the utilization of Fe0 was proposed. These results demonstrate that Fe0/TiO2@D201 is a promising alternative composite catalyst for the efficient Cr(VI) removal from contaminated water.
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Affiliation(s)
- Ting Jiang
- School of Engineering, China Pharmaceutical University, Nanjing, 211198, People's Republic of China
| | - Jian Chai
- School of Engineering, China Pharmaceutical University, Nanjing, 211198, People's Republic of China
| | - Yingying Wang
- School of Engineering, China Pharmaceutical University, Nanjing, 211198, People's Republic of China
| | - Qiong Du
- School of Engineering, China Pharmaceutical University, Nanjing, 211198, People's Republic of China.
| | - Jing Shi
- School of Engineering, China Pharmaceutical University, Nanjing, 211198, People's Republic of China
- State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, People's Republic of China
| | - Zhengwen Xu
- Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Nanjing, 210044, People's Republic of China
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Liu M, Ye Y, Xu L, Gao T, Zhong A, Song Z. Recent Advances in Nanoscale Zero-Valent Iron (nZVI)-Based Advanced Oxidation Processes (AOPs): Applications, Mechanisms, and Future Prospects. NANOMATERIALS (BASEL, SWITZERLAND) 2023; 13:2830. [PMID: 37947676 PMCID: PMC10647831 DOI: 10.3390/nano13212830] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Abstract] [Key Words] [Track Full Text] [Subscribe] [Scholar Register] [Received: 09/05/2023] [Revised: 10/19/2023] [Accepted: 10/23/2023] [Indexed: 11/12/2023]
Abstract
The fast rise of organic pollution has posed severe health risks to human beings and toxic issues to ecosystems. Proper disposal toward these organic contaminants is significant to maintain a green and sustainable development. Among various techniques for environmental remediation, advanced oxidation processes (AOPs) can non-selectively oxidize and mineralize organic contaminants into CO2, H2O, and inorganic salts using free radicals that are generated from the activation of oxidants, such as persulfate, H2O2, O2, peracetic acid, periodate, percarbonate, etc., while the activation of oxidants using catalysts via Fenton-type reactions is crucial for the production of reactive oxygen species (ROS), i.e., •OH, •SO4-, •O2-, •O3CCH3, •O2CCH3, •IO3, •CO3-, and 1O2. Nanoscale zero-valent iron (nZVI), with a core of Fe0 that performs a sustained activation effect in AOPs by gradually releasing ferrous ions, has been demonstrated as a cost-effective, high reactivity, easy recovery, easy recycling, and environmentally friendly heterogeneous catalyst of AOPs. The combination of nZVI and AOPs, providing an appropriate way for the complete degradation of organic pollutants via indiscriminate oxidation of ROS, is emerging as an important technique for environmental remediation and has received considerable attention in the last decade. The following review comprises a short survey of the most recent reports in the applications of nZVI participating AOPs, their mechanisms, and future prospects. It contains six sections, an introduction into the theme, applications of persulfate, hydrogen peroxide, oxygen, and other oxidants-based AOPs catalyzed with nZVI, and conclusions about the reported research with perspectives for future developments. Elucidation of the applications and mechanisms of nZVI-based AOPs with various oxidants may not only pave the way to more affordable AOP protocols, but may also promote exploration and fabrication of more effective and sustainable nZVI materials applicable in practical applications.
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Affiliation(s)
- Mingyue Liu
- School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, China
- Engineering Research Center of Recycling & Comprehensive Utilization of Pharmaceutical and Chemical Waste of Zhejiang Province, Taizhou University, Taizhou 318000, China
| | - Yuyuan Ye
- School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, China
| | - Linli Xu
- School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, China
| | - Ting Gao
- School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, China
| | - Aiguo Zhong
- School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, China
| | - Zhenjun Song
- School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, China
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10
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Alaydaroos AH, Sydorenko J, Palanisamy S, Chiesa M, Al Hajri E. Efficient photoelectrocatalytic degradation of amoxicillin using nano-TiO 2 photoanode thin films: A comparative study with photocatalytic and electrocatalytic methods. CHEMOSPHERE 2023; 339:139629. [PMID: 37495042 DOI: 10.1016/j.chemosphere.2023.139629] [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: 05/29/2023] [Revised: 07/13/2023] [Accepted: 07/21/2023] [Indexed: 07/28/2023]
Abstract
Excessive utilization of antibiotics in human, animal, and aquaculture poses a substantial threat to human health and the environment. Photoelectrochemical processes are increasingly applied for water remediation because they generate oxidizing species and mineralize organic pollutants, making even small water quantities more amenable for utilization. Thus, this study presents the fabrication of an efficient nano-TiO2 photoanode thin film (PATF) specifically designed for the photoelectrocatalytic (PEC) degradation of amoxicillin (AMX). The TiO2 PATFs were deposited on fluorine-doped tin oxide (FTO) substrate using an ultrasonic spray pyrolysis process with various titanium isopropoxide (TTIP) acetylacetone (AcacH) molar ratios (1:1 to 1:10). The PEC oxidation of AMX was investigated using various molar ratios of TTIP:AcacH TiO2 PATF/FTO by linear sweep voltammetry, and a 1:8 M ratio of PATF exhibited superior PEC oxidation activity than other TiO2 PATFs. Subsequently, the PEC degradation efficiency of AMX was compared with that of photocatalytic (PC) and electrocatalytic (EC) methods. The results demonstrated that the PEC process effectively eliminated 76.2% of AMX within 120 min at 0.8 V, outperforming the removal rates attained by the EC (32.3%) and PC (52.6%). Notably, increasing the voltage to 1.0 V accelerated the PEC degradation of AMX, attaining a removal efficiency of 91.2% within 90 min and exceeding 95% within 120 min.
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Affiliation(s)
- Alia Husain Alaydaroos
- Laboratory for Energy and Nano Science (LENS), Masdar Campus, Khalifa University, Abu Dhabi, United Arab Emirates
| | - Jekaterina Sydorenko
- Tallinn University of Technology, Department of Materials and Environmental Technology, Ehitajate tee 5, 19086, Tallinn, Estonia
| | - Selvakumar Palanisamy
- Laboratory for Energy and Nano Science (LENS), Masdar Campus, Khalifa University, Abu Dhabi, United Arab Emirates.
| | - Matteo Chiesa
- Laboratory for Energy and Nano Science (LENS), Masdar Campus, Khalifa University, Abu Dhabi, United Arab Emirates; ARC-Arctic Centre for Sustainable Energy, Department of Physics and Technology, UiT The Arctic University of Norway, 9010, Tromsø, Norway.
| | - Ebrahim Al Hajri
- Laboratory for Energy and Nano Science (LENS), Masdar Campus, Khalifa University, Abu Dhabi, United Arab Emirates
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Diao FM, Chen ML, Tong LY, Chen YN, Diao ZH. A green synthesized medicine residue carbon-based iron composite for the removal of chromium (VI) and cadmium (II): Performance, kinetics and mechanism. ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH INTERNATIONAL 2023; 30:84011-84022. [PMID: 37355513 DOI: 10.1007/s11356-023-28429-5] [Citation(s) in RCA: 1] [Impact Index Per Article: 0.5] [Reference Citation Analysis] [Abstract] [Key Words] [MESH Headings] [Grants] [Track Full Text] [Subscribe] [Scholar Register] [Received: 12/19/2022] [Accepted: 06/21/2023] [Indexed: 06/26/2023]
Abstract
Nowadays, clean-up of heavy metals from wastewaters using waste residue carbon-based material has received increasing attention. In this work, a novel Chinese medicine residue carbon-based nano zero-valent iron composite (CM-nZVI) had been successfully prepared using the combined Chinese medicine residue, FeCl3 and green tea extract. Cr(VI) and/ or Cd(II) removal in water by the CM-nZVI were systematacially investigated with a series of batch experiments. The most relevant findings indicated the adsorption efficiecy and capacity of Cr(VI) by CM-nZVI were respecitvely nearly 98% and 26 mg/g under optimized reaction conditions. The negative influences of the cations on the Cr(VI) removal followed the order of Al3+ > Ca2+ > Mg2+ Na+ > K+, but the anions followed the order of HCO3- > PO43- > NO3- > Cl- > SO42-. Humic acid (HA) and ionic strength with high concentrations severely inhibited Cr(VI) removal. The Cr(VI) adsorption on CM-nZVI fitted well by the pseudo-second-order kinetic and Langmuir models. A monolayer endothermic chemisorption occurred on Cr(VI) adsorption over CM-nZVI, and Cr(VI) removal by CM-nZVI primarily involved in the absorption, reduction, precipitation and complexation processes. Both Cr(VI) and Cd(II) removals had been achieved by CM-nZVI at their low concentrations. This CM-nZVI showed a better reusability proprity for Cr(VI) and Cd(II) removal with the regeneration of CM-nZVI through simple pickling. The outcomes of this work show that CM-nZVI could be used an effective material for heavy metals removal from water.
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Affiliation(s)
- Fa-Ming Diao
- Guangdong Hospital of Traditional Chinese Medicine, Guangzhou, 510120, China
| | - Man-Li Chen
- College of Resources and Environment, Zhongkai University of Agriculture and Engineering, Guangzhou, 510225, China
| | - Lin-Yin Tong
- College of Resources and Environment, Zhongkai University of Agriculture and Engineering, Guangzhou, 510225, China
| | - Ying-Nan Chen
- College of Resources and Environment, Zhongkai University of Agriculture and Engineering, Guangzhou, 510225, China
| | - Zeng-Hui Diao
- College of Resources and Environment, Zhongkai University of Agriculture and Engineering, Guangzhou, 510225, China.
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Liu H, Fu P, Liu F, Hou Q, Tong Z, Bi W. Degradation of ciprofloxacin by persulfate activated with pyrite: mechanism, acidification and tailwater reuse. RSC Adv 2022; 12:29991-30000. [PMID: 36321107 PMCID: PMC9582745 DOI: 10.1039/d2ra05412d] [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: 08/29/2022] [Accepted: 10/05/2022] [Indexed: 11/25/2022] Open
Abstract
Residues of ciprofloxacin (CIP) in the environment pose a threat to human health and ecosystems. This study investigated the degradation of CIP by persulfate (PS) activated with pyrite (FeS2). Results showed that when [CIP] = 30 μM, [FeS2] = 2.0 g L-1, and [PS] = 1 mM, the CIP removal rate could reach 94.4% after 60 min, and CIP mineralization rate reached 34.9%. The main free radicals that degrade CIP were SO4˙- and HO˙, with contributions of 34.4% and 35.7%, respectively. Additionally, compared to the control (ultrapure water), CIP in both tap water and river water was not degraded. However, acidification could eliminate the inhibition of CIP degradation in tap water and river water. Furthermore, acidic tailwater from CIP degradation could be utilized to adjust the pH of untreated CIP, which could greatly promote the degradation of CIP and further reduce disposal costs. The reaction solution was not significantly biotoxic and three degradation pathways of CIP were investigated. Based on the above results and the characterization of FeS2, the mechanism of CIP degradation in the FeS2/PS system was that FeS2 activated PS to generate Fe(iii) and SO4˙-. The sulfide in FeS2 reduced Fe(iii) to Fe(ii), thus achieving an Fe(iii)/Fe(ii) cycle for CIP degradation.
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Affiliation(s)
- Hui Liu
- College of Resources and Environment, Shanxi Agricultural University Shanxi 030801 China
| | - Peng Fu
- College of Resources and Environment, Shanxi Agricultural University Shanxi 030801 China
| | - Fenwu Liu
- College of Resources and Environment, Shanxi Agricultural University Shanxi 030801 China
| | - Qingjie Hou
- College of Resources and Environment, Shanxi Agricultural University Shanxi 030801 China
| | - Zhenye Tong
- College of Resources and Environment, Shanxi Agricultural University Shanxi 030801 China
| | - Wenlong Bi
- College of Resources and Environment, Shanxi Agricultural University Shanxi 030801 China
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Sun S, Li S, Hao Y, Yang X, Dou X. Construction of g/C3N4-ZnO composites with enhanced visible-light photocatalytic activity for degradation of amoxicillin. KOREAN J CHEM ENG 2022. [DOI: 10.1007/s11814-022-1181-5] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Track Full Text] [Journal Information] [Subscribe] [Scholar Register] [Indexed: 11/24/2022]
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14
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fEffective degradation of amoxicillin by multi-stage flow-through electrochemical system using porous electrodes. Sep Purif Technol 2022. [DOI: 10.1016/j.seppur.2022.121832] [Citation(s) in RCA: 0] [Impact Index Per Article: 0] [Reference Citation Analysis] [Track Full Text] [Journal Information] [Subscribe] [Scholar Register] [Indexed: 11/20/2022]
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Liu W, Wang Y, Qi K, Wen F, Wang J. Broad Spectral Response Z-Scheme Three-Dimensional Ordered Macroporous Carbon Quantum Dots/TiO 2/g-C 3N 4 Composite for Boosting Photocatalysis. LANGMUIR : THE ACS JOURNAL OF SURFACES AND COLLOIDS 2022; 38:4839-4847. [PMID: 35420818 DOI: 10.1021/acs.langmuir.1c03483] [Citation(s) in RCA: 5] [Impact Index Per Article: 1.7] [Reference Citation Analysis] [Abstract] [Track Full Text] [Subscribe] [Scholar Register] [Indexed: 06/14/2023]
Abstract
Photocatalytic degradation technology is one of the effective protocols to solve environmental problems. TiO2 has always been favored for its photostability and low cost. However, the insufficient photocatalytic activity of TiO2 limits its application due to the severe recombination of photogenerated electrons and holes and a narrow light response range. Therefore, 3DTCN, a TiO2/g-C3N4 composite with a three-dimensional ordered macroporous structure was prepared by a colloidal crystal template technique to form a heterojunction for inhibiting the photogenerated electron-hole recombination. On 3DTCN, carbon quantum dots (CQDs) were loaded by impregnation to obtain x % CQDs/3DTCN with a broad spectral response to light. The physical and chemical properties of samples were investigated by X-ray diffraction, scanning electron microscopy, transmission electron microscopy (TEM), high-resolution-TEM, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, Brunauer-Emmett-Teller analysis, photoluminescence spectroscopy, and ultraviolet-visible diffuse reflectance spectroscopy. The photocatalytic activity was evaluated via degrading the rhodamine B (RhB) dye, and the degradation efficiency of 1% CQDs/3DTCN (98%) was found to be much higher than that of 3DTCN (42%) in 80 min under simulated sunlight irradiation. Furthermore, it also possessed excellent durability. Meanwhile, the sample also showed an outstanding photoelectric property. Finally, the proposed mechanism of the composites had been mainly analyzed by density functional theory calculations. This work thus provides an idea to form a 3D structure heterojunction and further improve the photocatalytic activity.
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Affiliation(s)
- Wenliang Liu
- College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
| | - Yan Wang
- College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
| | - Kai Qi
- College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
| | - Fushan Wen
- College of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, China
| | - Jiqian Wang
- College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
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Yang K, Liu M, Weng X, Owens G, Chen Z. Fenton-like oxidation for the simultaneous removal of estrone and β-estradiol from wastewater using biosynthesized silver nanoparticles. Sep Purif Technol 2022. [DOI: 10.1016/j.seppur.2021.120304] [Citation(s) in RCA: 4] [Impact Index Per Article: 1.3] [Reference Citation Analysis] [Track Full Text] [Journal Information] [Subscribe] [Scholar Register] [Indexed: 01/23/2023]
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