APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Jianhua Yang,Zhengkui Li,Hongjie Zhu
A novel hydrogel catalyst (p(HEA/NMMA)-CuS) with the function of adsorption and degradation of organic pollutants in water was successfully synthesized using irradiation polymerization and in situ precipitation methods The composite hydrogel catalyst was characterized by SEM-EDS, TEM, swelling kinetics, zeta potential, TGA, XPS, FTIR and XRD. Besides, the effects and mechanisms of adsorption and degradation of sulfamethoxazole(SMX) as the representative pollutant by p(HEA/NMMA)-CuS hydrogel were observed. The results presented that adsorption process of SMX on complex hydrogel fit well to Langmuir monolayer adsorption, and followed a pseudo-second-order rate equation. The decomposition of SMX by p(HEA/NMMA)-CuS hydrogel in aqueous solution under 500 w visible light achieved balance in 24 h, the removal ratio reached 95.91%, and the SMX was mineralized with 43.56%. Hydroxyl radicals was detected as the reactive species using EPR in the system, degradation intermediates of SMX were further analyzed by LC-TOF-MSMS, a possible pathway for SMX degradation was presented. The degradation mechanism of SMX was also illustrated by theoretical calculations of frontier electron densities. Furthermore, mineralization, stability and regeneration results indicated that the developed hydrogel catalyst, p(HEA/NMMA)-CuS hydrogel, was promising in practical application.
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Nanomaterials
·
2025
·Vol. 15
·期 6
·432
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IF 4.3
Xin Zhong,Xiaojun Liu,Meihuan Ji,Fubin Jiang
As the most promising techniques for refractory antibiotic degradation in wastewater management, sulfate radical-based advanced oxidation processes (SR-AOPs) have attracted considerable attention. However, systematic studies on potassium peroxymonosulfate (PMS) activation by MOF-derived metal oxides coated with LDH materials are still lacking. In this work, a series of catalysts consisting of CoCu-MOFs coated with CuAl/LDH were synthesized for PMS activation in the removal of sulfamethoxazole (SMX). As expected, CoCu-MOFs coated with CuAl/LDH catalyst showed high SMX removal and stability in PMS activation. In the CoCu/LDH/PMS reaction, the SMX removal was nearly 100% after 60 min, and the mineralization reached 53.7%. The catalyst showed excellent catalytic stability and low metal leaching concentrations (Co: 0.013 mg/L, Cu: 0.313 mg/L), as detected by ICP. Sulfate radicals and hydroxyl radicals were identified as the dominant reactive species in the CoCu/LDH/PMS system. Moreover, the presence of 1 O 2 in the process revealed the coupling of non-radical and radical processes. The XPS results showed that the layered structure of CoCu/LDH promoted the recycling of metal ions (high and low valence), which facilitated heterogeneous PMS activation. The effects of different reaction conditions and reuse cycles were also determined. The SMX oxidation pathways were proposed based on the intermediates identified by LC/MS. The high activity and stability of CoCu/LDH provide a new mechanistic understanding of PMS activation catalysts and their potential utilization in practical wastewater treatment.
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TALANTA
·
2024
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IF 5.6
Xian Yang,Yujie Xiao,Yue Zhao,Hongping Han,Hong Zheng,Xue Zhang
In this study, Cu doped carbon dots (Cu-CDs) of uniform particle size and good water solubility was synthesized using Angelica Sinensis Radix as precursor materials through a one-step hydrothermal. The Lucigenin-(Cu-CDs) chemiluminescence sensor allows the simultaneous determination of o -toluenesulfonamide (TFA) and sulfamethoxazole (STZ) concentrations. Under optimal conditions, the sensor demonstrates the capability to detect TFA and STZ within the ranges of 50 μM–800 μM and 15 μM–120 μM, respectively. The limits of detection (LOD) for TFA and STZ are determined as 0.09 μM and 0.05 μM, respectively. While the limits of quantification (LOQ) are established at 0.3 μM and 0.17 μM, respectively. The feasibility of the method for determining TFA and STZ content in chicken samples was substantiated, demonstrating spiked recovery rates ranging from 97.5% to 102.3 % and 97.5%–99.8 %, respectively. The possible reaction mechanism was clarified based on chemiluminescence, UV–vis measurement and free radical analysis results. The newly established system is characterized by stability, convenience, and robust anti-interference capabilities, thus expanding the application of carbon dots and offering a promising strategy for the detection of TFA and STZ.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Songhang Du,Minghao Sui,Yali Guo,Yichen Tian,Xinyuan Lv,Xingqi Qi
The piezocatalysis, in which piezoelectric polarization charges on the surface of piezocatalyst can initiate the generation of highly active species, has emerged as one of the effective strategies for organic pollutant removal in water and wastewater treatment. In this work, the composite piezoelectric material MoS 2 /SrTiO 3 (MS/STO) was prepared and characterized. The synergistically piezoelectric effect between SrTiO 3 and MoS 2 was proven by electrochemical tests. Using ultrasound (US) as inputting mechanical energy, MS/STO exhibited effective degradation (∼ 70.2 % in 20 min) towards target antibiotic (sulfamethoxazole, SMX) in water. Further improving effect of peroxymonosulfate (PMS) on US/(MS/STO) for the degradation of SMX was also investigated. The results revealed that SMX was completely degraded within 20 min. Influencing factors including operation parameters and water composition for SMX degradation in US/(MS/STO)/PMS were studied, which demonstrated the good environmental adaptability of the system. The active species generated in the reaction system were identified via quenching experiments and electron paramagnetic resonance analysis, revealing the presence of O 2 •− , 1 O 2 , • OH, and SO 4 •− . The possible reaction mechanism in US/(MS/STO)/PMS and the degrading pathway of SMX were proposed.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2025
·
IF 6.1
Yurong Zhang,Tiejun Li,Yuxin Lin,Dongdong Xu,Haifeng Jiao
Sulfonamide antibiotics, widely used in human and veterinary medicine as well as agriculture, pose environmental concerns due to their stability and poor biodegradability. This study fills a critical gap in understanding the ecological impact of sulfonamide antibiotics on marine microalgae, particularly Skeletonema costatum , a key primary producer in marine ecosystems. This study investigated the biological responses of the marine microalga Skeletonema costatum to sulfadiazine (SD) and sulfamethoxazole (SMX). Both antibiotics significantly impacted S. costatum , with SD having a more pronounced effect. Growth studies showed a clear dose-response relationship: Low concentrations (0.5 mg/L) of SD and SMX stimulated growth, while higher concentrations (3 mg/L, 5 mg/L, and 10 mg/L) inhibited growth. The 96-hour half-maximal inhibitory concentrations (96h-IC 50 ) were 1.654 mg/L and 1.838 mg/L, respectively, initially indicating that SD has a stronger inhibitory effect on S. costatum than SMX. Photosynthetic activity, measured by chlorophyll a content and the maximum quantum yield of photosystem II ( Fv/Fm ) values, showed that low concentrations (0.5 mg/L) of SD and SMX increased photosynthetic efficiency, while high concentrations (3 mg/L, 5 mg/L, and 10 mg/L) significantly inhibited it. Antioxidants activity analysis revealed that SD and SMX exposure altered superoxide dismutase (SOD), glutathione peroxidase (GSH-Px), glutathione reductase (GR), and malondialdehyde (MDA) levels. SOD, GR, and GSH-Px levels initially increased but later decreased, suggesting a synergistic effect, while MDA levels consistently increased, indicating oxidative stress and biochemical disruption in algal cells. The Integrated Biomarker Response Version 2 (IBRv2) index provided a comprehensive evaluation of the ecological risks posed by SD and SMX, demonstrating that these antibiotics can significantly disrupt the physiology of marine microalgae. The IBR v2 index provided a comprehensive evaluation of the ecological risks posed by SD and SMX, demonstrating that these antibiotics can significantly disrupt the physiology of marine microalgae. Higher IBR v2 values for SD exposure indicated more substantial impacts on S. costatum . This study underscores the significant ecological risks of sulfonamide antibiotics in marine environments, highlighting the need for further research and regulation to mitigate their impact.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Weichen Zeng,Yunan Gao,Xiaofei Li,Han Zhang,Yufei Cheng,Xueding Jiang,Hailong Wang
Antimony-doped tin dioxide reactive electrochemical membranes (ATO-REMs) exhibit robust catalytic activity, yet their large-scale application is hindered by the laborious multi-step synthesis of the conventional sol-gel method. Herein, we propose a facile electrodeposition strategy for fabricating ATO-REMs, involving sequential deposition of Sb and Sn on porous Ti substrates followed by thermal annealing. This method achieved uniform distribution of interconnected ATO clusters with low charge transfer resistance and high electrocatalytic activity. Through systematic analysis of experimental conditions and electrodeposition processes, a comprehensive mechanistic framework was established to elucidate how operating conditions and synthesis parameters influence electrocatalytic performance. By tuning the electrodeposition process, the optimized electrodeposited ATO-REM (EPATO-REM) achieved 99.1% removal of sulfamethoxazole (SMX) during single-pass filtration with a low energy consumption of 0.5 kWh m −3 , outperforming the conventional sol-gel-derived ATO-REM. Further investigations revealed that SMX degradation was driven by •OH oxidation and direct electron transfer, with seven intermediates identified and degradation pathways proposed. Furthermore, EPATO-REMs exhibited oxidation stability during 8-h operation, universal efficacy for diverse contaminants, and practical applicability in complex water matrices. This work provides a facile and scalable alternative to the labor-intensive sol-gel method for ATO-REM fabrication, advancing the development of high-performance REMs for water treatment.
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WATER ENVIRONMENT RESEARCH
·
2022
·Vol. 94
·期 12
·e10817
·
IF 3.306
Luo Xu,Cong Li,Guozijian Wei,Jie Ji,Eric Lichtfouse,Andreina García,Yunshu Zhang
Sulfamethoxazole (SMX) is one of veterinary drugs and food additives, which has been frequently detected in surface waters in recent years and will cause damage to organisms. Therefore, SMX was selected as a target to be investigated, including the degradation kinetics, evolution of toxicity, and antibiotic resistance genes (ARGs) of SMX during chlorination in batch reactors and water distribution systems (WDS), to determine the optimal factors for removing SMX. In the range of investigated pH (6.3–9.0), the SMX degradation had the fastest rate at close to neutral pH. The chlorination of SMX was affected by the initial total free chlorine concentration, and the degradation of SMX was consistent with second-order kinetics. The rate constants in batch reactors are (2.23 ± 0.07) × 10 2 M −1 s −1 and (5.04 ± 0.30) × 10 M −1 s −1 for HClO and ClO −1 , respectively. Moreover, the rate constants in WDS are (1.76 ± 0.07) × 10 2 M −1 s −1 and (4.06 ± 0.62) × 10 M −1 s −1 , respectively. The degradation rate of SMX was also affected by pipe material, and the rate followed the following order: stainless-steel pipe (SS) > ductile iron pipe (DI) > polyethylene pipe (PE). The degradation rate of SMX in the DI increased with increasing flow rate, but the increase was limited. In addition, SMX could increase the toxicity of water initially, yet the toxicity reduced to the level of tap water after 2-h chlorination. And the relative abundance of ARGs ( sul 1 and sul 2) of tap water samples was significantly increased under different chlorination conditions. Practitioner Points The degradation rate of SMX in batch reactor and WDS is different, and they could be described by first- or second-order kinetics. The degradation of SMX had the fastest rate at neutral pH. The degradation rate of SMX was also affected by pipe material and flow velocity. SMX increased the toxicity of water initially, yet the toxicity reduced after a 2-h chlorination. SMX increased the relative abundance of antibiotic resistance genes sul1 and sul2 .
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CHEMOSPHERE
·
2021
·
IF 7.086
Jieqi Feng,Qibin Tao,Hao Lan,Yi Xia,Qizhou Dai
In this study, nitrogen-doped carbon nanosheets (NCNSs) were prepared and successfully combined into the PbO 2 electrode by the composite electrodeposition technology , thereby NCNS–PbO 2 electrode was obtained. The electrochemical degradation of sulfamethoxazole (SMX) in aqueous solution by NCNS–PbO 2 electrode was studied. The main influence factors on the degradation of SMX, such as the initial concentration of SMX, current density, electrolyte concentration and initial pH value, were analyzed in detail. Under the optimal process conditions, after 120 min of treatment, the removal ratio of SMX and chemical oxygen demand (COD) reached 99.8 % and 60.7 %, respectively. The results showed that the electrochemical degradation of SMX fitted pseudo-first-order reaction kinetics. The electrochemical performance of NCNS–PbO 2 electrode was better than that of PbO 2 electrode by scanning electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy, as well as the use of cyclic voltammetry and electrochemical impedance spectroscopy for electrochemical performance testing. This was because the doping of nitrogen atoms improved the properties of carbon nanosheets. After the composite, the active sites on the surface of PbO 2 were improved, the particle size of PbO 2 was reduced, and the electrical conductivity and electrocatalytic activity of the electrode were improved. In addition, the intermediate products were determined by GC-MS method, and the possible degradation pathways of SMX were proposed.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Rui Wang,Jingjing Lou,Haijie Cao
Peroxymonosulfate(PMS)-based advanced oxidation process has demonstrated significant potential for the remediation of emerging organic contaminants in water. In this study, a sea urchin-like nickel-cobalt double hydroxide (Ni 1 Co 2 -LDH) catalyst was developed and exhibited superior performance and robust durability in PMS activation. The system achieved 99.28% removal of sulfamethoxazole (SMX) within 60 minutes, with a reaction rate constant of 0.1393 min −1 , and also exhibits broad applicability for degrading various representative organic pollutants. Radical quenching experiments and electron paramagnetic resonance spectroscopy identified singlet oxygen ( 1 O 2 ) as the predominant reactive species responsible for SMX degradation, followed by hydroxyl and sulfate radicals. Density functional theory calculations further revealed the critical role of oxygen molecules in both PMS activation via electron transfer and the generation of O •− 2 , a key precursor to 1 O 2 . The singlet oxygen exhibited high selectivity in degrading SMX through 1,2-addition reaction pathways. This study highlights the role of oxygen in PMS activation and provides valuable insights for addressing the challenge of persistent organic pollutants in complex aquatic environments.
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Frontiers in Bioengineering and Biotechnology
·
2024
·
IF 4.3
Ren Jiawei,Lu Hongbin,Lu Shaoyong,Huang Zhanggen
Antibiotics are an important pharmaceutical class excessively used by humans. Its presence in the soil can impact plant growth and induce antibiotic resistance. This research studies the effect of sulfamethoxazole (SMX) on plant growth, rhizosphere bacteria composition, and resistance genes. Two sets of vegetables (basil, cilantro, and spinach) were treated separately with water and SMX solution. The plant growth data and soil samples were collected and analyzed. The results revealed that SMX increased spinach leaf length (34.0%) while having no significant impacts on basil and cilantro. On the other hand, SMX improved the bacterial diversity in all samples. The shifts in the abundance of plant growth-promoting bacteria could indirectly affect vegetable stem and leaf length. SMX also significantly increased the abundance of resistance genes Sul1 and Sul2. A further study into the correlation between bacteria highlights the importance of Shingomonas and Alfipia for inhibiting the spread of key resistance gene hosts, namely, Pseudomonas, Stenotrophomonas, and Agrobacterium. This research provides insight into SMX’s impact on vegetable growth and microbial diversity. It also points out important microbial interactions that could potentially be utilized to mitigate ARG proliferation.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Wenhao Zhang,Rui Li,Mingfang Zhu,Wen Zhou,Mushen Lai,Huanru Liang,Rongkun Zhu,Hongqing Ye
The Ag 2 O @ MWCNTs nanocomposites material was prepared via simple, one-step situ precipitation method using conventional reagent. The obtained Ag 2 O @ MWCNTs was structurally characterized by scanning electron microscopy (SEM), fourier transform infrared spectroscopy (FTIR) and ultraviolet and visible spectrophotometry (UV–Vis). The functional GCE with Ag 2 O @ MWCNTs exhibits good electrochemical performances with a pair of quasi-reversible redox peak. While sulfamethoxazole (SMX) can interact with Ag(I) to form Ag-SMX complex, which makes the concentrations of silver ion involved in the redox reaction decreased, thus reducing the redox peak of Ag 2 O @ MWCNTs composites. The decreased oxidation peak current is found to be linear with the SMX concentrations from 0.02–100 nM and the detection limit was 4.06×10 -12 M (S/N=3) by using DPV method. Furthermore, the proposed method demonstrated excellent selectivity, repeatability and reproducibility, and can be successfully applied for the SMX analysis in human serum.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Sujuan Hu,Yongqi Wei,Jiao Wang,Yingjian Yu
Electroanalysis is an effective monitoring method for organic pollution in environmental samples. However, chemical fouling with the formation of non-conductive fouled films easily occurs on the surface of the electrode during organic pollution detection that would inactivate the electrode and affect the detecting sensitivity of organic pollution. In this work, we found that zeolitic imidazolate framework-8 (ZIF-8) electrode can achieve effective degradation of non-conductive fouled films under the light illumination during electrochemical detection of some typical organic pollution (sulfamethoxazole (SMX), Bisphenol A (BPA) and diclofenac sodium (DS)). Profiting from the charge transfer capability and photoelectric characteristics, ZIF-8 electrode exhibits a lower detection limitation for organic pollution detection and superior regeneration property. The nice detection and superior regenerated property are mainly due to non-selective superoxide radical (·O 2 − ) and hydroxyl radicals (·OH) mediation produced by ZIF-8 electrode under light illumination that can mineralize anodic fouled products and resume surface reactive sites. Compared with the single electrochemical determination, photo-assisted electroanalysis provides a stable monitoring and a renewable pathway for practical applications.
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