CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Shizong Wang,Lejin Xu,Jianlong Wang
Metal-free carbonaceous persulfate activator has received increasing attention recently. Graphitic carbon nitride (g-C 3 N 4 ) is one of the promising carbon materials due to excellent stability and low cost, but its activity for peroxymonosulfate (PMS) activation is low. In this study, g-C 3 N 4 was modified with oxygen atoms in the first step (O-g-C 3 N 4 ), then exfoliated via sequential thermal and ultrasound treatment to produce O-g-C 3 N 4 nanoflakes to increase its catalytic activity to activate PMS. In the presence of O-g-C 3 N 4 nanoflakes, SMX degradation rate achieved 0.079 min −1 , which was much faster than that in the presence of pristine g-C 3 N 4 (0.0083 min −1 ) and untreated O-g-C 3 N 4 (0.012 min −1 ). The surface-bound radicals and direct electron transfer between SMX and PMS contributed to the SMX degradation. Density functional theory (DFT) simulation revealed that oxygen-doping changed the charge distribution. Furthermore, O-g-C 3 N 4 nanoflakes had higher adsorption energy for PMS and SMX (0.518 kcal/mol) than pristine g-C 3 N 4 (0.304 kcal/mol), which contributed to the enhanced PMS activation and SMX degradation. Cycling experiments and comparison of characterization results before and after experiments proved that O-g-C 3 N 4 nanoflakes had superior catalytic and structural stability. This study could provide a high efficient metal-free carbonaceous activator of PMS for the degradation of antibiotics in the wastewater.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Yali Song,Xiaoyu Wen,Ziyan Li,Cairong Yang,Xiaojing Zhang,Long Huang,Yongpeng Ma,Qiong Wang,Hongzhong Zhang
g–C 3 N 4 / PDI–g–C 3 N 4 homojunction (CPCN–X) was prepared to effectively remove sulfamethoxazole (SMX) from water under visible light. The band of CPCN–X bent and the new flat band potential resulted in the generation of a built–in electric field at the contact interface between PDI–g–C 3 N 4 (CNPDI) and g–C 3 N 4 (CN). This facilitated interlayer charge migration, optimized the transportation efficiency of photoinduced electron pairs, and thereby boosted photocatalytic activity. CPCN–6 photocatalyst prepared with a mass ratio of 1:6 (CNPDI to CN) exhibited the highest photocatalytic activity, which can degrade 97.0 % of SMX after 90 min of visible light irradiation. The related degradation rate constant was calculated as 0.0371 min −1 , which was a 2.3 and 4.7 fold increase in comparison to CNPDI and CN, respectively. Free radical scavenging experiments revealed that ·O 2 − and h + were the predominant active materials for the photocatalytic decomposition of SMX by CPCN–6, while ·OH and 1 O 2 exhibited a relatively negligible contribution. It was found that CPCN–6 exhibited the potential to degrade sulfonamide antibiotics and the limited ability to remove atrazine and phenol in the visible light region due to the difference of redox properties and molecular structure.
研究领域:
环境科学
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光催化
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材料化学
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水处理
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环境工程
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
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IF 7.968
Wenjun Zhu,Sylvestre Ndayiragije,Xiaohua Zuo,Xiaofei Zhang,Guanghui Wang,Xiaobo Wang
Single-atom Cu and N co-coordinated porous carbon (Cu-N-C) was synthesized by hydrothermal-calcination using zinc zeolite imidazole frameworks (ZIF-8) as the precursor. The catalyst showed excellent adsorption and catalytic ability due to the ideally-dispersed single atomic copper sites and the unique nitrogen-doped porous carbon. The complete removal of sulfamethoxazole (SMX, 18 mg/L) could be achieved within 40 min of pre-adsorption and 25 min of oxidative degradation in the present of peroxymonosulfate (PMS). The adsorption capacity of Cu-N-C (0.2 g/L) was evaluated to be 58.69 mg/g. The apparent degradation rate constant ( k ) of SMX on Cu-N-C was 0.155 min -1 , which was 14.1 times faster than that on N-C (0.011 min -1 ). From the activation mechanism, it was found that CuN units acted as the main active sites in Cu-N-C for PMS activation . EPR analysis and quenching experiments verified that the reactive oxygen species (ROSs) of SO 4 · - and 1 O 2 were involved in the decomposition and mineralization of SMX. This work provides a new perspective for the development of Fenton-like single-atom catalysts.
研究领域:
环境科学
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催化材料
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污染治理
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Hai-Liang Song,Chen Zhang,Yu-Xiang Lu,Hua Li,Yi Shao,Yu-Li Yang
Soil microbial fuel cells (MFCs) have been applied for the in situ remediation of soils polluted by single antibiotics. However, the investigation of only single antibiotic pollution has hindered MFC application in real-world soil remediation , where the effects of multiple antibiotics with similar chemical structures on the fate of antibiotics and their corresponding antibiotic resistance genes (ARGs) remain unknown. In this study, antibiotic removal rates, microbial community compositions, metabolite compositions, and ARG abundances were investigated in soil MFCs by adding two commonly used antibiotics (sulfadiazine, SDZ, and sulfamethoxazole, SMX), and comparing them with the addition of only a single antibiotic (SDZ). The antibiotic removal rate was higher in the soil MFC with addition of mixed antibiotics compared to the single antibiotic due to enhanced biodegradation efficiency in both the upper (57.24% of the initial antibiotic concentration) and lower layers (57.07% of the initial concentration) of the antibiotic-polluted soils. Bacterial community diversity in the mixed antibiotic conditions increased, and this likely resulted from the decreased toxicity of intermediates produced during antibiotic biodegradation. Moreover, the addition of mixed antibiotics led to lower risks of ARG release into soil environments, as reflected by higher abundances of host bacteria in the single antibiotic treatment. These results encourage the further development of soil MFC technology for in situ remediation of antibiotic-polluted soils.
研究领域:
环境科学
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微生物学
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生物技术
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DOI
PubMed
高影响因子
Water
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2024
·Vol. 16
·期 3
·505
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IF 3
Yuting He,Jiantao Lin,Yuchuan Yang,Minghua Liu,Yifan Liu
Modified sludge biochar, recognized for its notable economic and environmental benefits, demonstrates potential as an effective catalyst for peroxydisulfate (PDS) activation. Nevertheless, the specific mechanisms underlying its catalytic performance require more comprehensive investigation. In this study, a modified biochar (TSBC) doped with oxygen (O) and nitrogen (N) atoms was synthesized from sewage sludge and tannin extract, which significantly enhanced the activation of PDS for the degradation of sulfamethoxazole (SMX). The TSBC/PDS system demonstrated robust performance for SMX degradation, achieving over 90% efficiency over a wide pH range (3–10). Subsequent quenching experiments demonstrated that TSBC predominantly catalyzed PDS to generateO21, which effectively degraded SMX via a non-radical pathway. The O- and N-containing functional groups in TSBC were identified as the primary catalytic sites. Besides, density functional theory (DFT) calculations revealed that the incorporation of graphitic N significantly improved the adsorption capacity of PDS on the TSBC surface. Furthermore, based on the identification of intermediates and theoretical calculations, SMX was degraded mainly by two different pathways: S-N cleavage andO21oxidation. This study offers a foundational framework for the targeted modification of sludge biochar, thereby expanding its applications.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
Chemical Engineering and Processing-Process Intensification
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2023
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IF 4.3
Mohammad Zahir Akbari,Yifeng Xu,Chuanzhou Liang,Zhikun Lu,Siyuan Shen,Lai Peng
Nanocomposite-based photocatalytic degradation of sulfamethoxazole (SMX) is frequently used for wastewater treatment. However, applying various nanoparticles led to different removal efficiencies and levels of environmental toxicity. Herein, we synthesized and characterized ZnO@VC to enhance the photocatalytic degradation of SMX. Effects of SMX concentration, catalyst dosage, pH, water matrix and role of reactive oxygen specious (ROS) were evaluated. Results confirmed 97.69±0.95% (5 mg L −1 SMX/0.05 g L −1 catalyst) removal efficiency followed pseudo-first-order kinetic. Higher SMX concentration and higher catalyst dosage reduced degradation efficiency because of the prevention of catalyst active-sites and limiting light availability. SMX removal efficiency was slightly reduced in synthetic wastewater (SWW) and tap water (TW) by anions scavenging ROS. Due to pH reliance of SMX anionic-density, the degradation efficiency was positively and negatively impacted by acidic and basic environment, and pH values below and over the catalyst point of zero charge (PZC), respectively. Quenching test revealed that some specious of ROS play more important role in photocatalytic degradation of SMX. Two degradation pathways of SMX photocatalytic decomposition were described. The synthesized catalyst showed good stability in terms of reusability. The results revealed that ZnO@VC with high detoxification ability (97%) could be a promising photocatalyst for treatment of antibiotics from water and wastewater.
研究领域:
环境科学
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材料科学
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毒理学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Xueyu Wei,Saraschandra Naraginti,Xiaofan Yang,Xiaoping Xu,Jiyuan Li,Meiqing Zhu,Pengli Chen,Pei Jiang
The simultaneous degradation of organic pollutants and generation of value-added compounds like ammonia and hydrogen energy has recently gained considerable attention in photocatalysis . The present study deals with successful preparation of novel AgVO 3 nanowire@rGO-tetrahedral Ag 3 PO 4 (110) (AGA) heterojunction and utilized for enhanced generation of NH 3 and H 2 from N-containing antibiotic sulfamethoxazole (SMX) under visible light. The prepared catalyst was well characterized by XRD , SEM, TEM and XPS to confirm the formation of heterojunction . The results indicated that the composite exhibited 546.0 μmol g −1 of hydrogen evolution rate, which is approximately 3.6 (153.6 μmol g −1 ) and 5.1 (108.7 μmol g −1 ) times higher than the pure AgVO 3 and Ag 3 PO 4 respectively after 6 h. Similarly, 38.3 mg L −1 g −1 of NH 3 generation was observed during 6 h of SMX degradation, which is about 1.9 and 2.8 times higher than the pure AgVO 3 (20.1 mg L −1 g −1 ) and Ag 3 PO 4 (13.7 mg L −1 g −1 ) respectively. The formation of heterojunction between AgVO 3 and Ag 3 PO 4 not only promotes the transfer of electron but also prevents the recombination which eventually enhances the catalytic conversion of N-element to NH 3 and for H 2 generation during water splitting. Furthermore, the plausible degradation pathway in SMX was proposed and the results revealed that the SMX was mineralized by the composite further converted to NH 3 and generates H 2 during the degradation process . Thus, our study provides new insights into novel photocatalytic treatment methodologies for simultaneous degradation of SMX to produce NH 3 and H 2 as value-added compounds from antibiotic wastewaters during water treatment process.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2025
·
IF 7.3
Yu Han,Xingzhou Yu,Yanan Liu,Min Zhang,Xianke Huang,Yinan Zhang,Hangjun Zhang
As the metabolic center of crustacean invertebrates, hepatopancreas plays a crucial role in metabolic detoxification and nutrient storage. Although sulfamethoxazole (SMX) and tire micro-particles (TMPs) are emerging marine pollutants, their combined hepatotoxic effects on lipid metabolism in crustaceans remain poorly understood. In this study, Litopenaeus vannamei were exposed to SMX and TMPs for 14 days. Hepatopancreatic lesions, lipid metabolism parameters, SMX bioaccumulation, and transcriptomic analysis were evaluated. Results revealed that SMX and TMPs co-exposure induced: (1) significant histological damage to hepatopancreas, accompanied by elevated levels of hepatopancreatic lesion markers; (2) a marked increase in lipid accumulation and altered fatty acid composition in hepatopancreas; (3) enhanced activities of lipid synthesis enzymes, increased triglyceride and total cholesterol levels, and reduced lipase activity; (4) dysregulation of metabolic pathways, characterized by upregulation of fatty acid synthesis-related pathways and downregulation of fatty acid decomposition-related pathways, alongside disruption of oxidative stress and detoxification pathways. Comparative analysis illustrated that SMX and TMPs co-exposure exhibited more toxicity than individual treatments. These findings demonstrated that SMX and TMPs synergistically impair hepatopancreatic function via lipid metabolism disruption and bioaccumulation, posing a potential threat to crustacean health and significant ecological risks in marine environments.
研究领域:
海洋污染毒理学
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无脊椎动物病理学
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脂质代谢
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分子生态毒理学
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生物蓄积研究
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lixia Jia,Qi Zhou,Yuanwei Li,Weizhong Wu
In this study, Mn-C composites using different MnO 2 contents and solid carbon material were prepared to explore the synchronous removal performance of nutrients and SMX. Higher nitrate removal performance (97–98 %) with quickest nitrate removal rate (4.97 mg N L -1 h −1 ) was obtained in Mn_20 systems. The increased Mn content and Mn-P compound were observed via surface characteristics, indicating the involvement of MnOx in pollutants removal , particularly for higher phosphorus removal (84–89 %) via Mn-P precipitation and BioMnOx adsorption. Nevertheless, compared to systems based on Mn_0 composites (74 %), systems with Mn-C composites presented lower SMX reduction efficiency (34–51 %), which might be attributed to the large Mn(II) accumulation, impairing certain microbes and lower the MnOx function. Higher abundance of genera affiliated to Bacteroidetes_vadinHA17 and Rhodocyclaceae was observed in the Mn-C composites, as well as the gathering of Geobacter and Desulfovibrio as keystone taxa, responsible for the removal of nitrate and SMX and microbial interactions. Besides, the increase of sulfonamide ARGs was closely related to the predominant microbes in the Mn-C composites, which acted as the hosts of ARGs. This study broadens the knowledge of Mn-C composites in synergetic removal of nutrients and organics, and supports the potential application of manganese oxide in wastewater treatment.
研究领域:
环境科学
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废水处理
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微生物学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jialong Yin,Heng Zhang,Mengfan Luo,Jia Zhao,Bingkun Huang,Pinji Chen,Zhenpeng Cai,Yue Yuan,Yang Liu,Chuanshu He,Bo Lai
The ferrous species (Fe(II))-periodate (PI) system employs efficient decontamination by generating ferryl species (Fe(IV)-oxo) under acidic pH conditions. However, the mechanisms by which the Fe(II)/PI system operates across a broad pH range remain elusive. In light of the rapid oxidation and consumption of Fe(II) at neutral pH, we developed an electro-Fe(II) system utilizing an iron plate anode to activate PI (E(Fe/C)/PI). Efficient sulfamethoxazole (SMX) degradation was achieved under the E(Fe/C)/PI system across a range of pH values. Quenching and chemical probe experiments revealed a transition from Fe(IV)-oxo to singlet oxygen ( 1 O 2 ) as the predominant reactive species from acidic to near-neutral pH, respectively. Density functional theory (DFT) calculations indicated that the differences in one-electron transfer capacity and hydrolysis pathways for various protonated Fe(IV)-oxo species underlie the variations in catalytic mechanisms. This study not only enhances the efficiency of the Fe(II)/PI system but also provides a comprehensive understanding of the activation mechanisms at different pH levels.
研究领域:
环境化学
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电化学
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催化
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水处理
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Dawei Gao,Haixiang Wang,Qiaoli Lu,Chao Ye,Jingsheng Cai,Lili Wang
Antibiotics, widely used to treat bacterial infections and as agricultural feed additives, pose significant environmental threats due to their persistence, particularly sulfamethoxazole (SMX), which is frequently detected in various ecosystems. Traditional wastewater treatment methods are often ineffective in their removal. This study presents a cost-effective three-dimensional CCF@MoS 2 @GA-Fe (CMGF) catalyst, with cotton fabric as a support to enhance peroxymonosulfate (PMS) activation in advanced oxidation processes (AOPs). Findings indicates that Mo(IV) active sites in CMGF significantly enhanced electron transfer and redox cycling of Fe(II)/Fe(III), ensuring sustained PMS activation and achieving approximately 3.8 times higher degradation efficiency compared to non-catalytic processes. After five cycles, CMGF retains its high catalytic activity. Key active species during PMS activation include singlet oxygen ( 1 O 2 ), hydroxyl radicals (•OH), and sulfate radicals (SO 4 − •). This research elucidates the catalytic mechanisms and degradation pathways of the CMGF/PMS system, highlighting its potential for removing organic pollutants from water.
研究领域:
环境科学
·
化学工程
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Shengnan Li,Xuya Zhu,Hang Yu,Xizi Wang,Xiaqing Liu,Hui Yang,Fengxiang Li,Qixing Zhou
Antibiotic wastewater presents serious challenges in water treatment . Metal-organic frameworks (MOFs) have received significant attention as promising precursors and sacrificial templates in the preparation of porous carbon-supported catalysts. Herein, we investigated the sulfamethoxazole (SMX) degradation and electrochemical performance of microbial fuel cells (MFCs) that applied as-prepared Ni-MOF-74 and Ni–N–C (Ni-MOF-74 underwent pyrolysis treatment at different temperatures) as air-cathode catalyst. Firstly, the electrocatalytic activity towards oxygen reduction reaction (ORR) of the catalyst was investigated by rotating disk electrode. The results showed that electron transfer number for Ni-MOF-74 was 2.12, while that of 800Ni–N–C was 3.44, which was close to four-electron reduction. Applying Ni-MOF-74 in MFCs, a maximum power density of 446 mW/m 2 was obtained, which was close to that of 800Ni–N–C. Besides, using Ni-MOF-74 as cathode catalyst, a chemical oxygen demand removal rate of about 84% was obtained, and the degradation rate of 10 mg/L SMX was 61%. The degradation rate decreased with increasing antibiotic concentration, but the average degradation efficiency increased stepwise. Additionally, the relative abundance of resistant gene sul1 in the reactors of the new catalytic material was about 62% lower than that of sul1 in the control (Pt/C) reactors, and the relative abundance of sul2 was about 73% lower. Moreover, cost assessments related to the catalyst performance are presented. The findings of this study demonstrated that Ni-MOF-74 could be considered as a two-electron transfer ORR catalyst, and offers a promising technique for preparation of Ni–N–C for use as four-electron transfer ORR catalysts. In comparison, Ni-MOF-74 could be a promising ORR catalyst of MFCs for antibiotic degradation.
研究领域:
环境工程
·
生物化学
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催化
·
水处理
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产品关联
DOI
PubMed
高影响因子