Journal of Water Process Engineering
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2026
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IF 6.6
Lixun Fan,Yonggang Zhao,Mingli Ye,Hongyun Niu,Yaqi Cai
NH₂-MIL(Fe) is grafted onto amino-functionalized NH₂-PS resin to gain micro-nanoscale adsorbent. • SMX adsorption is favorable at pH 5.2–8.0 with an adsorption capacity of 250.61 mg·g −1 . • Hydrogen bonding and electrostatic attraction are the driving forces for SMX adsorption. • The Fe(III) centers in MOF endow NH₂-PS@NH₂-MIL(Fe) Fenton-like catalytic activity. Sulfonamide antibiotics (SAs) are ubiquitous in the aquatic environment and difficult to remove using conventional wastewater treatment processes. Adsorption and Fenton-like oxidation are efficient techniques for the elimination of SAs from water. In this study, a novel hierarchical micro-nano structural adsorbent was synthesized by grafting Fe-based MOFs (NH 2 -MIL(Fe)) onto amino-functionalized polystyrene-divinylbenzene resin (NH 2 -PS). The physicochemical properties and structural features of the composite (NH 2 -PS@NH 2 -MIL(Fe)) were systematically characterized by SEM, EDS, XRD, FTIR, BET and XPS, confirming the successful immobilization of NH 2 -MIL(Fe) on the PS surface and the presence of abundant active sites. The adsorption behavior of sulfamethoxazole (SMX) on NH 2 -PS@NH 2 -MIL(Fe) was evaluated under various conditions, including pH, adsorbent dosage, and coexisting anions. The adsorption process followed the pseudo-second-order kinetic model and Langmuir isotherm model, indicating a monolayer sorption with a maximum capacity of 250.6 mg·g −1 at pH 5.2 and thermodynamic analyses revealed that the adsorption was spontaneous and exothermic. Based on FTIR, XRD and XPS analyses, electrostatic attraction, hydrogen bonding, π–π stacking, and metal–ligand coordination/Lewis acid-base interaction collectively governed the adsorption of SMX. Furthermore, the Fe(III) centers endowed NH 2 -PS@NH 2 -MIL(Fe) Fenton-like catalytic activity. With the addition of H 2 O 2 , over 95% of SMX was eliminated rapidly from water in a wide pH range. Based on the dual functions, this material can efficiently remove SMX from surface water samples. These results highlight the great potential of NH 2 -PS@NH 2 -MIL(Fe) for efficient removal of sulfonamide antibiotics. Download: Download high-res image (319KB) Download: Download full-size image
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Catalysts
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2026
·Vol. 16
·期 9
·769
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IF 4.5
Jingsi Liu,Fan Yang,He Guo
Sulfamethoxazole (SMX), a persistent sulfonamide antibiotic widespread in aquatic environments, resists conventional water treatment degradation. This work developed a NaOAc/Fe3+/O3homogeneous ozonation system for SMX abatement. Four comparative reaction groups confirmed significant synergism between trace Fe3+and sodium acetate. Under optimized near-neutral conditions, 96.19% SMX was removed within 30 min with kobs= 0.107 min−1, outperforming sole O3, O3/NaOAc and O3/Fe3+by 11.0%, 31.0% and 21.9% respectively. Single-factor tests revealed excess Fe3+or acetate suppressed catalytic activity, while alkaline conditions accelerated degradation yet aggravated iron precipitation. Radical quenching and p-CBA probing indicated that acetate coordination did not increase bulk ·OH exposure, while the stronger TEMP-derived TEMPO response after acetate addition was consistent with enhanced1O2-associated oxidation, suggesting that acetate altered the relative contributions of ozone-derived oxidation pathways. Post acetate background deduction, the ternary system achieved higher TOC/COD elimination. Twelve SMX intermediates were identified via LC-MS, with three ring-opening degradation pathways proposed. QSAR toxicity evaluation indicated that most intermediates possessed lower bioconcentration and developmental risks than raw SMX. Overall, the results indicate that weak acetate ligands can alter iron-mediated ozone oxidation pathways, providing a low-dose and economical strategy for antibiotic wastewater treatment.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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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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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
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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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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Yibo Zhang,Ming Li,Fang Chang,Malan Yi,Hongmei Ge,Jie Fu,Chenyuan Dang
Cyanobacteria and green algae are the OECD recommended test organisms for environmental toxicity assessments of chemicals. Whether the differences in these two species' responses to the identical chemical affect the assessment outcomes is a question worth investigating. Firstly, we investigated the distinct resistance mechanisms of Synechococcus sp. (cyanobacteria) and R. subcapitata (green algae) to sulfamethoxazole (SMX). The antioxidant system analysis demonstrated that R. subcapitata mainly relies on enhancing the activity of first line defense antioxidants, including superoxide dismutase (SOD), catalase (CAT) and glutathione peroxidase (GPx), which is the most powerful and efficient response to get rid of ROS, whereas Synechococcus sp. depends upon increasing the activity of glutathione-S-transferase (GST) and GPx to resist oxidative stress. Besides, a total 7 transformation products (TPs) of SMX were identified in R. subcapitata culture medium. The analysis of conjectural transformation pathways and the predicted toxicity indicates that R. subcapitata could relieve SMX toxicity by degrading it to low eco-toxic TPs. Additionally, we summarized numerous exposure data and assessed the environmental risk of various antibiotics, revealing an inconsistent result for the same type of antibiotic by using cyanobacteria and green algae, which is most likely due to the different resistance mechanisms. In the future, modified indicators or comprehensive assessment methods should be considered to improve the rationality of environmental toxicity assessments.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Huihui Zhang,Sisi Xiao,Yansheng Du,Shilin Song,Kun Hu,Yuyue Huang,Huijuan Wang,Qiangshun Wu
Herein, dielectric barrier discharge (DBD) plasma and MnO 2 -cellulose acetate (MnO 2 /CA) composite films was coupled together to degrade sulfamethoxazole (SMX) in water. The MnO 2 /CA composite films were firstly prepared successfully though heating blending method in this study and then characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), Raman spectra, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TG). Catalytic effect of the MnO 2 /CA films was investigated by comparing the removal percentages, the kinetic constants, the energy utilization efficiencies ( G 50 ) as well as the COD and TOC removal during the SMX degradation in the DBD plasma system with or without the MnO 2 /CA films addition under different reaction conditions. The optimal catalytic performance was obtained by adding the 3% MnO 2 /CA films into the DBD plasma system and the alkaline solution condition was favorable for the SMX degradation. After four times using, the MnO 2 /CA composite films still maintained the catalytic activity. Catalytic mechanism of the MnO 2 /CA films was speculated by analyzing the changes of solution pH and conductivity during the reaction, concentrations of the formed O 3 and H 2 O 2 in water and the generated active species ( 1 O 2 and ·OH) in both the DBD plasma system and the DBD-MnO 2 /CA films system. The quenching test was also carried out to figure out the important effect of the ·O 2 − , 1 O 2 and ·OH for the SMX degradation in the synergistic system. Finally, LC-MS was used to analyze the main intermediates generated during the SMX degradation and the possible degradation pathways were accordingly speculated. The research could provide a new direction for the development and application of the DBD plasma technology as well we the composite films catalyst.
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Journal of Environmental Sciences
·
2022
·
IF 6.796
Tian-Yang Zhang,Yong-Shan Lu,Zhen-Ning Luo,Wen-Jun Sun,Bin Xu,Chen-Yan Hu,Yu-Lin Tang,Zheng-Yu Dong,Xiao-Meng Ren
UV/peroxymonosulfate (UV/PMS) advanced oxidation process has attracted significant attention for removal of micropollutants in water. However, during practical water treatment applications, the PMS treatment must be performed before the UV treatment to achieve full contact. In this study, sulfamethoxazole (SMX) was selected as the target micropollutant. Four different operational approaches, including UV alone, PMS alone, simultaneous UV/PMS and sequential PMS-UV, were compared for their differences in SMX removal and disinfection by-product (DBP) formation potentials during chlorine-driven disinfection. Among the four approaches, UV/PMS and PMS-UV achieved over 90% removal efficiencies for SMX without substantial differences. For raw water, the trichloronitromethane (TCNM) formation potential after treatment with PMS-UV was lower than that after UV/PMS treatment. The time interval over which the PMS-UV process was conducted had little effect on the final removal efficiency for SMX. However, a brief (5 min) pre-PMS treatment significantly reduced the TCNM formation potential and the genotoxicity from DBPs. The formation risk for TCNM during chlorination increased markedly with increasing PMS dosages, and the appropriate dosage under these experimental conditions was suggested to be 0.5–1.0 mmol/L. Under alkaline conditions, PMS-UV treatment can enhance SMX degradation as well as dramatically reduced the formation potentials for haloketones, haloacetonitriles and halonitromethanes. This study suggests that proper optimization of UV/PMS processes can remove SMX and reduce its DBP formation.
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CHEMOSPHERE
·
2021
·
IF 7.086
Wei Li,Chun Ding,Gregory Korshin,Jiping Li,Hu Cheng
Chlorination is the most common disinfection technology used to treat wastewater effluent discharged into receiving aquatic environments. Effluent organic matter (EfOM) abundant in wastewater is a well-known photosensitizer and it greatly affects phototransformation of antibiotics in water. However, effects of chlorination on the characteristics and photochemical properties of EfOM have not been studied in sufficient detail. This paper investigated effects of chlorination on the characteristics of EfOM, and its impact on the phototransformation of sulfamethoxazole (SMX). Correlations between the EfOM characteristics and steady-state concentrations of reactive intermediates (RI) formed in the system were established. Chlorination was shown to preferentially remove the aromatic protein-like substances in EfOM, and the incorporation of chlorine into followed by the cleavage of the aromatic rings in EfOM molecules led to the formation of low molecular aliphatic organic matter. Both unaltered and chlorinated EfOM promoted the photodegradation of SMX whose rate constant in the wastewater was 1.32–1.65 times higher than that in pH 8 phosphate buffer. However, the rate of SMX photodegradation decreased at higher chlorination concentrations. The photodegradation of SMX was found to proceed through direct photolysis and oxidation by the RIs generated from EfOM and the self-sensitization of SMX. The steady-state concentrations of ·OH, 1 O 2 and 3 EfOM* were 2.15–5.50 × 10 −16 , 0.42–1.51 × 10 −13 , and 2.54–5.82 × 10 −14 M in unaltered and chlorinated wastewater. The steady-state concentrations of ·OH were well correlated with the removal of the fluorescence regional integration (ΔFRI) for humic-like and soluble microbial products (SMPs), while the photodegradation rate constant of SMX and the steady-state concentration of 1 O 2 and 3 EfOM* showed good correlations with ΔFRI for tryptophan and fulvic-like substances. Six transformation products (TPs) of SMX were identified. These findings provide new insights into the photochemical properties of chlorinated EfOM in the aquatic environments and its roles in the degradation of antibiotics and other trace-level pharmaceuticals.
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高影响因子
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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yingxin Zhao,Cailian Zhao,Ying Yang,Zhuoran Li,Xiaojie Qiu,Junzhi Gao,Min Ji
As a widely used antibiotic, sulfamethoxazole (SMX) has attracted increasing research attention. However, acidic condition was normally required for efficient SMX removal, and the energy variation of adsorption system is not fully elucidated. In this study, based on a typical mineral adsorbent of volcanic rock (VR), anion exchange was introduced by Polypyrrole (PPy) modification to overcome the electrostatic repulsion in alkaline environment, and site energy distribution (SED) theory was applied to explore adsorption behavior and mechanism on SMX from an energy perspective. The batch adsorption experiments and a series of complementary characterization were combined, confirming that pore filling and hydrogen bonding are the dominant adsorption mechanisms for SMX removal by VR. While the adsorption distinction between PPy supported VR (PPy-VR) and VR could be explained by electrostatic attraction, π-π electron donor-acceptor interaction (π-π EDA) and ion exchange, which further explained the wide pH application potential of modified sorbent. Moreover, Dubinin-Ashtakhov (DA) model was used to calculate the energy distribution, and PPy-VR exhibited a stronger adsorption affinity ( E m = 8.55–11.57KJ/mol) and energy heterogeneity ( δ e *=2.15–2.57) for SMX. The high-energy adsorption centers increased significantly (92.63%) after modification, which mainly attributed to π-π EDA and ion exchange introduced by PPy loading. The surface modification method provides a feasible idea for the improvement of application environment of adsorbents, and the analysis of SED is expected to promote the understanding of the connection between site energy and adsorption mechanism.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yufang Chen,Zhenhua Yan,Yan Zhang,Peiyuan Zhu,Runren Jiang,Min Wang,Yonghua Wang,Guanghua Lu
The concerns on the carriers of microplastics (MPs) on co-existing pollutants in aquatic environments are sharply rising in recent years. However, little is known about their interactions on the colonization of microbiota, especially for the spread of pathogens and antibiotic resistance genes (ARGs). Therefore, this study aimed to investigate the influences on the propagation of ARGs in sediments by the co-exposure of different MPs and sulfamethoxazole (SMX). The results showed that the presence of MPs significantly enhanced the contents of total organic carbon , while having no effects on the removal of SMX in sediments. Exposure to SMX and MPs obviously activated the microbial carbon utilization capacities based on the BIOLOG method. The propagation of ARGs in sediments was activated by SMX, which was further promoted by the presence of polylactic acid (PLA) MPs, but significantly lowered by the co-exposed polyethylene (PE) MPs. This apparent difference may be attributed to the distinct influence on the antibiotic efflux pumps of two MPs. Moreover, the propagation of ARGs may be also dominated by microbial carbon metabolism in sediments, especially through regulating the carbon sources of carboxylic acids , carbohydrates, and amino acids. This study provides new insights into the carrier effects of MPs in sediments.
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高影响因子
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