WATER RESEARCH
·
2023
·
IF 12.8
Huimin Liu,Dejin Liu,Yuancai Chen
Considering the negligent degradation of sulfamethoxazole (SMX) by Citrobacter freundii JH , the incorporation of bio-FeS could initiate the SMX biodegradation to 0.0444 (S-FeS), and further to 0.0564 mg L −1 mg −1 protein d −1 (SN-FeS) when coexisted with nitrate. Electrochemical (LSV, I-t , DPV, EIS and EDC) and respiratory inhibition experiments clarified that the bio-FeS could greatly switch/redistribute electron transmembrane-transfer from intracellular to extracellular mainly via FDH/Hases-S-chain, as revealed by the significant increase of ipa- FDH/Hases / ipa- FC-Cyts and ipc- FDH/Hases / ipc- FC-Cyts (from 1.09 and 1.07 (SN-native) to 1.50 and 3.58 (SN-FeS)), while nitrate (linear fitting with NADH ( R 2 = 0.9903)) mainly intensified CoQ-L-chain related INET from Complex I to CoQ to compensate for the electronic competition with SMX. SN-FeS system detoxified the SMX on microbial metabolism (such as membrane rupture and oxidative stress induction) with high SOD activity (737.93 U g FW −1 ). Structural equation modeling indicated that bio-FeS up-regulated PMF-mediated ATP synthesis ( P PMF-ATPs from 0.12 (SN-native) to 0.74 (SN-FeS)) and PMF-mediated NADH ( P PMF-NADH from -0.72 (SN-native) to 0.63 (SN-FeS)), and the nitrate addition intensified this positive feedback. Overall, this study provides a new perspective for bionanoparticles via electron transfer/redistribution to detoxify and launch the antibiotics biodegradation in ecological environment.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Chen Zhong,Hongbin Cao,Qingguo Huang,Yongbing Xie,He Zhao
In this work, we demonstrate for the first time the abatement of sulfamethoxazole (SMX) induced by stabilized ortho-semiquinone radicals (o-SQ•–) in the MnO2-mediated system in the presence of humic acid. To evaluate the performance of different MnO2/mediator systems, 16 mediators are examined for their effects on MnO2 reactions with SMX. The key role of the bidentate Mn(II)-o-SQ• complex and MnO2 surface in stabilizing SQ•– is revealed. To illustrate the formation of the Mn(II)-o-SQ• complex, electron spin resonance, cyclic voltammetry, and mass spectra were used. To demonstrate the presence of o-SQ• on the MnO2 surface, EDTA was used to quench Mn(II)-o-SQ•. The high stability of o-SQ•– on the MnO2 surface is attributed to the higher potential of o-SQ•– (0.9643 V) than the MnO2 surface (0.8598 V) at pH 7.0. The SMX removal rate constant by different stabilized o-SQ• at pH 7.0 ranges from 0.0098 to 0.2252 min–1. The favorable model is the rate constant ln (kobs, 7.0) = 6.002EHOMO(o-Qred) + 33.744(ELUMO(o-Q) – EHOMO(o-Qred)) – 32.800, whose parameters represent the generation and reactivity of o-SQ•, respectively. Moreover, aniline and cystine are competitive substrates for SMX in coupling o-SQ•–. Due to the abundance of humic constituents in aquatic environments, this finding sheds light on the low-oxidant-demand, low-carbon, and highly selective removal of sulfonamide antibiotics.
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FUEL
·
2023
·
IF 7.4
Zhonghua Xue,Yali Feng,Haoran Li,Chenglong Xu,Jinrong Ju,Lianping Dong,Chongyi Yang,Weiren Bao,Jiancheng Wang,Haoyu Wang,Ruiyu Ma
The search for efficient adsorbents to mitigate the impact of antibiotic pollutants on marine ecosystems, food security and human health is a burgeoning field of research. Further, Trimethoprim (TMP) and sulfamethoxazole (SMX) are widely distributed in the marine environment and are difficult to degrade. In this research, we used gravity separation to enrich the residual carbon from the coal gasification coarse slag and used the resulting carbon-high product (GC) as a low-cost and high-efficiency adsorbent. TMP and SMX were investigated for their adsorption behavior in seawater using GC under varied conditions. The findings indicated that the adsorption capacities of TMP and SMX by GC were 5.0017 mg/g and 5.1391 mg/g, respectively. The equilibrium durations of TMP and SMX by GC were 21 min and 40 min, respectively. Various adsorption models were fitted to the adsorption behavior of two pollutants by GC. The results showed that the adsorption processes of the two pollutants were consistent with the Freundlich equation and the quasi-secondary kinetic model, suggesting that both pollutants were adsorbed on GC surface by both physical and chemical processes. GC more effectively adsorbed TMP than SMX under a competitive adsorption procedure. When we introduced molecular dynamics simulation into this research, the microscopic procedures of GC adsorbing two pollutants were investigated. The energy composition and hydrogen bond types in the adsorption process were quantified. Finally, we summarized the adsorption mechanism of GC adsorbing two pollutants. This work will pave the way for developing effective, low-cost and environmentally friendly novel materials for the adsorption and purification of antibiotic pollutants in the marine environment. This research can produce positive economic and environmental effects in the comprehensive utilization of coal gasification slag.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Yuming Zhang,Wenjie Xiu,Miao Yan,Xinrui Guo,Zhihua Ni,Jihai Gu,Ting Tang,Fengsong Liu
Sulfamethoxazole (SMZ), a kind of sulfonamide antibiotic, is widely used in both human and veterinary medicine. Frequent detection of SMZ in natural aquatic environments has prompted growing attention and posed ecological risks to the ecosystem and human health. In this study, we investigated the ecotoxicological properties of SMZ upon Daphnia magna , and the mechanisms of the deleterious effects of SMZ were attempted to be elucidated by investigating a chain of parameters, including survival, reproduction, growth, locomotor behavior, metabolism, as well as levels of related enzyme activity and gene expression. After a 14-d sub-chronic exposure to SMZ at environmentally relevant concentrations, we observed virtually no lethal effect, weak growth inhibition, significant reproductive damage, evident ingestion rate decline, obvious change in locomotor behavior, and remarkable metabolic disorder. Notably, we identified SMZ as an inhibitor against acetylcholinesterase (AChE)/lipase in D. magna both in vivo and in vitro, which explained the adverse effects of SMZ on locomotor ability and lipid metabolism at the molecular levels. Furthermore, the direct interactions between SMZ and AChE/lipase were confirmed by using fluorescence spectrum and molecular docking. Together, our findings provide a new insight to advance the understanding of the environmental effects of SMZ on freshwater organisms.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Sheng-Nan Zhang,Yi-Tong Zhou,Jun Xia,Yu-Meng Wang,Jun-Wei Ma,Li-Kun Wang,Kashif Hayat,Shan-shan Bai,Cheng-han Li,Ming-Rong Qian,Hui Lin
Cadmium (Cd) and sulfamethoxazole (SMX) frequently coexist in farmlands, yet their synergistic toxicological impacts on terrestrial invertebrates remain unexplored. In this study, earthworms were exposed to artificial soils percolated with Cd (5 mg/kg), SMX (5 mg/kg) or combination of them for 7 days, followed by a 12-day elimination phase in uncontaminated soil. The uptake of Cd and SMX by the earthworms, along with their subcellular distribution, was meticulously analyzed. Additionally, a suite of biomarkers—including superoxide dismutase (SOD), catalase (CAT), malondialdehyde (MDA), and weight loss—were evaluated to assess the health status of the earthworms and the toxicological effects of the Cd and SMX mixture. Notably, the cotreatment with Cd and SMX resulted in a significantly higher weight loss in Eisenia fetida (41.25 %) compared to exposure to Cd alone (26.84 %). Moreover, the cotreatment group exhibited substantially higher concentrations of Cd in the total internal body, fraction C (cytosol), and fraction E (tissue fragments and cell membranes) in Eisenia fetida compared to Cd alone counterparts. The combined exposure also significantly elevated the SMX levels in the total body and fraction C compared with the SMX-only treated earthworms. Additionally, Eisenia fetida subjected to the combined treatment showed markedly increased activities of SOD, CAT, and MDA compared to those treated with Cd alone. The effect addition indices (EAIs), ranging from 1.00 to 2.23, unequivocally demonstrated a synergistic effect of the combined treatments. Interestingly, relocating the earthworms to clean soil did not mitigate the observed adverse effects . These findings underscore the increased risk posed by the Cd-SMX complex to terrestrial invertebrates in agricultural areas.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiaoqian Hao,Shengjun Xu,Yan Huang,Shuanglong Ma,Boqiang Gao,Jia Song,Jingzhen Wang,Sihui Zhan
Molybdenum disulfide serves as an ideal support for single atom catalysts (SACs), offering not only coordination elements but also abundant active sites, such as surface defects and vacancies. Herein, a novel Co-SAC (MoSO-Co-C) containing a four-coordinated configuration (Mo-Co-C 3 ) is designed and synthesized, in which the carbon intercalation is utilized to regulate sulfur vacancies for anchoring the Co atom. The introduction of Co atoms and C intercalation significantly enhances the E ads between catalyst and peroxymonosulfate (PMS), favoring the formation of metastable intermediates. The k obs of sulfamethoxazole (SMX) removal for MoSO-Co-C is 9.2 times and 1.8 times higher than those of catalysts without Co or C intercalation. SMX is removed mainly by electron transfer pathway, wherein SMX and PMS act on the same Co site of MoSO-Co-C, and electrons are transferred from SMX to MoSO-Co-C and eventually to PMS. The MoSO-Co-C demonstrated excellent SMX degradation in the diverse water matrices, and the removal efficiency of SMX maintained above 95 % after 72 h of continuous degradation. This study provides new insights into the design of transition metal-based SAC and in-depth understanding of PMS activation mechanism.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Peiwen Li,Qiansheng Li,Hong Lu,Ze Fu,Jiti Zhou,Chenghao Sun,Xuehai Wang
Some nano-biochars (nano-BCs) as electron mediators could enter into cells to directly promote intracellular electron transfer and cell activities. However, little information was available on the effect of nano-BCs on SMX degradation. In this study, nano-BCs were prepared using sludge-derived humic acid (SHA) and their effects on SMX degradation by Shewanella oneidensis MR-1 were investigated. Results showed that nano-BCs (Carbon dots, CDs, <10 nm) synthesized using SHA performed a better accelerating effect than that of the nano-BCs with a larger size (10–100 nm), which could be attributed to the better electron transfer abilities of CDs. The degradation rate of 10 mg/L SMX in the presence of 100 mg/L CDs was significantly increased by 84.6% compared to that without CDs. Further analysis showed that CDs could not only be combined with extracellular Fe(III) to accelerate its reduction, but also participate in the reduction of 4-aminobenzenesulphonic acid as an intermediate metabolite of SMX via coupling with extracellular Fe(III) reduction. Meanwhile, CDs could enter cells to directly participate in intracellular electron transfer, resulting in 32.2% and 25.2% increases of electron transfer system activity and ATP level, respectively. Moreover, the activities of SMX-degrading enzymes located in periplasm and cytoplasm were increased by around 2.2-fold in the presence of CDs. These results provide an insight into the accelerating effect of nano-BCs with the size of <10 nm on SMX degradation and an approach for SHA utilization.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Jiahui Huang,Bufan Yang,Xin Ma,Xin Zhang,Sinong Huang,Erdeng Du,Xiaoyan Ma,Jing Deng
Antibiotics removal from wastewater by conventional methods is limited, and their lingering presence in the environment can be hazardous to both human health and the ecosystem. Sulfamethoxazole (SMX) is one of the primary study subjects for antibiotic contamination, the degradation behavior, mechanism, transformation pathway, disinfection byproducts (DBPs) formation and variations about toxicity in UV/nitrite (NO 2 − ) system were examined in this study. Compared with UV irradiation, the first-order reaction rate of SMX in UV/NO 2 − system rose from 0.0397 to 0.0528 min −1 . This enhancement was linked to the generation of reactive oxygen species (ROS) and reactive nitrogen species (RNS), which promoted the degradation. SMX removal was more favorable under high dissolved oxygen (DO) levels and acidic conditions. When NO 2 − concentrations ranged from 0.1 to 1.0 mM, the higher concentration was more favorable to the degradation. The addition of 10 mM of HA and HCO 3 − hindered the oxidation of SMX by 48.46 % and 26.85 %, respectively, while the addition of Cl − slightly accelerated the decay of SMX at certain concentrations (5, 10 mM). The results of HPLC-ESI-MS and DFT computation suggested three possible SMX degradation pathways, including nitrification, hydroxylation, and bond breaking (such as sulfonamide cleavage). The primary DBPs produced by the post-chlorination of SMX in UV/NO 2 − system were TCM (87.02 % of the total detected DBPs) with a minor quantity of DBPs containing nitrogen. The presence of bromide ions (Br − ) can lead to the production of highly toxic bromine containing disinfection by-products (Br-DBPs). After adding Br − in UV/NO 2 − system, 100 % of N-DBPs (TCNM, DCAN) and 93.43 % of C-DBPs (TCM, DCAA, TCAA) were converted to Br-DBPs (TBM, DBAA, TBAA, BDCM, DBCM), with the production of Br-DBPs accounting for 82.63 % of the detected DBPs.
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Separations
·
2024
·Vol. 11
·期 12
·356
·
IF 2.5
Zhaowei Wu,Meiyi Hu,Pengfan Zhuo,Jie Wang,Shaoping Tong
A composite Fe-MOF-C/N was prepared with Fe-MOF and g-C3N4precursors, and its activation property of peroxymonosulfate (PMS) in the degradation of Sulfamethoxazole (SMX) was studied. XRD, SEM, and TEM analyses showed that Fe-MOF-C/N was porous and mainly composed of phases of Fe3N, C0.08Fe1.92, and graphite. XPS indicated that Fe-MOF-C/N mainly had Fe, C, N, and O elements, among which Fe existed in the form of Fe2+and Fe3+. Fe-MOF-C/N was used to activate PMS to degrade SMX, and the result showed that Fe-MOF-C/N had excellent catalytic performance and 84.17% of SMX could be removed in 8 min. Free radical quenching experiments showed that1O2was the main active species in Fe-MOF-C/N/PMS. The stability experiment showed that Fe-MOF-C/N had good stability, and the degradation rate of SMX only decreased by 5.8% after five times of use.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Qingmuke Su,Yaguang Du,Dongyun Du,Tian C. Zhang
In recent years, the effective treatment of antibiotics and the rational resource utilization of high‑carbon industrial wastewater have become hot research in the industry. However, there is no research on combining the two together for efficient resource recycling. In this study, sulfamethoxazole (SMX) was added to distillery wastewater with high COD for anaerobic digestion (AD), and its effects on substrate metabolism and methane production in AD systems were investigated. The results show that SMX can be completely metabolized in the AD system of the winery. The methane yield is the highest (810.73 mL CH 4 /g·VS) when the concentration is 0.5 mg/L, which is increased by 55.09 %. Polysaccharides and proteins were more susceptible to SMX, accumulated in the extracellular area and then were used as carbon sources in the subsequent microbial activities. The microbial community and macrogenomic analyses showed that SMX regulated the microbial community and enriched the acetate-type methanogens, leading to more methane production. Meanwhile, the analysis of KEGG metabolic pathway showed that the abundance of functional genes of key enzymes synthesizing antioxidant amino acids was enhanced, which resisted the hydroxyl radicals generated by SMX, leading to the additional production of acetic acid under this metabolic pathway. In addition, functional genes related to glycolysis, amino acid metabolism, tricarboxylic acid (TCA) cycle, and methane metabolism were increased in abundance by 20–90 %, resulting in maximized methane production.
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ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Fang Yang,Lihe Zhu,Zushen Xu,Yongwei Han,Xue Lin,Junyou Shi,Zhong Sun,Xixin Duan
Sulfamethoxazole (SMX) is one of major antibiotic contaminants in current aqueous environment. In this paper, waste loofah and melamine were co-carbonized to prepare biochar-doped g-C 3 N 4 (CCN) by a one-pot method and then combined with Co 2 PMo 11 VO 40 (CoPMoV) using a binder to obtain the novel polyoxometalates (POMs) photocatalytic composites (CCN/CoPMoV). The incorporation of CoPMoV dramatically reduced the photogenerated carrier recombination and led to a small band gap. Under visible light, the synergetic activation from biochar, g-C 3 N 4 and POMs can remove 98.5% of SMX ( k = 0.215 min −1 ) in the peroxymonosulfate (PMS) system within 20 min and keep its high stability with the degradation of 88.9% after five cycles. Multi-active sites from CCN/CoPMoV are contributed to develop the most active species of SO 4 − ∙ , ·OH, 1 O 2 , and h + . The validity in the degradation of SMX makes CCN/CoPMoV a promising and potential material for the removal of aqueous pollutants in the future.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Irfan Ijaz,Aysha Bukhari,Ezaz Gilani,Ammara Nazir,Hina Zain,Attia Shaheen,Mohammed Rafi Shaik,Mujeeb Khan,Mohamed E. Assal
A rising quantity of drugs has been discharged into the aquatic environment, posing a substantial hazard to public health. In the current work, a novel hydrogel (i.Carr@Bent@PTC), comprised of iota-carrageenan, bentonite, and 4-phenyl-3-thiosemicarbazide, was successfully prepared. The introduction of 4-phenyl-3-thiosemicarbazide and bentonite in iota-carrageenan significantly increased the mechanical strength of iota-carrageenan hydrogel and improved its degree of swelling, which can be attributed to the hydrophilic properties of PTC and Bent. The recorded contact angle was 70.8°, 59.1°, 53.9°, and 34.6° for pristine i.Carr, i.Carr@Bent, and i.Carr@Bent@PTC, respectively. The low contact angle measurement of the Bent and PTC loaded-i.Carr hydrogel was attributed to the hydrophilic Bent and PTC. The ternary i.Carr@Bent@PTC hydrogel demonstrated broad pH adaptability and excellent adsorption capacities for sulfamethoxazole (SMX) and losartan potassium (LP), i.e., 467.61 mg. g −1 and 274.43 mg. g −1 at 298.15 K, respectively. The pseudo-first-order (PSO) model provided a better fit for the adsorption kinetics . The adsorption of SMX and LP can be better explained by employing the Sips and Langmuir isotherm models. As revealed by XPS and FTIR investigations, π-π stacking, complexation, electrostatic interaction , and hydrogen bonding were primarily involved in the adsorption mechanisms.
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