SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Siqi Wang,Jia Wang,Lingzhi He,Fang Luo,Zhuwei Liao,Yi Wu,Zhuo Liu,Yu He,Zhuqi Chen
Complete remediation of organoarsenics from environmental matrix hits the bottleneck, that is, the sluggish efficiency of oxidative degradation towards organoarsenics and unsatisfying immobilization performance towards generated inorganic arsenic. Herein, we establish a biochar accelerated Fenton (BA-Fenton) process to decontaminate water from roxarsone (ROX). In comparison with Fe 2+ /H 2 O 2 process (10 μΜ/0.2 mM), the incorporation of 0.5 g L -1 biochar promoted ROX degradation from 48.2% to 98.2% and total arsenic elimination from 67.6% to 97.3%, respectively. In BA-Fenton process, •OH as the dominant reactive oxygen species (ROS), exhibited a cumulative concentration of 0.42 mM, three times higher than that in classical Fenton process. Crucially, the presence of biochar in Fenton process significantly enhanced the stability of arsenic-iron sludge, whereas the secondary leaching of total arsenic decreased from 433.8 μg-As L -1 to 13.9 μg-As L -1 , meeting the prescribed environmental quality standards for surface water in China (50 μg-As L -1 , GB 3838-2002). Mechanistic studies unveiled ROX remediation mechanism by BA-Fenton process, highlighting the dual functionality of biochar. On one hand, biochar efficiently reduced Fe 3+ to Fe 2+ with a rate constant of 0.225 min -1 , overcoming the rate-determining step of classical Fenton process for •OH production, consequently promoting the transformation of ROX to As(V). On the other hand, molecular spectroscopy analysis elucidated that in-situ formed As(V) was adsorbed by ferric hydroxides with the formation of arsenic-iron sludge. Subsequently, biochar immobilized arsenic-iron sludge through hydrogen bonds, electrostatic attraction and surface complexation. Furthermore, real water studies demonstrated the effective remediation of organoarsenics by BA-Fenton process in tap water, lake water and chicken manure leachate. This “Two Birds with One Stone” strategy with low-cost, environmental-friendly and sustainable biochar holds great promise for the ultimate disposal of industrial wastewater containing organoarsenics.
研究领域:
环境科学
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污染控制
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水处理技术
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产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
·
IF 8.91
Mengke Li,Zhiguo He,Hui Zhong,Wei Sun,Mingqiang Ye,Yetao Tang
The contamination of organoarsenic is becoming increasingly prominent while SR-AOPs were confirmed to be valid for their remediation. This study has found that the novel metal/carbon catalyst (Fe/C–Mn) prepared by solid waste with hierarchical pores could simultaneously degrade roxarsone (ROX) and remove As(V). A total of 95.6% of ROX (20 mg/L) could be removed at the concentration of 1.0 g/L of catalyst and 0.4 g/L of oxidant in the Fe/C–Mn/PMS system within 90 min. The scavenging experiment and electrochemical test revealed that both single-electron and two-electron pathways contributed to the ROX decomposition. Spectroscopic analysis suggested the ROX has been successfully mineralized while As(V) was fixed with the surface Fe and Mn. Density functional theory (DFT) calculation and chromatographic analysis indicated that the As7, N8, O9 and O10 sites of ROX molecule were vulnerable to being attacked by nucleophilic, electrophilic and radical, resulting in the formation of several intermediates such as phenolic compounds . Additionally, the low metal leaching concentration during recycling and high anti-interference ability in various water matrices manifested the practicability of Fe/C–Mn/PMS system.
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
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yi Zhou,Jie He,Xia Li,Jian Lu,Yanbo Zhou
High-risk roxarsone (ROX) can be converted to highly toxic arsenite (As(III)) through biological and abiotic processes, which can cause severe arsenic contamination of water and crops. Traditional oxidation processes can only treat organic arsenic compounds instead of releasing inorganic arsenic (iAs). Herein, an Fe(II)/resorcinol formaldehyde resin (RF) solar light-driven in-situ Fenton system was applied to remove ROX and its released iAs. Under solar light illumination, RF can reduce oxygen to produce H 2 O 2 through a two-electron reduction pathway. Fe(II) simultaneously catalyzed the decomposition of H 2 O 2 to generate ·OH, participating in the oxidation of ROX. The C-As bond of ROX was preferentially attacked by ·OH to form 2-nitrohydroquinone and As(III). Moreover, As(III) was further converted to low-toxicity arsenate (As(V)) through further oxidation with oxygen bubbling. Finally, the released As(III) (1.9%) and As(V) (98.1%) were removed by adsorption onto the surface of ferric hydroxide. As a result, more than 99.9% of ROX was degraded by the Fe(II)/RF in-situ Fenton system during the pre-oxidation process. The total organic carbon (TOC) removal efficiency of ROX and total arsenic removal efficiency of the Fe(II)/RF-O 2 in-situ Fenton system reached 75% and more than 97%, respectively. Furthermore, the residual arsenic in this Fenton system was less than 12.5 µg/L, which met the recommended limit for arsenic (100 µg/L) in reclaimed water. In addition to the removal of ROX, the Fe(II)/RF in-situ Fenton system showed excellent general applicability in the removal of emerging organic contaminants (EOCs). The TOC removal rate of EOCs was approximately 50%–64%. Thus, the Fe(II)/RF-O 2 solar light-driven in-situ Fenton system provides a novel strategy for the high-efficiency removal of organoarsenic compounds and EOCs.
研究领域:
环境科学
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化学
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水处理工程
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产品关联
DOI
高影响因子
VACUUM
·
2025
·
IF 3.9
Xingyuan Zhong,Riming Luo,Binbin Tan,Huidi Zhang,Jiang Wang,Jing Wang,Yao Deng,Guoen Yang,Ting Yang,Wenlei Wang
Despite potential of layered double hydroxides (LDHs) in photocatalytic wastewater treatment was demonstrated, their practical applications remain constrained by inherent limitations including sluggish charge separation kinetics and insufficient stability. To overcome these critical challenges, we engineered a boron-doped porous lignin carbon loaded with copper-iron layered double hydroxides (B-PLC/CuFe LDH) photocatalyst through hydrothermal synthesis. The dual-modification strategy overcomes inherent limitations of conventional LDH systems through boron-induced electronic coupling and interfacial engineering. Boron doping modulates the electronic structure of the porous lignin carbon (PLC), strengthening interfacial interactions with CuFe LDH layers, while the hierarchical carbon framework enhances LDH dispersion and charge transfer efficiency. Systematic characterization (UV-DRS, Mott-Schottky) revealed that boron doping synergistically widened the composite's bandgap from 1.54 eV (pristine PLC) to 1.83 eV (B-PLC-3/CuFe LDH), while maintaining strong visible-light harvesting. According to Electrochemical impedance spectroscopy (EIS), boron doping reduced electrochemical impedance, and increased photogenerated radical formation (·O 2 - and ·OH), collectively enabling efficient arsenic pollutant degradation. The optimized B-PLC-3/CuFe LDH achieved 84.7% roxarsone (ROX) degradation within 60 min under visible light, outperforming pristine PLC by 2.05 times. This work establishes a new paradigm for overcoming LDH's intrinsic limitations through defect-engineered carbon hybridization, opening avenues for sustainable heavy metal remediation.
研究领域:
环境化学
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材料科学
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光催化
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环境污染治理
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纳米复合材料
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可持续修复技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wenlin Liu,Chengxiong Dang,Weiquan Cai
Roxarsone (ROX) as a phenylarsenic feed additive, causes markedly threats to human health and water environment, and the key to treat it by adsorption method is to develop green large-scale preparation method of low-cost and efficient adsorbent. Herein, boehmite microspheres with superior ROX removal performance were efficiently synthesized on a large scale via a microwave-assisted green liquid phase precipitation (MP) method by regulating the carbon chain length of carboxylate ester precipitants. Especially, the ethyl acetate (EA) with short chain length results in hierarchical boehmite hollow microspheres (S-MP-EA) composed of three levels including crystalline grain at the nanoscale, hierarchical mesoscale packing of the nanoflakes centering around 3.8 nm and 10.5 nm, assembly of a self-supporting hollow microspheres driven by ionic conduction heating of microwave. Its fixed-bed dynamic adsorption for ROX with an initial concentration of 200 mg·L −1 showed that 5 g powder maintained its complete removal for the first 51 h, while the 10 g granulated adsorbent with diameters of 4.0 ± 0.1 mm achieved removal efficiency more than 90 % over 121 h suggesting its superior adsorption capability and long-term stability. Its synergistic adsorption mechanisms involving hydrogen bonding, electrostatic attraction and pore filling were significantly enhanced by microwave-enhanced hydroxyl density, positively charged distribution, hierarchical hollow structure and mesoporous structure. Combined with aluminum utilization efficiency of 95.50 % under precipitation conditions at 60 °C for only 30 min with environmental-friendly and easily obtainable raw materials, our work provides alternative functional aluminas with engineering applicability for highly efficient adsorption of organic arsenic wastewater.
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DOI
高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Qian-He Liu,Li Yuan,Zheng-Hao Li,Kenneth Mei Yee Leung,Guo-Ping Sheng
Agricultural wastewater, a significant component of the anthropogenic water cycle, often contains complex mixtures of contaminants, including non-antibiotic feed additives, posing largely uncharacterized risks for antimicrobial resistance (AMR) evolution. This study addresses the critical knowledge gap regarding the combined impact of commonly co-occurring roxarsone (ROX) and heavy metals (Zn, Cu) at environmentally relevant concentrations on the de novo evolution and persistence of multidrug resistance in aquatic environments. Using a 90-day laboratory evolution experiment with Escherichia coli , we demonstrate that while ROX alone induced moderate resistance (e.g., 6.2-fold increase in minimum inhibitory concentration (MIC) for chloramphenicol), co-exposure with Zn and Cu synergistically drove multidrug tolerance to nine antibiotics and selected for stable, heritable resistance to chloramphenicol, tetracycline, and kanamycin (up to 8.2-fold MIC increase). This robust resistance persisted even after pollutant removal, highlighting a significant long-term threat to water quality and public health via the dissemination of resilient AMR bacteria from agricultural sources. Co-exposure intensified oxidative stress-induced mutagenesis and selected for key adaptive strategies enhancing bacterial survival and AMR persistence in contaminated water. These include upregulated efflux pumps, increased secretion of extracellular polymeric substances (1.1-3.2-fold), enhanced motility (1.1-1.5-fold), and cell filamentation (lengths 2.4-8.2-fold greater). These findings illuminate a potent, previously underestimated environmental pathway where mixtures of common agricultural pollutants in wastewater synergistically select for persistent multidrug resistance. This research underscores the urgent need to revise water quality criteria and wastewater treatment paradigms to address the co-selection pressures exerted by non-antibiotic chemical mixtures in aquatic ecosystems.
研究领域:
环境微生物学
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抗生素耐药性
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水环境污染
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分子生态毒理学
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细菌进化
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环境健康
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DOI
PubMed
高影响因子
FOOD CHEMISTRY
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2024
·
IF 8.5
Xia Niu,Wen-Yuan Pei,Jian-Fang Ma
Herein, a novel FeCoNi(b)-800 ternary metal nanoalloy was uniformly mixed with reduced graphene oxide (RGO) to synthesize the FeCoNi(b)-800@RGO(2:1) composite. The addition of RGO not only stopped the accumulation of FeCoNi(b)-800 alloy, but also heightened the electrocatalytic activity of composite. Particularly, the FeCoNi(b)-800@RGO(2:1) composite displayed the significantly strong electrocatalytic capacity for the reduction of roxarsone (ROX). Furthermore, the FeCoNi(b)-800@RGO(2:1) composite possessed enough porosity and metal catalytic sites, facilitating the transport and electrochemical reduction of the ROX. Thus, the FeCoNi(b)-800@RGO(2:1) composite modified glassy carbon electrode (FeCoNi(b)-800@RGO(2:1)/GCE) showed the superb electrochemical detection effect for ROX with relatively wide working range (0.1–1500 μM) and low detection limit (0.013 μM). Importantly, the FeCoNi(b)-800@RGO(2:1)/GCE sensor could accurately determine the contents of ROX in actual pork, chicken, duck and egg samples, indicating that it had good suitability in food safety monitoring.
研究领域:
材料科学
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分析化学
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食品安全
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Xia Li,Jie He,Jian Lu,Yi Zhou,Yanbo Zhou
Fenton technology performs well in high-risk roxarsone (ROX) removal, but it is limited by the high H 2 O 2 transportation and storage risks. Herein, FeS 2 decorated resorcinol-formaldehyde resins (FeS 2 -RFR) were successfully prepared to in-situ produce and utilize H 2 O 2 for efficient removal of ROX. Under solar light illumination, resorcinol-formaldehyde resins (RFR) efficiently generated a high concentration of H 2 O 2 , with a yield of 500 μmol g −1 h −1 . FeS 2 can in-situ decompose H 2 O 2 to generate · OH, participating in the oxidation of ROX. As a result, the FeS 2 -RFR catalyst degraded more than 97% of ROX within 2 h and ROX was selectively degraded into low-toxic As(V), which can be simply removed by traditional adsorption or precipitation processes. During the degradation of ROX, · OH played a dominant role. Moreover, the cations (Na + , K + , and Ca 2+ ), anions (SO 4 2− , Cl − ), and humic acid had no noticeable inhibition effect on ROX removal. Furthermore, FeS 2 -RFR can still remove 70% of ROX even after three cycles, proving that this in-situ photo-Fenton system exhibited stability. This study innovatively proposed a double-active site FeS 2 -RFR photocatalyst for in-situ production and activation of H 2 O 2 and showed a sustainable and eco-friendly way for organoarsenic compounds degradation.
研究领域:
环境科学
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化学工程
·
材料科学
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DOI
高影响因子
ChemPlusChem
·
2023
·Vol. 88
·期 4
·e202300061
·
IF 3.4
Zhecheng Kang,Qian Zhou,Kun Wang,An Wang,Tianyi Chen,Hongbo Wei,Tengjiao Wang
Graphical An anti-infection nanocomposite was constructed by loading bactericide Roxarsone onto nitrosylated mesoporous polydopamine. The designed nanocomposite achieves NO-enhanced chemo-photothermal antibacterial therapy under near-infrared laser irradiation, and in vitro antibacterial evaluation has confirmed the effective elimination against the Gram-negative tetracycline-resistant Escherichia coil and Gram-positive methicillin-resistant Staphylococcus aureus of the nanocomposite. Current treatments for infections caused by multidrug-resistant bacteria still remain challenging and therapeutic materials with high efficacy are of demand. Herein, a bactericidal nanocomposite was constructed by loading Roxarsone (ROX) onto nitrosylated mesoporous polydopamine (named mPDA@NO-ROX). The designed nanocomposite exhibited considerable photothermal effect and controlled NO and ROX co-delivery under the irradiation of near-infrared laser (NIR) to achieve enhanced chemo-photothermal antibacterial therapy. The in vitro antibacterial evaluation of the mPDA@NO-ROX demonstrated the effective elimination of the Gram-negative tetracycline-resistant Escherichia coil and Gram-positive methicillin-resistant Staphylococcus aureus under mild NIR irradiation compared to merely ROX loaded unmodified mPDA, indicating the NO enhanced chemo-photothermal therapy. In addition, the cytotoxicity experiments indicated that mPDA@NO-ROX exhibited only 5 % of hemolysis rate and high cell viability at 1 mg mL −1 against mammalian fibroblasts, suggesting the excellent biocompatibility. In conclusion, the mPDA@NO-ROX could be a promising candidate for anti-infection therapy of multidrug-resistant bacteria.
研究领域:
医学
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生物材料学
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感染病学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Pin Peng,Xinyu Yan,Lixiang Chen,Xiang Li,Huiying Yang,Yijing Miao,Feng Zhao
Livestock wastewater is characterized by high concentrations of organic matter and diverse antibiotics. A major challenge in its anaerobic treatment is the effective degradation and thorough removal of coexisting antibiotic contaminants. In this study, an external voltage was applied to establish an electroactive biofilm, thereby enhancing the co-metabolic degradation of sulfamethoxazole and roxarsone. Application of +0.6 V (Ag/AgCl) increased the 72 h TOC removal efficiency to 52.1 %. At the same time, sulfamethoxazole and roxarsone removal efficiencies reached 90.8 % and 100 %, respectively. The results from liquid chromatography-mass spectrometry (HPLC-MS/MS) and density functional theory calculations revealed sulfamethoxazole degradation pathways: N–O bond cleavage and hydroxylation. Roxarsone degradation primarily involved nitro group reduction and C–As bond cleavage. The pharmacophore of sulfamethoxazole was effectively removed, and inorganic arsenic from roxarsone degradation was efficiently immobilized. Toxicity analysis confirmed that the electroactive biofilm notably reduced toxic intermediate accumulation. Elevated concentrations of NADH and ATP in the electroactive biofilm indicated enhanced microbial substrate metabolism and generation of more electron donors. The higher absolute abundance of the sulfamethoxazole degradation gene ( SadABC ) in the electroactive biofilm indicated that sulfamethoxazole degrading enzyme (sadABC) gained more electrons. Microbiome analysis revealed the upregulation of genes linked to extracellular electron transfer, the tricarboxylic acid (TCA) cycle, nitro-reduction, and sulfate reduction pathway, confirming the electroactive biofilm enhances substrate metabolism and co-metabolic antibiotic degradation. Electroactive biofilm offers a viable strategy for antibiotic removal in livestock wastewater.
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yao Jia Peng,Cheng Feng,Min Lin,Ge Lin Liu,Yan Su,Hao Zhe Hou,Jian Ping Wang
Roxarsone and arsanilic acid are all organoarsenic compounds, and they are usually used as feed additives. However, their residues in foods of animal origin and their metabolites distributing into the environment are the public concerns. The inspection of their appearances in animal feeds can avoid the above problems. In this study, a type of magnetic molecularly imprinted microsphere was synthesized that was combined with a carbon-dots labeled fluorescent tracer to develop a semi-homogeneous fluorescence method for determination of the two drugs in animal feeds. Results showed this method contained only one step (sample-loading), the limits of detection for roxarsone and arsanilic acid were 0.02 and 0.12 mg/kg respectively, and the magnetic microsphere could be reused for 4 times. In addition, the method sensitivity when using carbon-dots labeled fluorescent tracer was higher than that when using fluorescein isothiocyanate labeled fluorescent tracer. This method exhibited better performances than the previous immunoassays and molecularly imprinted polymer-based method for determination of the two analytes. So this method could be used as a simple tool for screening of roxarsone and arsanilic acid in animal feeds.
研究领域:
分析化学
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环境科学
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食品科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2017
·Vol. 24
·期 19
·16429-16439
·
IF 2.741
Yao Lixian,Huang Lianxi,Bai Cuihua,He Zhaohuan,Zhou Changmin
Roxarsone (ROX), a widely used feed organoarsenic additive, occurs as itself and its metabolites in animal manure that is commonly land used as fertilizer. Soil property impacts arsenic (As) speciation and bioavailability. Fourteen soils across China were used to conduct culture experiments to investigate As uptake by garland chrysanthemum ( ChrysanthemumL coronarium ), with the soils fertilized with chicken manure bearing ROX and its metabolites. The results show As(III) was the sole As form in garland chrysanthemum shoots, and As(III) and As(V) occurred in roots. Only inorganic As was detected in all soils when the plants were harvested. Stepwise regression analysis shows soil-exchangeable Ca predominated shoot As(III) concentration (shoot As(III) = 1.60030 soil Ca, R
2 = 0.8832***). Therefore, ROX is transferred into the human food chain finally as inorganic As in plants. Application of animal manure bearing ROX and its metabolites is not recommended in Ca-rich soils to avoid excess inorganic As dietary exposure.
研究领域:
环境科学
·
农学
·
土壤化学
·
植物生理学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）