Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Zhaoyi Han,Hao Shi,Wentao Qiu,Dongdong Zhu,Wei Li,Dihua Wang
The excessive use of antibiotics like sulfamethoxazole (SMX) is causing environmental pollution and endangering human health and the ecosystem. Using transition metals as catalysts to activate persulfate (PS) can effectively degrade the organic pollutants in the advanced oxidation process (AOP). However, the high dissolution of the transition metals leads to poor stability, low efficiency in pollutant degradation, and secondary pollution. In this work, a graphitized carbon encapsulated Co (Co@EC) anode is developed for electrochemically activating peroxymonosulfate (PMS) to degrade SMX. It is found that the synergistic effect of Co@EC, PMS, and current significantly enhances SMX degradation. Under optimal conditions (current density of 5 mA cm −2 , pH of 9, and PMS concentration of 0.25 mM), the Co@EC anode can completely remove 10 μM of SMX in 9 min, a much higher efficiency compared to processes without PMS, Co, or current. The rapid reaction kinetics (6.69×10 −1 min −1 ) at optimal conditions are associated with the two main active species of 1 O 2 and O 2 • − during electroactivation. Furthermore, the Co@EC anode maintains high degradation efficiency and low dissolution after repeated cycling tests due to its structural stability. These findings provide new insights and strategies for developing stable catalysts.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Zhikang Deng,Yongfei Ma,Jinyao Zhu,Chenyu Zeng,Rui Mu,Zulin Zhang
Conventional electrochemical activation of peroxymonosulfate (PMS) is not very cost-effective and practical by the excessive input of energy. The electricity generated by photosynthetic microalgae fuel cells (MFCs) is utilized to activate PMS, which would achieve the combination of green bioelectricity and advanced oxidation processes for sustainable pollutants degradation. In this study, a novel dual-chamber of MFCs was constructed by using microalgae as anode electron donor and PMS as cathode electron acceptor, which was operating under both close-circuit and open-circuit conditions. Under close-circuit condition, 1–12 mM PMS in cathode was successfully in situ activated, where 32.00%–99.83% of SMX was removed within 24 h, which was about 1.21–1.78 times of that in the open-circuit of MFCs. Meanwhile, a significant increase in bioelectricity generation in MFCs was observed after the accumulation of microalgae biomass (4.65–5.37 mg/L), which was attributed to the efficient electron separation and transfer. Furthermore, the electrochemical analysis demonstrated that SMX or its products were functioned as electronic shuttles, facilitating the electrochemical reaction and altering the electrical capacitance. The quenching experiments and voltage output results reflected that complex active radical (SO 4 ⋅ - , ⋅OH, and 1 O 2 ) were involved in SMX removal. Seven degradation products of SMX were detected and S–N bond cleavage was the main degradation pathway. Predicted toxicity values calculated by ECOSAR program showed that all the products were less toxic or nontoxic. Finally, the density functional theory (DFT) calculations revealed that the O and N atoms on SMX were more susceptible to electrophilic reactions, which were more vulnerable to be attacked by reactive species. This study provided new insights into the activation of PMS by bioelectricity for SMX degradation, proposing the mechanisms for PMS activation and degradation sites of SMX.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Xiangzhi Wang,Jing Wang,Zelong Li,Muhan Yang,Arbaz Rehman
Pharmaceuticals and personal care products (PPCPs), known for their severe ecological risks, are frequently detected in coastal waters worldwide. However, the environmental fate in marine systems remains poorly understood. This study investigated the co-metabolic degradation mechanism of a typical PPCP, sulfamethoxazole (SMX), by a marine consortium SAB using alginate—a natural organic matter—as a co-substrate, aiming to elucidate the biodegradation process of PPCPs in actual marine environments. An integrated approach, including metagenomic sequencing (with binning), RT-qPCR, molecular docking, metabolic modeling, and metabolomics, was employed. Results demonstrated that the SAB consortium efficiently degraded SMX at concentrations from 50 μg/L to 10 mg/L, achieving over 96% removal within 24 h. SMX degradation was achieved through metabolic cross-feeding of alginate by key species within the SAB consortium. Specifically, alginate is initially converted by Vibrio into the central metabolite 2-keto-3-deoxy-D-gluconate (KDG). KDG is subsequently metabolized by Tritonibacter , Halopseudomonas , and Vibrio , generating key metabolites such as acetyl-CoA, serine, cysteine, and guanine. These metabolites support microbial growth and induce production of SMX-degrading enzymes, such as threonine dehydratase, cysteine S-conjugate β-lyase, and guanine deaminase, leading to SMX cleavage and mineralization. Additionally, acetyl-CoA provides acetyl groups for arylamine N-acetyltransferase-mediated SMX acetylation. These processes collectively drive the co-metabolic degradation of SMX. Overall, this study provides critical insights into PPCPs' fate in marine environments.
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CARBOHYDRATE POLYMERS
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2012
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IF 3.628
Qiu Huamin,Fan Lulu,Xiangjun Li,Leilei Li,Sun Min,Luo Chuannan
A novel flow injection chemiluminescence (FI-CL) sensor for the determination of sulfamethoxazole (SMZ) was established which using chitosan/graphene oxide-molecularly imprinted polymers (CG-MIP) as recognition element. The SMZ-CG-MIP was synthesized in acetone as solvent and chitosan/graphene oxide for support, using acrylamide as functional monomer, ethylene glycol dimethacrylate as cross-linker and 2,2-azobisisobutyronitrile as initiator. The CG-MIP showed satisfactory recognition capacity for the SMZ. Then the synthesized CG-MIP was employed as recognition by packing into a lab-made tube connected in FI-CL analyzer to establish a novel CL sensor respectively. The CL intensity responded linearly to the concentration of SMZ in the range 1.0 × 10 −7 mol/L to 2.3 × 10 −3 mol/L with a detection limit of 2.9 × 10 −8 mol/L (3 σ ), which is lower. The relative standard deviation for the determination of 4.0 × 10 −4 mol/L of SMZ was 1.92% ( n = 11). The sensor is reusable and has a great improvement in sensitivity and selectivity for CL analysis which applied to the determination of SMZ in drug samples.
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ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2025
·Vol. 47
·期 2
·1-12
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IF 3.8
Guan Qianhui,Shu Xiao,Wu Wensheng,Zhang Yue,Wang Chenhui,Li Mingfu,Liang Ni,Chen Quan
The coexistence and interaction of free metal cations in the environment can significantly affect the migration of organic pollutants, leading to varied effects depending on environmental conditions. However, the mechanisms affecting the adsorption of organic pollutants in the presence of metal ions remain poorly understood due to limited molecular-level studies. This study investigated the adsorption behavior of sulfamethoxazole (SMX) on montmorillonite (MT) at different pH values (1.6, 3.0, and 5.0) in the presence of three metal cations with different valences: Na + , Ca 2+ , and Cr 3+ . At pH 5.0, the adsorption of SMX by MT at pH 5.0 in Ca 2+ and Cr 3+ systems increased significantly—by 7.25 times and 47 times, respectively, compared to those at pH 1.6. In contrast, Na + had a less pronounced effect on SMX adsorption. Density functional theory (DFT) calculations indicated that as the pH value increases, the interaction between SMX, metal ions, and MT strengthens. Furthermore, the adsorption binding energy of SMX in the high-valence Cr 3+ system (− 94.51 kcal/mol) was significantly lower than in the low-valence Na + system (− 36.55 kcal/mol). As pH and cation valency increased, the bonding density of cation bridges also increased, leading to a more substantial enhancement in SMX adsorption. This study provides insights into the adsorption mechanism of SMX on MT in the presence of metal cations, contributing valuable understanding of the environmental behavior of organic pollutants under varying cationic conditions.
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Journal of Advanced Research
·
2026
·
IF 17.1
Hangjun Zhang,Hongmei Yang,Yongjian Shao,Xindi Ye,Xuetong Qu,Zhiquan Liu
Introduction Antibiotics are frequently detected in aquatic environments, and previous studies have explored antibiotic effects on aquatic organisms. However, the molecular mechanism linking sulfamethoxazole (SMX) and lipid metabolism in amphibians remains unclear. Objectives To assess the ecotoxicological mechanisms and environmental risk of SMX pollution. Methods Here, the effect of SMX on lipid metabolism was assessed in P. nigromaculata by screening typical symptoms, including substance contents, enzyme activities, and gene expression in lipid digestion, lipid synthesis, and lipid transport metabolism. This assessment was subsequently validated through molecular docking (MD), molecular dynamics simulation (MDS), and in vitro spectroscopic analysis. Additionally, to evaluate the role of peroxisome proliferator-activated receptors α (PPARα), frogs were exposure to 1 μM of PPARα antagonist GW6471 alone and in conjunction with concentrations of 10 μg/L SMX, over a duration of 21 days. Results SMX at environmentally relevant concentrations induced lipid metabolism disorder, evidenced by an increase in the hepatosomatic index and the accumulation of triglycerides and total cholesterol. Transcriptomic data identified PPARα as primary molecular targets, with both concentrations of SMX perturbing fatty acid metabolism and gene set enrichment analysis revealing enrichment in PPAR pathway. Subsequently, MD, MDS, and in vitro spectroscopic spectra further confirmed that SMX may bind directly to frog PPARα. To further assess the role of PPARα, the frog was exposed to SMX, a PPARα agonist (WY-14643) or co-exposed to SMX with a PPARα antagonist (GW6471) for 21 days. Antagonist co-exposures counteracted the increased lipid content altered by SMX, indicating that PPARα plays a key role in SMX-induced lipid metabolic disorder. Conclusion Our study revealed that exposure to SMX at environmentally relevant concentrations led to lipid metabolic disorder in frogs via PPARα, providing new insights into the potential hazards of antibiotics at environmentally relevant concentrations.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Hui Feng,Jiaxin Xu,Jieyu Xu,Hua Zou
Sulfamethoxazole (SMX), a widely detected antibiotic residue, threatens human health and ecosystems. For selective SMX removal, a green molecularly imprinted polymer (CD-MIP) was synthesized using β-cyclodextrin (β-CD) as functional monomer via a facile route, with comparative evaluation against conventional methacrylic acid-based MIP (MAA-MIP). Molecular conformation modeling and spectroscopic analysis revealed stronger SMX-β-CD binding, guiding polymer design. CD-MIP achieved both higher sorption capacity (8.02 mg/g) and imprinting factor (2.34) within 60 min compared to MAA-MIP (7.21 mg/g; 1.10). CD-MIP demonstrated eco-friendliness with minimal desorption, strong matrix interference resistance, and high SMX selectivity. Practical tests confirmed its high selectivity, underscoring its potential for safeguarding water supply security. Adsorption was driven by physisorption via hydrogen bonding, π-π and hydrophobic interactions, with imprinted sites playing a crucial role. The host-guest recognition capability of β-CD was preserved in CD-MIP, with diverse functional groups enabling efficient imprinting, and non-imprinted polymer controls could reduce template use. A comprehensive sustainability assessment incorporating green metrics, life cycle analysis and economic evaluation confirmed the environmental and economic viability. This work establishes β-CD-based molecular imprinting as a sustainable strategy that effectively combines inherent molecular recognition with environmental adaptability, offering a cost-effective solution for safeguarding water supply.
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CHEMOSPHERE
·
2023
·
IF 8.8
Dongdong Zhu,Fengyin Zhou,Yongsong Ma,Yu Xiong,Xiangyun Li,Wei Li,DiHua Wang
Electrochemically activating peroxydisulfate (PDS) to degrade organic pollutants is one of the most attractive advanced oxidation processes (AOPs) to address environmental issues , but the high cost, poor stability, and low degradation efficiency of the anode materials hinder their application. Herein, an economic, self-supporting, robust, and durable LiFe 5 O 8 on Fe substrate (Fe@LFO) anode is reported to degrade sulfamethoxazole (SMX). When PDS is electrochemically activated by the Fe@LFO anode, the degradation rate of SMX is significantly improved. It is found that hydroxyl radicals (•OH), superoxide radical (O 2 •– ), singlet oxygen ( 1 O 2 ), Fe(Ⅳ), activated PDS (PDS*), and direct electron transfer (DET) reactions synergistically contribute to the degradation of SMX, which can realize the degradation of SMX in four possible routes: cleavage of the isoxazole ring, hydroxylation of the benzene ring, oxidation of the aniline group, and cleavage of the S–N bond, as evidenced by a series of tests of radicals quenching, electron paramagnetic resonance (EPR), linear sweep voltammetry (LSV) and liquid chromatograph mass spectrometer (LC-MS). Furthermore, Fe@LFO has good structural stability, excellent cyclability and low degradation cost, demonstrating its great potential for practical applications. This work contributes to a stable and effective anode material in the field of AOPs.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Qibang Tong,Congyi Li,Guixin Wang,Yao Wang,Shuo Peng,Jihang Wang,Bo Lai,Yong Guo
The abuse of antibiotics has drawn wide attention owing to their potential risk in human health and ecosystem. As one of the most commonly used sulfonamide antibiotics, sulfamethoxazole (SMX) can hardly be removed by conventional wastewater treatment methods, and thus it has become one of the most frequently detected antibiotics in water environment. In this study, a new cobalt-based heterogeneous catalyst (Co-bHAP) was successfully prepared using the simple impregnation method with animal bone-derived hydroxyapatite (bHAP) as the support, and applied to activate peroxymonosulfate (PMS) for the degradation of SMX in water. The physicochemical properties of Co-bHAP catalyst were investigated by series of characterization methods, and the results showed that this catalyst has a rough and porous morphological structure, as well as homogeneously distributed active component, which is mainly in the form of Co 3 O 4 . The developed Co-bHAP can provide abundant reaction active sites and exhibit excellent catalytic activity and stability in PMS activation . The kinetic constant of Co-bHAP activating PMS to degrade SMX is up to 0.1524 min −1 , which is 4.5 times larger than that of bare Co 3 O 4 . The SMX (20 mg/L) degradation efficiency within 30 min in Co-bHAP/PMS system reached as high as 98.7% and still maintained at 86% after 5 times consecutive operation, with slight cobalt ions leaching less than 0.1 mg/L. Based on radical quenching experiment, electron paramagnetic resonance (EPR) test and XPS analysis, the reaction mechanism was proposed. The balance among Co 3+ / Co 2+ , O 2− /O 2 and PMS decomposition in Co-bHAP/PMS system ensured the continuous generation of sulfate radical (SO 4 •– ) and hydroxyl radical (HO • ), both of which are responsible for SMX degradation, while SO 4 •– plays a leading role. In addition, four possible pathways of SMX degradation were proposed according to the eight detected intermediate products. All the results suggested that this catalyst could have a promising potential in activating PMS to degrade sulfonamide antibiotic pollutants in water.
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REVIEWS ON ADVANCED MATERIALS SCIENCE
·
2023
·Vol. 62
·期 1
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IF 3.6
Yuchen Guan,Zhixin Ren,Yan Lang,Tianze Liu,Zhao Gong,Yuguang Lv
Graphite-carbon nitride (g-C 3 N 4 ) was prepared by thermocondensation, and g-C 3 N 4 /BiVO 4 material (GCB) and g-C 3 N 4 /CNTs composite material (GCC) were prepared by doping different contents of BiVO 4 and carbon nanotubes (CNTs) with g-C 3 N 4 samples, respectively. Then, BiVO 4 , CNTs, and g-C 3 N 4 samples with different contents were doped to prepare ternary composite material (GCBC). In the performance experiment, Sulfamethoxazole (SMZ) was used as degradation material to evaluate the photocatalytic performance of the prepared samples, and the degradation reaction kinetics equation, quadric cycle stability experiment, free radical capture, and intermediates identification were studied. The intermediates of photocatalytic degradation of SMZ were analyzed by high-performance liquid chromatography-mass spectrometry. From the experimental data, it can be seen that for SMZ solution, when the reaction time T = 0 min and retention time rt = 7.53 min, there is a peak corresponding to the substance with m / z [M + H] + of 254, which is judged as SMZ. At 20, 40, and 60 min, rt was 2.00, 7.06, and 9.57 min, indicating the presence of intermediates in the photocatalytic process. Experimental analysis shows that there are three intermediates of SMZ degradation by composite sample GCBC. In this work, three kinds of composite materials were successfully prepared, and a variety of characterization, SMZ as pollutants, test the photocatalytic performance of composite materials (GCB, GCC, and GCBC) samples, and elucidated the cyclic stability of the material, active species capture, and photocatalytic degradation mechanism.
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Agronomy-Basel
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2022
·Vol. 12
·期 2
·476
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IF 3.949
Gang Chu,Zifeng Han,Zimo Wang,Defeng Kong,Wenxiu Qin,Youbin Si,Guozhong Wang,Christian E. W. Steinberg
Massive biomass waste with lignocellulose components can be used to produce biochar for environmental remediation. However, the impact of lignocellulose pyrolysis on biochar structure in relation to the sorption mechanism of ionizable antibiotics is still poorly understood. In this paper, diverse techniques including thermogravimetric analysis and13C nuclear magnetic resonance were applied to investigate the properties of biochars as affected by the pyrolysis of cellulose and lignin in feedstock. Cellulose-derived biochars possessed more abundant groups than lignin-derived biochars, suggesting the greater preservation of group for cellulose during the carbonization. Higher sorption of sulfamethoxazole (SMX) was also observed by cellulose-derived biochars owing to hydrogen bond interaction. Sorption affinity gradually declined with the conversion aliphatic to aromatic carbon, whereas the enhanced specific surface area (SSA) subsequently promoted SMX sorption as evidenced by increased SSA-N2and SSA-CO2from 350 to 450 °C. The decreasedKd/SSA-N2values with increasing pH values implied a distinct reduction in sorption per unit area, which could be attributed to enhanced electrostatic repulsion. This work elucidated the role of carbon phases from thermal conversion of lignocellulose on the sorption performance for sulfonamide antibiotics, which will be helpful to the structural design of carbonaceous adsorbents for the removal of ionizable antibiotics.Keywords:biochar;lignocellulose pyrolysis;carbon phase;ionizable antibiotics;sorption mechanism
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CHEMOSPHERE
·
2021
·
IF 7.086
Jingyi Fu,Li Feng,Yongze Liu,Liqiu Zhang,Shuo Li
Electrochemical activation of peroxymonosulfate (PMS) at carbon cloth anode (E (Carbon cloth Anode)/PMS system) was investigated for sulfamethoxazole (SMX) degradation. The results indicated that PMS could be activated at carbon cloth anode during electrolysis, resulting in the improvement of SMX degradation. The degradation efficiency of SMX was facilitated with the higher PMS concentration and current density, respectively. The degradation rate constant of SMX increased with the rising pH from 3.6 to 6.0, and reached the highest value at pH 6.0, and then decreased with further increasing pH to 8.0. The presence of chloride ion (Cl − , 5–100 mM) significantly enhanced SMX degradation, while addition of humic acid (HA, 1–5 mgC L −1 ) inhibited SMX degradation. Addition of carbonate (HCO 3 − , 5–20 mM) had a negligible impact on SMX degradation. Small amounts of phosphate (PO 4 3− , 0–5 mM) could promote degradation, while a large amount of PO 4 3− (10–20 mM) inhibited the degradation. Moreover, the quenching experiments demonstrated that sulfate radical (SO 4 · − ), hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ) contributed to SMX degradation in E (Carbon cloth Anode)/PMS system. The degradation intermediates of SMX were identified by LC-MS/MS and the degradation pathways were deduced to be hydroxylation, the cleavage of S–N bond, and oxidation of aniline group. Moreover, the micronucleus test of Vicia faba root tips indicated that the E (Carbon Cloth Anode)/PMS system could reduce the genetic toxicity of SMX contaminated water to some extent.
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