JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2024
·Vol. 99
·期 12
·2665-2676
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IF 2.8
Yongming Wang,Qiang Chen,Yuezong Su,Yuxuan He,Jin Qian,Kailin Xu
BACKGROUND The increasing presence of antibiotics in aquatic environments poses significant ecological risks, with sulfamethoxazole (SMX) being a prominent example due to its persistence and widespread use in medical and veterinary practices. Advanced oxidation processes, particularly those based on peroxymonosulfate (PMS), have shown promise in degrading such contaminants. This work explored the efficacy of a bimetallic selenide catalyst, FeSe 2 /MoSe 2 (FM), synthesized via a hydrothermal method, for the rapid activation of PMS and subsequent degradation of SMX. RESULTS Over 95% SMX degradation was achieved with a 0.25 g/L catalyst dosage and 1.5 g/L PMS dosage, demonstrating that FM was an effective PMS activator capable of efficiently oxidizing SMX. The EPR tests and quenching experiments confirmed the presence of 1 O 2 , SO 4 •– and • OH in the degradation system, with SO 4 •- predominating. The redox cycling of Mo with Fe was involved in the activation of PMS. Moreover, the DFT calculations of the SMX molecule revealed that the vulnerable sites were mainly in the vicinity of the sulfonamide group and the oxygen-containing group. The toxicity assessment disclosed that most of the primary degradation intermediates of SMX were toxic, while the further small molecule products were non-toxic. CONCLUSION This work underscores the potential of the FM/PMS system as an efficient and sustainable solution for degrading antibiotic contaminants like SMX in water. The low toxicity of the final degradation products further supports the environmental safety of this approach, making it a promising candidate for real-world water treatment applications. © 2024 Society of Chemical Industry (SCI).
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Kangfeng Pang,Wei Sun,Feng Ye,Lihui Yang,Mengjie Pu,Cao Yang,Qichun Zhang,Junfeng Niu
N,S-co-doped carbons were synthesized through the calcination of sulfur-modified chitosan for the first time, and utilized as persulfate activators for sulfamethoxazole (SMX) remediation in water. The chitosan and sulfonyl chloride underwent one-step sulfonylation reaction to generate S-modified chitosan. The catalyst NSC-3 showed both excellent adsorption and catalytic oxidation efficiency, corresponding 98.62% removal and 81.34% mineralization rate within 90 min. The rate constant ( k obs ) was up to 0.0578 min −1 , with 75.60-folders higher than that of sulfur-free catalyst NC (7.6580 ×10 −4 min −1 ). The synergy of N and S contributed to the improvement of removal efficiency. The adsorption and oxidation performance were highly depended on the S/N atomic ratio. At the S/N ratio of 0.18, the maximum adsorption and oxidation capability were obtained. The NSC-3/PS system exhibited outstanding adaptability at the wide pH range from 3.07 to 9.28, while the inhibitory effect occurred at strong basic conditions (pH = 11.01). The thiophene sulfur and structural defects were identified as the catalytic sites in activating PS. Both radical and non-radical pathways were responsible for degradation process, where 1 O 2 played a major role, SO 4 ·- exerted a minor contribution, and O 2 ·- acts as the precursor for the production of 1 O 2 . Another source of 1 O 2 was assigned to the activation of PS by structure defects . This work indicates that N,S-co-doped carbon at an optimal S/N atomic ratio effectively catalyzes persulfate, and provides an innovative method to construct bifunctional carbon materials of adsorption and oxidization.
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JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2020
·Vol. 146
·期 12
·04020134
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IF 1.264
Mahdi Hassan,Guangcan Zhu,Zhonglian Yang,Yongze Lu
A three-dimensional bioelectrochemical reactor (3D-BER) system combining heterotrophic and autotrophic denitrification processes was developed, which possesses the effects of pH on nitrate or nitrite removal and simultaneously elimination of antibiotic sulfamethoxazole (SMX) from simulated municipal wastewater. The experimental results demonstrated that the variation of microbial communities was examined with electric current from 0 to 90 mA at pH 6.50±0.12 to 7.9±0.04. When the current increased from 0 to 90 mA, the nitrate removal efficiency increased from 59.05% to 99.21%, and SMX removal efficiency of 43.9%–93.9% was achieved. The optimum pH of this reactor was 7.0±0.20 to 7.50±0.31, and a lower or higher pH condition may effect autotrophic and heterotrophic denitrification processes. Simultaneously, the denitrification mechanism in this system was analyzed through pH variation in the effluent. The CO2 produced from the anode acted as a good pH buffer, automatically controlling pH in the reaction zone. A low current intensity does not effect the degradation by-products but increases the SMX removal efficacy. Bacterial community analysis revealed substantial changes in microbial communities at the phylum, class, and genus levels after SMX acclimatization. Thauera, a well-known aromatic-degrading bacteria, was the most dominant genus present in acclimatized conditions at 60 mA. In summary, this study shows that high currents changed the microbial structure, and the acclimatized sludge can play a vital role in the biodegradation of SMX, and removal of NO3−─ N from simulated municipal wastewater by a novel 3D-BER.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jianglong Shi,Chen Sun,Zongli Huo,Jia Gu,Jun Ma
This study demonstrated the synergy between peroxymonosulfate (PMS) and p- benzoquinone ( p -BQ) in the sulfamethoxazole (SMX) degradation under the ultraviolet (UV) irradiation. In the UV/ p -BQ/PMS process, the SMX degradation showed positive dependence on the initial dosages of PMS, p -BQ and SMX. The variation of the observed pseudo-first-order rate constant ( k obs ) exhibited aligned with the speciation of SO 5 2− across pH 7–10, and the anomalous decline of k obs emerged at pH 10–12. It suggested that SO 5 2− might be significant for the SMX degradation. The quenching experiments and the electron paramagnetic resonance spectroscopy confirmed the dominant reactive oxygen species (ROS) (i.e., sulfate radicals (SO 4 •– ), hydroxyl radicals (OH • ), singlet oxygen ( 1 O 2 ), peroxymonosulfate anion radical (SO 5 •– )) in the UV/ p -BQ/PMS process. The generation of SO 5 •– might be attributed to the single electron transfer (SET) mechanism from PMS to the triplet excited-state of p -BQ, which subsequently triggered the formation of SO 4 •– and 1 O 2 via disproportionation. The possible degradation pathways of SMX were identified by LC-MS, including the hydroxylation, the cleavage of S N bond, the nitration and the oxidation of amino group. Compared to p -BQ, methyl- p -benzoquinone, with an electron donating group, was found to suppress the activation of PMS, which validated the rationality of the SET mechanism. While tetrachloro-1,4-benzoquinone, with an electron withdrawing group, inhibited the SMX degradation by scavenging the generated radicals. Furthermore, the coexisting ions made no diffidence to the SMX degradation. The results provided the critical insights into the role of quinones in the PMS-based advanced oxidation processes for water treatment.
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BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Jiacheng Qin,Rongting Ji,Qian Sun,Wei Li,Hu Cheng,Jiangang Han,Xin Jiang,Yang Song,Jianming Xue
Excellent biochar properties are crucial for sorption performance, and a developed pore structure is especially important. Herein, novel porous carbon/porous biochar (PC/PB) composites, in which the porous biochar and porous carbon were prepared at the same time, were synthesized via a green method from algal biomass with the help of the self-activation of citrate for the first time, and the composites were evaluated for the sorption of sulfamethoxazole (SMX). Many micro/meso/macropores were introduced into the PC/PB composites, which showed high specific surface areas (up to 1415 m 2 /g) and pore volumes (up to 1.08 cm 3 g −1 ). The PC/PB composites displayed excellent SMX sorption capacities, which reached 844 mg g −1 . Pore filling played a crucial role in determining the sorption capacity, and hydrogen bonding, electrostatic interactions and π-π stacking controlled the sorption rate. This study provides an improved method for preparation of porous biochar.
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CHEMOSPHERE
·
2022
·
IF 8.943
Chenxin Su,Muhan Jia,Xiaofei Xue,Chenliu Tang,Lingyun Li,Xiang Hu
A core-shell covalent organic framework encapsulated Co 1.2 Fe 1. 8 O 4 magnetic particles (CFO@COF) was designed and prepared successfully to activate peroxymonosulfate (PMS) for sulfamethoxazole (SMX) degradation. It displays amazing catalytic reactivity since the unique interior structure and synergistic effect between COF shell and CFO core, reaching 99.8% removal of SMX (10 mg/L) within 30 min and 90.8% TOC removal. The synergy between bimetals vests high reactivity to CFO core. And the outer COF shell can stabilize the CFO core under intricate reaction conditions to restrain the leaching of Co ions (decreased from 0.75 to 0.25 mg/L). Further investigation compared the activation mechanism in two different system, CFO/PMS system and CFO@COF/PMS system. The result showed that the radical mechanism controlled by SO 4 ⋅- guided the SMX degradation in CFO/PMS system whereas the 1 O 2 played a pivotal role in CFO@COF/PMS system called non-radical leading. The influences of various factors on degradation experiments and SMX degradation pathway were also studied. Most importantly, risk assessment in CFO@COF/PMS/SMX system was estimated via “ecological structure activity relationships”. In most case, the toxicities of intermediates were lower than the initial samples, which confirmed the effectiveness of CFO@COF/PMS/SMX system in the reduction of toxicity of SMX.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 29
·期 47
·71766-71773
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IF 5.19
Huo Junyu,Li Chaoyu,Hu Xiaojin,Xie Huijun,Hu Zhen,Wu Haiming,Liang Shuang,Zhang Jian
Iron ore and manganese ore were used as substrate of constructed wetlands (CWs) to enhance nitrogen (N) removal. However, the N purification performance in CWs filled with iron or manganese ore under antibiotics stress needs further study. In this study, three groups of CWs filled with river sand, limonite (a kind of iron ore), and manganese ore sand were constructed, which were named as C-CWs, Fe-CWs, and Mn-CWs, respectively. The effect and mechanism of the composite antibiotics sulfamethoxazole (SMX) and trimethoprim (TMP) on N removal in CWs were investigated. While the addition of SMX and TMP inhibited about 40% nitrification and promoted about 25% denitrification in all CWs, Fe-CWs and Mn-CWs always had better N removal performance than C-CWs. Changes in microbial community structure in CWs indicated that the better N removal performance in Fe-CWs and Mn-CWs was attributed to the presence of more abundant and diverse N-associated bacteria, especially Fe- and Mn-driven autotrophic denitrifying bacteria. What’s more, the addition of iron ore or manganese ore contributed to the better N removal performance with highest relative abundance of N-transferring bacteria under antibiotics stress.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hui He,Yuexin Wang,Juan Li,Shanliang Jiang,Subhan Sidra,Wenxue Gong,Ying Tang,Yang Hu,Rule Wei,Dongxiao Yang,Xuesheng Li,Zhongxing Zhao
High light adsorption and fast charge separation are crucial for photo-Fenton catalytic activity of MOFs. Herein, bottom-up design was proposed to fabricate polypyrrole (PPy C ) nanowires in MIL-88B(Fe) cages as photo-Fenton catalyst for Sulfamethoxazole (SMX) efficient degradation. Pyrrole was prior anchored into MIL-88B(Fe) cluster via Fe-N coordination, and then the additional monomer pyrrole was further triggered bottom-up polymerization in confined cages of MIL-88B(Fe) and formed PPy C @Py-MIL(Fe) composite. These PPy C nanowires were dispersed in Py-MIL(Fe) cages and tightly connected with MOFs clusters via Fe-N bonding. Characterization proved that: (1) Interfacial Fe-N can significantly promote the efficient electron transport from PPy C nanowires to Py-MIL(Fe), enhance optical absorption property, and construct strong Lewis acidic sites and ligand vacancies in PPy C @Py-MIL(Fe). (2) The confined PPy C nanowire via Fe-N connection remarkably promote photo-generated electron-hole separation, Fe 2+ |Fe 3+ redox ability of MOF, and improved photo-electric corrosion ability. As a result, it significantly enhanced the photo-Fenton catalytic performance for SMX degradation. Catalytic oxidation was attributed to the generation of ‧OH species that oxidized 93% SMX in 60 min, showing ultra-rapid degradation and TOC removal rates of 33.7 min −1 ·mg·g −1 and 8.68 min −1 ·mg·g −1 respectively, which was about 4–220 times higher than those reported state-of-the-art catalysts. Additionally, the PPy C @Py-MIL(Fe) catalyst showed minimal loss in catalytic activity even after recycling for 10 times, exhibiting good recycling stability compared to many MOFs. Systematic analysis shown that in-situ anchored growth of polypyrrole in confined porous cages of MOF can effectively enhance the catalytic activity and stability of MIL-88B(Fe), and has great development potential applications for photo-Fenton catalytic degradation of organic pollutants.
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WATER RESEARCH
·
2020
·
IF 9.13
Tianyu Li,Lifa Ge,Xingxing Peng,Wei Wang,Weixian Zhang
Advanced oxidation processes (AOP) based on nonradicals have attracted growing attentions because nonradical systems require much less oxidants and have low susceptibility to radical scavengers. Herein, a novel Fenton-like system that utilizes nonradicals was explored. It was derived from g-C 3 N 4 /MgO activated H 2 O 2 , and can reduce the H 2 O 2 stoichiometry from 0.94%−0.18% to 0.03%. Sulfamethoxazole (SMX), a widely used sulfonamide, was used as the model pollutant to evaluate the efficacy of the system. It was observed for the first time that organic pollutants can be degraded with singlet oxygen ( 1 O 2 ) through a nonradical pathway in the g-C 3 N 4 /MgO H 2 O 2 system. The reduced H 2 O 2 consumption was the net result of continuously-recycled H 2 O 2 from the reactions between H 2 O 2 and g-C 3 N 4 /MgO. Based on experimental results and theoretical calculations, the synthesis of g-C 3 N 4 and MgO forms a N-Mg bond with strong ability to absorb electrons and the electron transfer of H 2 O 2 to N-Mg bonding is accelerated, activation of H 2 O 2 to generate 1 O 2 . Experimental data showed that organic pollutants can be degraded rapidly over a wide pH range. Findings of this study point to a cyclical but stable Fenton-like system with reduced H 2 O 2 requirement for cost-effective remediation and treatment of organic pollutants and toxic wastes.
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MICROCHEMICAL JOURNAL
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2020
·
IF 3.594
Xizhuang Yue,Zaiyu Li,Shuang Zhao
A novel electrochemical sensor based on graphene (GR) and ZnO nanorods (GR-ZnO/GCE) was developed to detect sulfamethoxazole (SMX) and trimethoprim (TMP) simultaneously. SEM image showed that ZnO had a rod shaped morphology. XRD result indicated a hexagonal wurtzite phase of ZnO nanorods. The electrochemical experiment results showed that the synergetic effect of GR and ZnO endowed the prepared sensor excellent electrocatalytic behavior towards the oxidation of SMX and TMP. SMX and TMP were detected by DPV method at 0.85 V and 1.06 V, respectively. Under the optimal conditions, the GR-ZnO/GCE showed superior wide linear responses in concentration range of 1–220 μmol/L for SMX and 1–180 μmol/L for TMP with the limit of detection (LOD) of 0.4 μmol/L and 0.3 μmol/L, respectively. In addition, the sensor has good stability, good selectivity, anti-jamming ability and reproducibility. We tested SMX and TMP in lake water, tap water, urine and serum with recovery between 93.2% and 108%. The proposed sensor has a good application prospect in biomedicine and environmental protection.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Shiwen Zhang,Lele Cui,Yanhui Zhao,Huijun Xie,Maoyong Song,Haiming Wu,Zhen Hu,Shuang Liang,Jian Zhang
Constructed wetlands (CWs) are reservoirs of microplastics (MPs) in the environment. However, knowledge about the impact of MPs on antibiotic removal and the fate of antibiotic resistance genes (ARGs) is limited. We focused on sulfamethoxazole (SMX) as a representative compound to examine the effects of MPs on SMX removal and the proliferation and dissemination of two SMX-related ARGs ( sul1 and sul2 ) in vertical subsurface-flow CW (VFCW) microcosm. The presence of MPs in the substrate was found to enhance the proliferation of microorganisms owing to the large specific surface area of the MPs and the release of dissolved organic carbon (DOC) on MP surfaces, which resulted in a high SMX removal ranging from 97.80 % to 99.80 %. However, the presence of MPs promoted microbial interactions and the horizontal gene transfer (HGT) of ARGs, which led to a significant increase in the abundances of sul1 and sul2 of 68.47 % and 17.20 %, respectively. It is thus imperative to implement rigorous monitoring strategies for MPs to mitigate their potential ecological hazards.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yizhen Cheng,Jingrui Yang,Jimin Shen,Pengwei Yan,Shan Liu,Jing Kang,Lanbo Bi,Binyuan Wang,Shengxin Zhao,Zhonglin Chen
Heteroatom doping technology is of great significance for adsorption. However, the effect of P with relatively lower electronegativity (2.19) doped in the π-electron system and phosphorus-containing functional groups on the adsorption has always been neglected. Herein, P-doped biochar (PBC) was successfully synthesized via the in-situ activation method and applied in a bath experiment and a long-term fixed-bed dynamic adsorption for sulfamethoxazole (SMX) removal. Compared to pristine BC, the pH pzc , ash content and graphitization degree of PBC would be reduced significantly after phosphoric acid (H 3 PO 4 ) was treated, but it gained a large specific surface area (SSA = 233 m 2 g −1 ), as well as abundant surface functional groups. In the adsorption process, the behavior of SMX adsorbed onto PBC conformed to pseudo-second-order kinetic and Langmuir models in batch experiments. Its excellent adsorption capacity (148.62 mg g −1 ) benefited from a large number of functional groups. DFT calculation indicates that the C 3 -P-O configuration mainly promoted the adsorption of SMX. It is speculated that the hydrogen-bond interaction between SMX and C 3 -P-O was the main adsorption mechanism, and electrostatic and π-π EDA interaction also contributed. Various parameters during the dynamic process were thoroughly explored. The saturated adsorption capacity of the column would be promoted when influent SMX concentration and bed depth increased, but negatively correlated with solution pH and influent rate. Moreover, PBC fixed-bed column for SMX removal was well fitting Thomas, Yoon-Nelson and BDST models, which provided a predictable strategy for practical application.
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