SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Xinyu Peng,Xiaoxian Zhang,Hongrui Chen,Xiaoran Zhang,Chaohong Tan,Xiaojuan Bai,Yongwei Gong,Yang Qu,Haiyan Li,Ziyang Zhang
In recent years, the escalating attention on Pharmaceutical and Personal Care Products (PPCPs) and Heavy Metals in urban stormwater runoff highlights the critical role of Road-deposited sediments (RDS) as a significant carrier for pollutant occurrence and transport in runoff. However, existing research has overlooked the composite characteristics of PPCPs and Heavy Metals, hampering a holistic understanding of their transformation in diverse forms within runoff. This limitation impedes the exploration of their subsequent migration and conversion properties, thereby obstructing coordinated strategies for the control of co-pollution in runoff. This study focuses on the typical PPCP sulfamethoxazole (SMX) and heavy metal Cu(II) to analyze their occurrence characteristics in the Runoff-RDS system. Kinetics and isotherm studies reveal that RDS effectively accumulates SMX and Cu(II), with both exhibiting rapid association with RDS in the early stages of runoff. The accumulation of SMX and Cu(II) accounts for over 80 % and 70 % of the total accumulation within the first 240 min and 60 min, respectively. Moreover, as runoff pH values decrease, the initially synergistic effect between the co-pollutant transforms into an antagonistic effect. In the composite system, varying pH values from 2.0 to 6.0 lead to an increase in SMX accumulation from 4.01 mg/kg to 6.19 mg/kg and Cu(II) accumulation from 0.43 mg/g to 3.39 mg/g. Compared to the single system, the composite system capacity for SMX and Cu(II) increases by 0.04 mg/kg and 0.33 mg/g at pH 4.0. However, at pH 3.0, the composite system capacity for SMX and Cu(II) decreases by 0.21 mg/kg and 0.36 mg/g, respectively. Protonation/deprotonation of SMX under different pH conditions influences electrostatic repulsion/attraction between SMX and RDS. The mechanism of RDS accumulation of SMX involves Electron Donor-Acceptor (EDA) interaction, hydrogen bond interaction, and Lewis acid-base interaction. Cu(II) enrichment on RDS includes surface complexation reaction, electrostatic interaction, and surface precipitation. Complex formation enhances the accumulation of both SMX and Cu(II) on RDS in runoff. This study elucidates the co-occurrence characteristics and mechanisms of SMX and Cu(II) co-pollution in runoff systems. The findings contribute valuable insights to understanding the existence patterns and mechanisms of co-pollution, providing a reference for investigating the migration and fate of co-pollutant in runoff. Moreover, these insights could offer guidance for the development of effective strategies to mitigate co-pollution in rainwater.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Ya Jiao,Xian Li,Guohao Cheng,Jingfan Chen,Li Wang,Yongli Liu,Guifen Zhu
Metal–organic frameworks (MOFs) are used as novel adsorption materials owing to their large surface area and tunable pore size. However, the lack of selectivity considerably limits their application. Consequently, designing functionalized MOFs with specific recognition abilities is essential for enhancing their adsorption performance. Herein, we synthesized a functionalized NH 2 -UiO-66 composite modified by molecularly imprinted polymers (MIP@NH 2 -UiO-66) via a one-step polymerization process in which NH 2 -UiO-66 and MIP were formed simultaneously. Results demonstrate that MIP@NH 2 -UiO-66 effectively recognized sulfamethoxazole (SMX) in complex matrices. The adsorption equilibrium was reached in only 30 min, and this fast SMX adsorption on MIP@NH 2 -UiO-66 was described by the Avrami kinetic model, which indicates a spontaneous and exothermic adsorption process. Within the pH range of 3.0–10.0, MIP@NH 2 -UiO-66 exhibited an optimal binding capacity for SMX, and the maximum adsorption of SMX was 68.36 mg g −1 at 25°C, which exceeded those of existing adsorption materials (< 60.10 mg g −1 ). Additionally, MIP@NH 2 -UiO-66 was regenerated for ∼17 cycles compared to less than eight cycles for the other adsorbents. MIP@NH 2 -UiO-66 effectively removed 90.58%–99.60% of SMX from river water, rainwater, soil, sediment, chicken, pork, and milk samples, with a relative standard deviation of less than 4.43%. The superior adsorption of SMX on MIP@NH 2 -UiO-66 was primarily driven by the synergistic effects of the imprinting sites, hydrogen bonding, and electrostatic forces. The one-step polymerization method substantially simplified the synthesis process and reduced the costs, which are promising factors for the synthesis of MOFs with high selectivity.
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高影响因子
Journal of Environmental Health Science and Engineering
·
2021
·Vol. 19
·期 1
·23-38
·
IF 2.13
Hassan Mahdi,Zhu Guangcan,Yang Zhonglian,Lu Yongze
In this study, at an electric current intensity at 60 mA, more than 90.50 ± 4.76% of Sulfamethoxazole (SMX) was degraded. The strengthening of bacterial metabolisms and the sustainment of electrical stimulation contributed to the rapid removal of SMX and nitrates from simulated wastewater by a novel 3D-BER system. From the literature, very few studies have been performed to investigate the high risk of nitrates and antibiotics SMX found in wastewater treatment. The highest antibiotic SMX and nitrogen removal efficiency was 96.45 ± 2.4% (nitrate-N), 99.5 ± 1.5% (nitrite-N), 88.45 ± 1.4% (ammonia-N), 78.6 ± 1.0% (total nitrogen), and SMX (90.50 ± 4.76%), respectively. These results were significantly higher as compared to control system ( p < 0.05). The highest denitrification efficiency was achieved at the pH level of 7.0 ± 0.20 ̶ 7.5 ± 0.31. Lower or higher pH value can effect on an approach of heterotrophic-autotrophic denitrification. Moreover, low current intensity did not show any significant effect on the degradation, however, enhanced the removal rate of nitrate or nitrite as well as antibiotic SMX. Based on the results of HPLC and LC-MS/MS analysis, the intermediate products were proposed after efficient biodegradation of SMX. Finally, these results is expected to provide some new insights towards the high electric currents, changes the bacterial community structure, and the activated sludge which played an important role in the biodegradation of SMX and nitrates removal more efficiently.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Qingdong Qin,Ting Liu,Jiaxuan Zhang,Rui Wei,Shijie You,Yan Xu
Hematite (α-Fe 2 O 3 ) has been commonly used as an eco-friendly catalyst for peroxymonosulfate (PMS) to generate free radicals (SO 4 •- and/or •OH). However, the activation efficiency of PMS relies heavily on the conversion of Fe(III) to Fe(II) that is slow and rate-limiting. In this study, oxygen vacancies enriched α-Fe 2 O 3 was prepared from thermally treated goethite (α-FeOOH) and employed as a PMS activator. Systematic characterization demonstrated that α-Fe 2 O 3 with most abundant oxygen vacancies could be obtained by heating α-FeOOH at 300 °C. The as-prepared α-Fe 2 O 3 exhibited excellent catalytic activity in activation of PMS for oxidation of sulfamethoxazole (SMX, k = 0.04 min −1 ). The SMX degradation rate was found to be positively correlated with the concentration of oxygen vacancies. Quenching experiments, EPR, LC/MS and XPS analysis revealed that singlet oxygen ( 1 O 2 ) was the predominant reactive oxygen species . The effects of pH, PMS dosage, catalyst loading, temperature, and anions on SMX degradation were comprehensively investigated. Moreover, the plausible degradation pathways of SMX in the α-Fe 2 O 3 /PMS system were proposed. This work not only provides a valuable insight into the mechanism of PMS activation by α-Fe 2 O 3 but also establishes a new strategy for the design of more efficient and practical iron-based catalyst for PMS activation.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Yali Song,Long Huang,Xiaojing Zhang,Hongzhong Zhang,Lan Wang,Huan Zhang,Yali Liu
A method combining g-C 3 N 4 and potassium peroxydisulfate (PDS) under simulated sunlight was put forward to effectively degrade sulfamethoxazole (SMX). The SMX removal efficiency was substantially improved compared with the processes involving only g-C 3 N 4 or PDS. The kinetic constants for the g-C 3 N 4, PDS and g-C 3 N 4 /PDS systems were 0.0023, 0.0239 and 0.068 min −1 , respectively. The g-C 3 N 4 /PDS process reached an SMX removal rate of 98.4 % after 60 min of simulated sunlight; in addition, the proposed system showed desirable efficiency for SMX degradation in two different actual water samples as well. The reaction mechanism was illustrated by trapping experiments, which showed that g-C 3 N 4 can promote S 2 O 8 2− to transfer SO 4 − , S 2 O 8 2− favored the generation of O 2 − , and O 2 − , SO 4 − and holes (h + ) were the main oxidative species for the SMX degradation in the combined reaction process under simulated sunlight. Then, to further explore this mechanism, the intermediates generated during the combined reaction process were analyzed by LC/MS and possible degradation pathways were proposed. The result showed that the breaking of the S N and C–S bonds, the hydroxylation of the benzene ring and the oxidation of the amino group were identified as the main pathways in the SMX degradation process by the g-C 3 N 4 /PDS system under simulated sunlight.
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Yuqing Zhang,Junrong Li,Lili Si,Mingming Gao,Shuguang Wang,Xinhua Wang
Antibiotic shock may potentially impact the performance of promising microalgae-nitrifying bacteria consortia (MNBC) processes. This study investigated physiological behaviors of MNBC under sulfamethoxazole (SMX) shock (mg/L level) and verified a light regulating strategy for improving process performance. Results showed that SMX shock did not affect ammonium removal but caused nitrite accumulation, resulting from combined effects of excessive reactive oxidative species (ROS) production, inhibited microalgal photosynthetic activity, upregulated expressions of amoA and hao , and downregulated expression of nxrA . Moreover, high ammonium concentration aggravated nitrite accumulation and reduced ammonium removal owing to significantly reduced dissolved oxygen (DO). Increasing light intensity enhanced microalgal photo-oxygenation and promoted expressions of all nitrification-related genes, thus improving ammonium removal and alleviating nitrite accumulation. A central composite design coupled with response surface methodology (CCD-RSM) further demonstrated the negative impacts of SMX shock and high ammonium on MNBC and the effectiveness of the light regulation in maintaining stable process performance. This study provides theoretical basis for physiological responses and regulatory strategy of the MNBC process facing short-term antibiotic shock.
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高影响因子
Green Processing and Synthesis
·
2024
·Vol. 13
·期 1
·
IF 3.8
Xiaofei Zhen,Han Zhan,Ruonan Jiao,Ke Li,Wenbing Wu,Lei Feng,Tie Du
Medium-temperature anaerobic digestion experiments lasting for 55 days were conducted using sulfamethoxazole (SMX)-containing chicken manure in sequential batch reactors added with nano-Fe 2 O 3 at a concentration of 300 mg·kg −1 ·TS or nano-C 60 at a concentration of 100 mg·kg −1 ·TS. The effects of nanoparticles on the anaerobic digestion properties of SMX-containing chicken manure were assessed by measuring the following indicators: biogas production by anaerobic digestion, chemical parameters, enzyme concentrations, and bacterial diversity and changes in antibiotic concentrations over time. The law of bacterial degradation of SMX was analyzed. The results showed that (1) adding either nano-Fe 2 O 3 or nano-C 60 promoted biogas production by anaerobic production from chicken manure containing different concentrations of SMX, and the cumulative biogas production in Fe 2 O 3 and nano-C 60 increased by 35.4% and 130.7%, respectively. The final cumulative biogas productions in different groups were as follows: 3,712(CK), 4,281(S1), 3,968(S2), 4,061(S3), 4,498(S4), and 4,639(S5) mL and the final concentration of SMX residues varied between 99.79% and 99.94%; (2) Bacterial abundance at the phylum level: on day 1, Firmicutes and Bacteroidota were the main dominant bacterial phyla, with relative abundances of 45.13–68.53% and 26.12–48.32%, respectively. The addition of nanoparticles increased the abundance of Bacteroidota in S4 and S5 significantly. The abundance of Bacteroidota was slightly higher in the group added with nanoparticles than in S2. On day 50, Firmicutes became the dominant bacterial phylum, and its relative abundance varied little across the groups, ranging from 90.87% to 94.54%; (3) At different stages, the bacterial community structure at the genus level was dramatically affected by substrates. As nutrients were being depleted, some bacterial communities lost their original competitive advantages. On day 5, the relative abundance of Prevotella increased. Especially, the relative abundances of Prevotella in S4 and S5 added with nanoparticles were lower than that in S2 by 8–10%. On day 15, the relative abundance of Prevotella in S2 decreased compared with the control group CK. A decrease was also observed in S4 and S5, although to a smaller extent than in S2.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zedian Li,Wenxuan Jiang,Yifan Li,Dahai Zhu,He Guo
The treatment of organics in aqueous systems with non-thermal plasma (NTP) technology has shown excellent advantages. However, the effects of spontaneous heat generation and the presence of effective free radicals in the system are often overlooked. This study explores the enhanced degradation of sulfamethoxazole in water using NTP-activated persulfate (PS), with a focus on the synergistic effects of heat and reactive radicals. The results indicate that combining PS (3 mM) with heat (30°C controlled) significantly enhances pollutant removal (30 mg L –1 ) in the pulsed dielectric barrier discharge reactor. Optimal efficiency reaches an impressive 99.1% elimination rate with a kinetic constant of 0.166 min -1 , using a PS dose ratio of 15:1 and an input power of 64.8 W. Notably, the reaction rate for NTP/PS at 30°C controlled is increased by 97.6% relative to room temperature condition. It demonstrates that the role of heat in a plasma system cannot be ignored. Radical quenching experiments and electron spin resonance tests identify SO 4 • – , •OH, •O 2 – , 1 O 2 , and e⁻ as the major active species contributing to the degradation process. The O 3 and H 2 O 2 play important roles in the production of SO 4 • - and•OH. Besides, the degradation process does not yield any highly toxic by-products, ensuring environmental safety. This research introduces an innovative and environmentally friendly method to enhance the removal of organic pollutants by plasma/PS-heat systems.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Bin-Di Mao,Kai-Yuan Li,Ashiwin Vadiveloo,Jun-Jie Gu,Feng Gao
Recent studies have revealed that N -acyl-homoserine lactones (AHLs), common quorum-sensing (QS) signal molecules in Gram-negative bacteria, can also influence microalgal cells. However, their role in regulating the metabolism of pollutants, such as antibiotics, within microalgae remains poorly understood. This study investigated the effects of N -hexanoyl-L-homoserine lactone (C6-HSL) on the degradation of sulfamethoxazole (SMX) in aquaculture wastewater by Chlorella vulgaris . The addition of 0.5 μM C6-HSL resulted in the highest biomass accumulation and the maximum SMX removal efficiency (95.6 %). At optimal concentrations, C6-HSL effectively modulated key secondary messenger signaling pathways including reactive oxygen species (ROS), nitric oxide (NO), and calcium ions (Ca 2+ ) in microalgal cells. Additionally, it upregulated the activity of detoxification enzymes such as glutathione S-transferase (GST) and cytochrome P450 (CYP450), thereby altering SMX degradation pathways and significantly enhancing its removal. Transcriptomic analysis further demonstrated that exogenous C6-HSL upregulated critical genes associated with ROS, Ca 2+ , and NO signaling, along with genes encoding antioxidant enzymes and those involved in SMX metabolism. These findings indicated that C6-HSL, as a bacterial QS signal, could enhance microalgal tolerance and antibiotic degradation, offering a novel strategy to improve microalgae-based antibiotic removal in wastewater treatment.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Heng Zhang,Mengfan Luo,Peng Zhou,Yang Liu,Ye Du,Chuanshu He,Gang Yao,Bo Lai
Recently, the enhancing role of hydrogen peroxide (H 2 O 2 ), a self-decay product of ferrate (Fe(VI)), on Fe(VI) reactivity has received increasing attention. In this study, we found that calcium peroxide (CaO 2 ) as a slow-releasing reagent of H 2 O 2 could also enhance the Fe(VI) performance for removing sulfamethoxazole (SMX). Compared with sole Fe(VI), sole CaO 2 and Fe(VI)-H 2 O 2 systems, the Fe(VI)-CaO 2 system showed higher reactivity to remove SMX. The radical scavenger and chemical probe test results indicated that the better oxidation performance of Fe(VI)-CaO 2 system than Fe(VI) alone was ascribed to the generation of Fe(Ⅳ) and Fe(Ⅴ) rather than • OH. In addition, the performance of Fe(VI)-CaO 2 system for degradation of contaminants was also superior to Fe(VI)-Na 2 SO 3 , Fe(VI)-NaHSO 3 and Fe(VI)-Na 2 S 2 O 3 systems under the same experimental conditions. Moreover, the effects of critical operating parameters, inorganic anions, inorganic cations, and humic acid on the degradation of SMX by Fe(VI)-CaO 2 system were revealed. The Fe(VI)-CaO 2 system exhibited good applicability in authentic water. Finally, the underlying degradation intermediates of SMX by Fe(VI)-CaO 2 system and their toxicity were confirmed. In conclusion, this study provides a new strategy for enhancing the oxidation capacity of Fe(VI) and comprehensively reveals the oxidation mechanism.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yongli He,Jiali Zhang,Hongyu Zhou,Gang Yao,Bo Lai
In this study, bimetallic particles (CuO@FeO x @Fe 0 ) were prepared by displacement plating and calcination to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). First, the key preparation parameters (i.e., theoretical Cu mass loading (TML Cu ) and calcination temperature) of CuO@FeO x @Fe 0 preparation were investigated by single-factor experiments. Then the properties of CuO@FeO x @Fe 0 were analyzed by scanning electron microscope energy dispersive spectrometry (SEM-EDS), energy dispersive spectrometry mapping (EDS-mapping), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Subsequently, effects of PMS dosage, CuO@FeO x @Fe 0 dosage and initial pH on the degradation of sulfamethoxazole were studied respectively. Meanwhile, the results of control experiments indicated that the initial SMX degradation efficiency of CuO@FeO x @Fe 0 system was slower, but the final degradation rate was higher than that of Fe 0 /PMS system, which was due to the sustained release effect of Fe 2+ . In addition, the quantitative experiment of SO 4 − indicated that SO 4 − generated continuously in CuO@FeO x @Fe 0 /PMS system. Furthermore, the detection results of quenching tests and electron paramagnetic resonance (EPR) revealed the generation of multiple reactive oxygen species (i.e., SO 4 − , HO , O 2 − , 1 O 2 ) in CuO@FeO x @Fe 0 /PMS system, which degraded SMX synergistically. Finally, the SMX degradation pathways were proposed based on the intermediates detected by Liquid Chromatography-Quadrupole time of flight – Mass Spectrum (LC-QTOF-MS/MS) and the activation mechanism of CuO@FeO x @Fe 0 /PMS system was analyzed in detail. This study provided a new insight on the application of CuO@FeO x @Fe 0 on organic pollutant degradation.
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高影响因子
ANALYTICA CHIMICA ACTA
·
2010
·
IF 3.757
Xueqiao Xie,Yun Wang,Juan Han,Yongsheng Yan
Based on the poly(propylene glycol) 400 (PPG 400 )–salt aqueous two-phase system (ATPS), a green, economical and effective sample pretreatment technique coupled with high performance liquid chromatography was proposed for the separation and determination of sulfamethoxazole (SMX). The extraction yield of SMX in PPG 400 –salt ATPS is influenced by various factors, including the salt species, the amount of salt, pH, and the temperature. Under the optimum conditions, most of SMX was partitioning into the polymer-rich phase with the average extraction efficiency of 99.2%, which may be attributed to the hydrophobic interaction and salting-out effect. This extraction technique has been successfully applied to the analysis of SMX in real water samples with the recoveries of 96.0–100.6%, the detection limits of 0.1 μg L −1 , and the linear ranges of 2.5–250.0 μg L −1 .
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危险品化学品经营许可证（带存储）