SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Qun Yu,Yuhang Yang,Yan Xu,Yuqiao Wang,Qingdong Qin
The application of metal doping has emerged as a prominent approach for modifying transition-metal-based heterogeneous catalysts in activating peroxymonosulfate (PMS). Herein, silver-doped α-MnO 2 (Ag-α-MnO 2 ) was synthesized via a one-step hydrothermal approach and utilized for activating PMS to degrade sulfamethoxazole (SMX). The catalyst was systematically characterized and examined to determine that the efficient dispersion of Ag increased the specific surface area and pore volume of α-MnO 2 . The degradation experiments demonstrated that SMX could be efficiently degraded by a combination of PMS and Ag-α-MnO 2 within 60 min. The apparent kinetic rate constant was 0.039 min −1 , which was approximately ten times higher than that of α-MnO 2 . The impacts of external water conditions on catalytic performance and the stability of Ag-α-MnO 2 were subsequently investigated. Density functional theory calculations revealed that Ag as a crucial active center reduced the PMS adsorption energy, promoted electron transfer, and orchestrated electron distribution. EPR spectra, quenching experiments, electrochemical tests, and XPS analysis were performed to validate the radical and non-radical mechanisms, including SO 4 − , OH, O 2 − and 1 O 2 . The two redox cycles of Ag + /Ag 0 and Mn 4+ /Mn 3+ on the surface of Ag-α-MnO 2 contributed to the activation of PMS. Additionally, probable degradation pathways for SMX were presented. This study provides an initially valuable insight into the cooperative mechanism of PMS activation for SMX degradation employing Mn-based catalysts doped with precious metal silver.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yan Ding,Kangping Cui,Zhi Guo,Minshu Cui,Yihan Chen
In this study, manganese peroxidase (MnP) was applied to induce the in vitro oxidation of sulfamethoxazole (SMX). The results indicated that 87.04% of the SMX was transformed and followed first-order kinetics (k obs = 0.438 h −1 ) within 6 h when 40 U L −1 of MnP was added. The reaction kinetics were investigated under different conditions, including pH, MnP activity, and H 2 O 2 concentration. The active species Mn 3+ was responsible for the oxidation of SMX, and the Mn 3+ production rate was monitored to reveal the interaction among MnP, Mn 3+ , and SMX. By integrating the characterizations analysis of the MnP/H 2 O 2 system with the density functional theory (DFT) calculations, the proton-coupled electron transfer (PCET) process dominated the catalytic circle of MnP and the transformation of Mn 3+ . Additionally, possible oxidation pathways of SMX were proposed based on single-electron transfer mechanism, which primarily included the S–N bond cleavage, the C–S bond cleavage, and one electron loss without bond breakage. It was then transformed to hydrolysis, N–H oxidation, self-coupling, and carboxylic acid coupling products. This study provides insights into the atomic-level mechanism of MnP and the transformation pathways of sulfamethoxazole, which lays a significant foundation for the potential of MnP in wastewater treatment applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Langming Bai,Zihan Liu,Haorui Wang,Guibai Li,Heng Liang
Ferrous-activated peroxymonosulfate (PMS) is regarded as a promising technology to treat organic pollutants. However, the excessive sulfate anions generated in the oxidation process need to be considered with respect to their potential harm to the environment and human health. The removal of organic compounds and sulfate anions by Fe(II)/PMS oxidation coupled with nanofiltration (NF) was studied in this research. The mechanism of Fe(II)/PMS coupled with NF in natural organic matter (NOM) and sulfamethoxazole (SMX) removal were systematically investigated by comparison with single Fe(II)/PMS and NF treatments. The results demonstrated that the hybrid system showed better performance than the single treatments for both pollutants. High-performance size exclusion chromatography (HPSEC) analysis indicated that macromolecular organic matter in Songhua River water was broken down and converted into small fragments with a size of approximately hundreds of Da by Fe(II)/PMS oxidation. Zeta potential analysis showed that the zeta potential of the effluent decreased under the effect of Fe(III) and that some small organic molecules generated in the process of oxidation were negatively charged. The SMX removal experiment showed that Fe(II)/PMS oxidation played a leading role in SMX removal in the hybrid system. Moreover, a radical quenching experiment was conducted to explore the effects of SO 4 ·− and HO · on SMX degradation. Fe(II)/PMS treatment effectively alleviated membrane fouling and improved the flux behaviour, with a stable sulfate anion rejection rate of approximately 90% achieved by NF in the long term. These results suggested that Fe(II)/PMS coupled with NF could control membrane fouling, intercept sulfate anions and improve effluent quality, which provides a new strategy for water treatment.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Dong Hui Liang,Yongyou Hu
Little information is available regarding the kinetics, products, and pathways of simultaneous SMX degradation and Cd(II) immobilization from wastewater. In this study, a novel bacterium ( Achromobacter sp. L3) with SMX degradation and Cd(II) immobilization capabilities was isolated. The boundary conditions of SMX degradation were as follows: initial pH 6–8, temperature 25–30 °C, and SMX concentration 10–40 mg/L −1 . The boundary conditions of Cd(II) immobilization were as follows: initial pH 7–9, temperature 25–35 °C, and SMX concentration 10–30 mg/L −1 . The maximum SMX degradation and Cd(II) removal were 91.98% and 100%, respectively. The SMX degradation and Cd(II) immobilization data fitted well with the pseudo-first-order kinetic model, indicating that the two pollutants conform to the same degradation rule. Moreover, the microbial degradation , sediment adsorption, and intermediates identified in the experiments were used to explore the mechanisms of SMX and Cd(II) removal. These results indicate that microbial removal and sediment adsorption play equally important roles in Cd(II) immobilization; however, microbial degradation plays a decisive role in SMX degradation. Furthermore, the relationship between aerobic denitrification, SMX degradation, and Cd(II) immobilization was proposed. These results may provide valuable insights for treatment of wastewater polluted by antibiotics and heavy metals.
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ENVIRONMENTAL RESEARCH
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2021
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IF 6.498
Zhi-Ling Li,Di Cao,Cai-Hua Bai,Xiao-Jing Yao,Xiao-Qiu Lin,Si-Pei Wang,Jun Nan,Bin Liang,Li-Wei Li,Kai Sun,Ai-Jie Wang
The response of the denitrification community to long-term antibiotic exposure requires further investigation. Here, the significantly altered denitrifying community structure and function were observed by continuous exposure to 1 mg/L sulfamethoxazole (SMZ) or chlortetracycline (CTC) for 180 d in the expanded granular sludge bed reactors. Thaurea , positively correlated with SMZ and NO 3 − removal efficiency ( NrE ), was highly enriched in the SMZ-added reactor, while, Comamons and Acinetobacter were largely inhibited. The acute inhibited and then gradual-recovered NrE (87.17–90.38 %) was observed with highly expressed narG , indicating the adaptability of Thaurea to SMZ. However, the abundance of Thaurea and Comamonas greatly decreased, while Melioribacter and Acinetobacter were largely enriched in the CTC-added reactor. CTC created more serious and continuous inhibition of NO 3 − reduction ( NrE of 64.53–66.95 %), with lowly expressed narG . Improved NO 2 − reduction capacity was observed in both reactors (70.16–95.42 %) with highly expressed nirS and nosZ , revealing the adaptability of NO 2 − reduction populations to antibiotics.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2019
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IF 7.149
Qian Xiang,Dong Zhu,Qing-Lin Chen,Patrick O’Connor,Xiao-Ru Yang,Min Qiao,Yong-Guan Zhu
Microplastics pollution in the environment is now receiving worldwide attention; however, the effects of copollution of antibiotics and microplastics on the gut microbiome of globally distributed and functionally important nontarget soil animals remain poorly understood. We studied a model collembolan (Folsomia candida) and found that the ingestion of microplastics (polystyrene, 2–2.9 μm) substantially altered the gut microbiome, antibiotic resistance gene (ARG) profile, and the isotopic fractionation in the soil collembolan tissue. Importantly, collembolans exposed to polystyrene microplastics loaded with sulfamethoxazole (MA) presented a distinctive gut microbiome, ARG profile, and isotopic fractionation compared to those exposed to polystyrene alone (MH). We observed that the abundance of ARGs and mobile genetic elements (MGEs) in the MA-treated collembolan guts was significantly higher than in the MH and the control treatments. There were also strong interactions between the gut microbiome and ARGs in the collembolan guts. We further found that bacterial β-diversity correlated significantly with the δ13C and δ15N values in collembolan body tissues. Together, our results indicate that changes in isotopic fractionation and ARG profiles in the collembolan were induced by the changes in gut microbiota and suggest that microplastics from diverse sources may have profound influences on soil fauna and soil food webs.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Xiaolin Shen,Zhiliang Zhu,Xiaochang Liu,Renlu Qiao,Hua Zhang,Yanling Qiu
Reutilization of spent adsorbent by converting the adsorbed organic pollutants into carbon matrix has attracted more attention in recent years, which delivers a greener way for the preparation of catalysis and environment remediation. In this work, CuBi 2 O 4 after adsorption of pollutant sulfamethazine was further transformed to a photocatalyst CBO-WC500 with high catalytic efficiency for degradation of typical pharmaceuticals. The XAFS analysis proved that Cu-C chemical bond was constructed during the preparation process. The obtained CBO-WC500 was applied to remove sulfamethoxazole (SMX) through photocatalytic Fenton-like reaction, and removal efficiency reached 88.9 % after 60 minutes with the initial 5 mg•L −1 SMX and 0.2 g•L −1 catalyst in peroxymonosulfate (PMS) system. The results showed that the introduction of carbon stem from waste improved separation of photo-generated carriers and electron transfer capability, thus more photo-induced electrons could participate in reaction with PMS. Moreover, Cu(I) and Cu(II) in CBO-WC500 with Cu-Bi-spinel structure played a vital role in PMS activation. Led by electron transportation, reactive species ( 1 O 2 , •OH, SO 4 •- ) originated from PMS contributed to degradation of SMX, and degradation pathway of target pollutant was proposed based on analysis of intermediates. Removal efficiency of CBO-WC500 for SMX kept stable after several cycles’ utilization, and it also showed decent eliminating performance of mixed pollutants in different water matrix. This study has provided a potential way for resource reuse of adsorbed pollutant and realizing reutilization of spent adsorbent as photocatalyst with higher efficiency.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Minghao Xu,Mei Qin,Xuerui Yang,Lei Zhou,Hui Liu
In this study, CoCuFe-LDH with SO 4 2− as interlayer anion was prepared by a pot solvothermal method, which exhibited excellent peroxymonosulfate (PMS) activation performance for the degradation of sulfamethoxazole (SMX) over a wide pH range (3.0–12.0). Under the optimal condition, the SO 4 2− -CoCuFe-LDH/PMS system resulted in 99.1 % SMX (10 ppm) degradation in 4 min. Even for 50 ppm SMX, the degradation efficiency and COD removal rate approached 93.3 % and 70.0 % within 10 min, respectively. The current catalyst showed excellent stability after 5 times recycling experiments. The high-valent metal-oxo species were the major reactive oxygen species, and the SO 4 •− , • OH, O 2 •− , and 1 O 2 were involved in the degradation of pollutant. The SO 4 2− interlayer could expand the interlayer spacing of LDH, which facilitated the diffusion of PMS and pollutants within the interlayer and improved the utilization efficiency of the active sites. The current study provided novel insights into the designation of LDH structures in advanced oxidation processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jie Zhong,Yong Feng,Ao-Xia Sun,Hang Wei,Meng-Qiang Sun,Ling Huang,Guang-Guo Ying,Zhi-Liang Chen
Transition metal oxide defect engineering can regulate the electronic properties of materials, thereby realizing nonradical reactions during catalytic processes. In this study, porous carbon/manganese-iron oxide (PC@MFO) composites with different Mn/Fe ratios were prepared via in-situ encapsulation strategy. PC@MFO exhibited superior catalytic degradation and stable recycling performance during peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX). After 10 min of reaction, >92 % of SMX was rapidly degraded, with high selectivity, through oxidative SMX removal from a complex aqueous solution. The kinetics of SMX degradation over different as-prepared samples were also investigated. A recycling study and regeneration treatment revealed no clear deactivation between the 1st and 6th cycles, suggesting that PC@MFO is a reusable heterogeneous catalyst for utilization in efficient oxidative SMX removal. Multiple characterization techniques and density functional theory calculations were used to study the mechanism of SMX degradation process. Nonradical oxidation was found to be the dominant reaction in the catalytic reaction, leading to SMX degradation. This was possibly due to the highly conjugated electron delocalization induced by Mn-Fe in the O-octahedra close to the oxygen vacancies, promoting rapid charge transfer and interfacial reaction kinetics. This study expands the understanding for the activation mechanism driven by Mn-Fe spinel oxides in deep-water treatment.
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ENVIRONMENTAL POLLUTION
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2025
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IF 7.3
Yu Han,Xingzhou Yu,Yanan Liu,Min Zhang,Xianke Huang,Yinan Zhang,Hangjun Zhang
As the metabolic center of crustacean invertebrates, hepatopancreas plays a crucial role in metabolic detoxification and nutrient storage. Although sulfamethoxazole (SMX) and tire micro-particles (TMPs) are emerging marine pollutants, their combined hepatotoxic effects on lipid metabolism in crustaceans remain poorly understood. In this study, Litopenaeus vannamei were exposed to SMX and TMPs for 14 days. Hepatopancreatic lesions, lipid metabolism parameters, SMX bioaccumulation, and transcriptomic analysis were evaluated. Results revealed that SMX and TMPs co-exposure induced: (1) significant histological damage to hepatopancreas, accompanied by elevated levels of hepatopancreatic lesion markers; (2) a marked increase in lipid accumulation and altered fatty acid composition in hepatopancreas; (3) enhanced activities of lipid synthesis enzymes, increased triglyceride and total cholesterol levels, and reduced lipase activity; (4) dysregulation of metabolic pathways, characterized by upregulation of fatty acid synthesis-related pathways and downregulation of fatty acid decomposition-related pathways, alongside disruption of oxidative stress and detoxification pathways. Comparative analysis illustrated that SMX and TMPs co-exposure exhibited more toxicity than individual treatments. These findings demonstrated that SMX and TMPs synergistically impair hepatopancreatic function via lipid metabolism disruption and bioaccumulation, posing a potential threat to crustacean health and significant ecological risks in marine environments.
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ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Pin Peng,Xinyu Yan,Lixiang Chen,Xiang Li,Huiying Yang,Yijing Miao,Feng Zhao
Livestock wastewater is characterized by high concentrations of organic matter and diverse antibiotics. A major challenge in its anaerobic treatment is the effective degradation and thorough removal of coexisting antibiotic contaminants. In this study, an external voltage was applied to establish an electroactive biofilm, thereby enhancing the co-metabolic degradation of sulfamethoxazole and roxarsone. Application of +0.6 V (Ag/AgCl) increased the 72 h TOC removal efficiency to 52.1 %. At the same time, sulfamethoxazole and roxarsone removal efficiencies reached 90.8 % and 100 %, respectively. The results from liquid chromatography-mass spectrometry (HPLC-MS/MS) and density functional theory calculations revealed sulfamethoxazole degradation pathways: N–O bond cleavage and hydroxylation. Roxarsone degradation primarily involved nitro group reduction and C–As bond cleavage. The pharmacophore of sulfamethoxazole was effectively removed, and inorganic arsenic from roxarsone degradation was efficiently immobilized. Toxicity analysis confirmed that the electroactive biofilm notably reduced toxic intermediate accumulation. Elevated concentrations of NADH and ATP in the electroactive biofilm indicated enhanced microbial substrate metabolism and generation of more electron donors. The higher absolute abundance of the sulfamethoxazole degradation gene ( SadABC ) in the electroactive biofilm indicated that sulfamethoxazole degrading enzyme (sadABC) gained more electrons. Microbiome analysis revealed the upregulation of genes linked to extracellular electron transfer, the tricarboxylic acid (TCA) cycle, nitro-reduction, and sulfate reduction pathway, confirming the electroactive biofilm enhances substrate metabolism and co-metabolic antibiotic degradation. Electroactive biofilm offers a viable strategy for antibiotic removal in livestock wastewater.
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ELECTROCHIMICA ACTA
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2025
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IF 5.6
Hailun Zhao,Jian Ke,Shangkun Zhu,Manting Li,Jianqiu Chen,Qiulian Yang
The performance of Fe-catalyzed electrochemical advanced oxidation in antibiotic degradation was typically hampered by poor reduction efficiency of Fe 3+ to Fe 2+ and a narrow pH working range. This work employed natural hematite (HM) as iron source and oxalic acid (OA) as complexing agent in conjunction with electrolysis (EC) to address these concerns. Results showed that the EC/HM/OA system can achieve a 99.77 % degradation efficiency of sulfamethoxazole (SMX) under the optimized reaction conditions. The SMX degradation rate constant in EC/HM/OA system was 2.53-fold higher than in EC/HM system, following pseudo first-order kinetics. The OA addition promoted the Fe 3+ reduction by complexing with HM in electrochemical system, as well as extended the pH application range of EC/HM system to 3 − 11. The ATR−FTIR test and DFT calculation demonstrated that the adsorption of OA on the HM surface occurred in a deprotonated bidentate mononuclear configuration. Radical quenching experiments and EPR analysis confirmed that the crucial reactive oxygen species for SMX degradation in EC/HM/OA system were the ·OH and ·O 2 - radicals. Five potential degradation pathways of SMX were proposed. ECOSAR model and Daphnia magna toxicity tests demonstrated attenuated toxicity of SMX after degradation. The EC/HM/OA system exhibited robust resistance to common anions (Cl⁻ and NO₃⁻), and achieved high SMX degradation (86.82 %–99.67 %) across different water matrices. The combination of natural HM with OA significantly improved the degradation performance of electrochemical process for persistent antibiotics.
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