INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Wenlan Ji,Yuan Wang,Tian Cheng Zhang,Like Ouyang,Shaojun Yuan
Addressing the ever-growing arsenite pollution in groundwater has become an essential and urgent issue for ensuring the safety of human beings and the environment. It is highly attractive to preoxidize As(III) to relatively low toxic As(V) for further efficient arsenic removal by adsorption, ion exchange, or coagulation. In this study, a novel heterostructure Cu2O@TiO2 nanotube array coated titanium anode (CTNTA) was fabricated by combination of electrochemical anodization and electrodeposition and used for the highly efficient photoelectrocatalytic oxidation conversion of As(III) to As(V) in aqueous solution. The morphology, composition, and photoelectric performances of the CTNTA anode were systematically characterized. The effect of the loading amount of Cu2O nanoparticles on the photoelectrocatalytic oxidation kinetics of As(III) was investigated, and the comparison study among photocatalytic, electrocatalytic, and photoelectrocatalytic oxidations of As(III) was also explored to demonstrate the synergistic effect of As(III) oxidation conversion performance. The heterostructure CTNTAs-1.00 delivered a substantially enhanced photoelectrocatalytic oxidation ratio of As(III) at 95% within 30 min at a current density of 10 mA·cm–2 under visible-light irradiation. The electrochemical deposition amount of Cu2O nanoparticles on TiO2 nanotube arrays (TNTAs) was found to be positively correlated with the achievement of boosted As(III) oxidation efficiency. The high photoelectrocatalytic oxidation performance of the CTNTA was ascribed to the favored separation efficiency of photoinduced carriers and electron–hole pairs under both visible light irradiation and electric potential conditions. The photoelectrocatalytic oxidation reaction mechanism was proven to be ascribed to the active species of holes (h+), superoxide radicals (•O2–), and hydroxyl radicals (•OH). These results highlight the high conversion rate of As(III) by the photoelectrocatalytic oxidation reaction on such a nanostructured anode, which offers a promising methodology for further in-depth oxidation of As(III) in aqueous solution.
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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水处理
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DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Zhongxin Zhuang,Jiawei Xu,Yan Chen,Zheng Guo,Zhonggang Liu,Xingjiu Huang
The highly toxic arsenite (As(III)) could cause serious cytotoxicity on metabolism, resulting in several diseases. However, it is still a great challenge on the precise sensing of As(III) in complicated conditions, especially in cellular environment. In this work, a nanoporous gold microelectrode (NPG-μE) was fabricated by a simple electrochemical alloying/dealloying method and developed for the electroanalysis of As(III) in the lung cancer cellular (A549 cells) environment. The as-fabricated NPG-μE exhibited the excellent electrochemical performance towards As(III) detection at physiological pH (0.1 M PBS solution , pH 7.4) with a high sensitivity of 5.07 μA ppb −1 cm −2 and a low limit of detection of 0.25 ppb (S/N = 3). The large surface area derived from the nanoporous structure, and the well-dispersed active sites as well as the highly electro-catalytic activity of gold played a critical role on the improved electrochemical behaviors. Furthermore, the effect of the exposure time on electrochemical monitoring As(III) in A549 cellular environment was successfully investigated, revealing the fatal impact of As(III) on cell cycle. This work offered a great trial on investigating of the cytotoxicity of arsenite and their precise detection in complicated cellular environment.
研究领域:
分析化学
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电化学
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毒理学
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生物医学工程
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细胞生物学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Huimin Hu,Qiwu Zhang,Chao Wang,Min Chen,Mengfei Chen
Iron manganese oxide resources are widely derived from the geological structure , and their combinations play an important role in the migration and transformation of arsenic. Iron oxide and manganese oxide exist generally in a mixed state in Fe-Mn oxides synthesized via the well studied co-precipitation methods using potassium permanganate and manganese/iron sulfates. Herein, a newly designed Fe-Mn-O compositing oxide with Fe-MnO 2 , Mn-Fe 2 O 3 , (Fe 0.67 Mn 0.33 )OOH solid solution and FeOOH as the main components, simply through solvent-free mechanical ball milling pyrolusite (MnO 2 ) and ferrihydrite (FeOOH) together has been reported. Atomic-scale integrations by doping Fe and Mn with each other were detected and an adsorption-oxidation bifunctionality was achieved, where Fe-doped MnO 2 served as oxidizer for As(III) and amorphous/ground FeOOH acted as adsorbent first for As(III) and then As(V) from the oxidization. The maximal adsorption for As(III) could reach 44.99 mg/g and over 82.5% of As(III) was converted to As(V). More importantly, high removal ability of arsenic worked in a wide pH range of 2–10.5%, and 87.2% of its initial adsorption-oxidation capacity could be kept even after 5-cycles reuse for treating 20 mg/L As(III) with a dosage at 1 g/L. Together with the enhanced adsorption capacity by the milled FeOOH, surface electron transfer efficiency of the developed Fe-MnO 2 surrounded with Mn-Fe 2 O 3 has been studied for the first time to understand the oxidization effect to As(V). Besides the environment-friendliness of ball milling method, the prepared sample is quite stable without noticeable metal release into solution. Mechanism studies of arsenic removal by the as-prepared Fe-Mn-O oxide provide a new direction for improving the oxidation efficiency of MnO 2 to As(III) based on the widely available cheap Mn and Fe oxides, contributing to the development of advanced oxidization process in the treatment of waste water.
研究领域:
环境科学
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材料科学
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水处理
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DOI
PubMed
高影响因子
RSC Advances
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2015
·Vol. 5
·期 83
·67951-67961
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IF 3.84
Jin Zhu,Zimo Lou,Yu Liu,Ruiqi Fu,Shams Ali Baig,Xinhua Xu
Iron–manganese binary oxide (FeMnOx) is considered highly effective for arsenic adsorption, however, the agglomeration effect hindered its practical application. In this study, graphene has been used as a supporting matrix to disperse FeMnOx due to its huge specific surface area, and the synthesized novel composite adsorbent (FeMnOx/RGO) was employed for arsenic removal. Results demonstrated that FeMnOx/RGO (mass ratio of FeMnOx to FeMnOx/RGO nanocomposites is 45%) has larger specific surface area (411 m2 g−1) in comparison with bare FeMnOx, and showed 10.16 mg As g−1 FeMnOx and 11.49 mg As g−1 FeMnOx adsorption capacities for As(III) and As(V), respectively, with 1 mg L−1 initial concentration. Increased in the initial concentration to 7 mg L−1, the adsorption capacities of As(III) and As(V) reached to 47.05 mg As g−1 FeMnOx and 49.01 mg As g−1 FeMnOx, respectively. The removal process perfectly obeys pseudo second-order kinetic model for both As(III) and As(V). And PO43− was found to strongly inhibit arsenic adsorption. Furthermore, adsorption tests and characterization analyses confirmed that MnO2 played a key role on the oxidation of As(III), while iron(III) oxide was found crucial to As(V) removal. Electrostatic interaction and surface complexation mechanisms involved in the adsorption. These findings suggested that the adsorbent could be used in real arsenic-contaminated water treatment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Wenlan Ji,Yuan Wang,Yuanjie Xiong,Tian C. Zhang,Shaojun Yuan
To strengthen the utilization of free radicals and effectively enhance electrocatalytic performance and service lifetime of the β -PbO 2 electrode, herein, a novel hydrophobic TNAs/SnO 2 /PPy/ β -PbO 2 -Ce-SDS (abbreviated as β -PbO 2 -Ce-SDS) anode was synthesized by doping Ce 3+ and anionic surfactant (SDS) to TNAs/SnO 2 /PPy/ β -PbO 2 (abbreviated as β -PbO 2 ), which was constructed by growing SnO 2 /PPy/ β -PbO 2 multilayers on TiO 2 nanotube arrays (TNAs) via combination of electrodeposition and electro-polymerization processes. Notably, co-modification with Ce 3+ and SDS remarkably enhanced the surface hydrophobicity, electrochemical performance and catalytic ability of β -PbO 2 anode. Such β -PbO 2 -Ce-SDS anode not only substantially enhanced the As(III) conversion (96.96%) in the electrocatalytic oxidation process, but also prominently strengthened its service lifetime. Furthermore, the as-prepared β -PbO 2 -Ce-SDS anode possessed an excellent stability as its kinetic constant was only reduced from 0.18 to 0.14 min −1 even underwent 10 cycles of the electrocatalytic process, while that of the unmodified β -PbO 2 electrode decreased markedly by about 49%, owing to its appropriate surface hydrophobicity, smaller grains and denser β -PbO 2 layer. The reaction mechanism of electrocatalytic oxidation was associated with synergistic effects of hydroxyl radical ( OH), superoxide radicals ( O 2 − ), and sulfuric acid root radicals ( SO 4 − ). The β -PbO 2 -Ce-SDS anode provides a novel and feasible approach to development of various electrodes by doping metal ions and/or regulating with surfactants.
研究领域:
电化学
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Yiqun Liu,Zhihao Chen,Xiaoshuang Yin,Yun Chen,Ying Liu,Wenzhong Yang
Arsenic pollution in natural water is a worldwide problem. In this work, a resin-based hydrated iron oxide (D303-HFO) adsorbent was designed to remove arsenate (As(V)) and arsenite (As(III)) in the groundwater. The structure and morphology of the D303-HFO adsorbent were characterized by FTIR, XRD , SEM and TEM tests. The specific surface area, pore volume and pore size increased with the incorporation of HFO nanoparticles in the resin. In addition, the effects of pH and coexisting ions on the arsenic removal efficiency were investigated. Results indicated that the D303-HFO had efficient removal performance for arsenic in the pH range of 3–9 and showed high selectivity for As(V) and As(III) under the influence of competitive ions. The adsorption kinetics study confirmed that the adsorption process was dominated by chemisorption , and the adsorption isotherms of As(V) and As(III) by D303-HFO fitted the Langmuir model. Thermodynamic parameters indicated that the adsorption reaction was spontaneous and exothermic. Moreover, the regeneration and stability experiment indicated that the D303-HFO adsorbent was super reusable after five consecutive cycles and could be put into service stably and permanently. The fixed-bed column test showed that the water sample containing As(V) and As(III) was treated with a volume of 900BV and 1100BV, respectively. After the treatment, the effluent concentration reached the drinking water standard stipulated by WHO.
研究领域:
环境科学
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水处理
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材料科学
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产品关联
DOI
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2018
·
IF 3.974
Bin Li,Bowen Gu,Zhaoguang Yang,Ting Zhang
Arsenic contamination of water is a global concern due to its heavy threat to human health. In this study, the submerged macrophyte Vallisneria natans (Lour.) Hara was used to remove environmentally relevant concentrations of arsenic in the binary As(III)/As(V) system. The concentrations of total arsenic (tAs) and As(III) in water dropped rapidly within 3 days, while As(V) first increased slightly within 3 days and then gradually decreased. About 1.2% dimethylarsinate (DMA) was detected at the 14th day of treatment. These findings indicated that As(III) could be oxidized to As(V) and methylated to DMA in water with V. natans . In relation to V. natans , both tAs and As(V) were much higher in roots compared to leaves. Arsenate was the predominant species (≥ 95.65 ± 0.10%) in roots, and As(III) was only found at the 14th day (3.45–6.96 mg kg –1 ). In leaves, As(III) significantly increased ( P < 0.05) as the treatment duration increased. The proportions of As(V) (27.99–40.03%) were lower than those of As(III) and arsenobetaine (AsB) was detected (0.52–1.87 mg kg –1 ) after 7 d. The results of arsenic speciation demonstrated that the transformation of arsenic species in V. natans included As(V) reduction and As(III) methylation to AsB. There were a decrease in chlorophyll content, and an increase in MDA level and antioxidant enzymes (SOD, CAT , and POD) activities. The MDA level was much higher in leaves than roots, whereas the activities of SOD, CAT, and POD were the opposite, suggesting their possible role in arsenic resistance and detoxification. Our results indicate the potential of V. natans in phytoremediation of arsenic-contaminated water.
研究领域:
环境科学
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植物修复
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水生生态学
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毒理学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Xiaoying Jin,Lu Yang,Heng Li,Zhiqiang Chen,Zuliang Chen
Despite the oxidation mechanism of antimonite (Sb(Ⅲ)) by biosynthesized iron nanoparticles (Fe NPs) has been reported, the impact of coexisting components in acid mine drainage (AMD) on the Sb(III) oxidation by Fe NPs is unknown. Herein, how the coexisting components in AMD affect Sb(Ⅲ) oxidation by Fe NPs was investigated. Firstly, Fe NPs achieved complete oxidation of Sb(Ⅲ) (100%), while only 65.0% of Sb(Ⅲ) was oxidized when As(Ⅲ) was added, due to competitive oxidation between As(Ⅲ) and Sb(Ⅲ), which was verified by characterization analysis. Secondly, the decline in solution pH improved Sb(Ⅲ) oxidation from 69.5% (pH 4) to 100% (pH 2), which could be attributed to the rise of Fe 3+ in solution promoting the electron transfer between Sb(Ⅲ) and Fe NPs. Thirdly, the oxidation efficiencies of Sb(Ⅲ) fell by 14.9 and 44.2% following the addition of oxalic and citric acid , respectively, resulting from the fact that these two acids reduced the redox potential of Fe NPs, thereby inhibiting Sb(Ⅲ) oxidation by Fe NPs. Finally, the interference effect of coexisting ions was studied, where PO 4 3− significantly reduced Sb(Ⅲ) oxidation efficiency due to the occupation of the surface-active sites on Fe NPs. Overall, this study has significant implications for the prevention of Sb contamination in AMD.
研究领域:
环境化学
·
纳米技术
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水处理
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产品关联
DOI
PubMed
高影响因子
ACS ES&T Water
·
2023
·
IF 5.3
Hongcen Zheng,Bingdang Wu,Guoyang Zhang,Tianyu Xie,Zhihao Chen,Shujuan Zhang
Redox transformation is a useful strategy to reduce the toxicity of metal oxysalts and to facilitate their removal from water. The synergy of the oxidation and reduction processes in a single system is of great value for the treatment of wastewater containing multiple pollutants. Here, by taking As(III) and Cr(VI) as modeling pollutants, the synergic effect in redox transformation of coexisting oxyanions was evaluated with a typical advanced oxidation process (AOP)─UV/H2O2, a well-established advanced reduction process (ARP)─UV/sulfite, and a newly developed UV/acetylacetone (AcAc) process. At near-neutral pH and low [AcAc]/[oxyanion] stoichiometric ratios (2.5–10:1), UV/AcAc could effectively fulfill As(III) oxidation and Cr(VI) reduction in a single process without any other treatment. More importantly, the electric energy consumption of UV/AcAc per mole of As(III) and Cr(VI) was only 1/7 of the sum of UV/H2O2 and UV/sulfite. We thus propose that UV/AcAc is an advanced oxidation and reduction process (AORP). Owing to the existence of long-lived radicals and multiple pathways, this AORP process showed an obvious synergic effect in redox transformation and was robust in the complex water matrix.
研究领域:
环境科学
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化学工程
·
水处理
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DOI
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Qimei Hu,Li Li,Jie Li,Xin Sun,Congqi Yan,Minlin Mao,Zhang Lin,Weizhen Liu
The arsenic sulfide sludge (ASS) generated from the treatment of acidic arsenic-containing wastewater by sulfide precipitation causes severe environmental pollution due to its potential to release highly toxic As(III). This work describes an alkaline-oxidative hydrothermal method that converted ASS to the highly stable johnbaumite mineral (Ca5(AsO4)3(OH)) in which arsenic exists as the less toxic As(V). Under the optimal reaction conditions, i.e., with H2O2 (ω = 3.3 wt %) and Ca(OH)2 (mCH/mASS = 1:1) at pH = 14.18 and 180 °C for 18 h, the arsenic leaching was reduced from 762.85 mg/L for the original ASS down to 0.04 mg/L for the hydrothermally treated product, far below the 1.2 mg/L limit set in the Chinese standard GB 18598-2019. The stabilization of arsenic mainly involved three steps: (i) As(III) in ASS was released into the alkaline solution and oxidized to AsO43–, (ii) the free AsO43– was captured by Ca2+ to form the Ca3(AsO4)2 and Ca5(AsO4)3(OH), (iii) the intermediate Ca3(AsO4)2 was further converted to johnbaumite under hydrothermal condition, and eventually AsO43– was stably encapsulated in the johnbaumite lattice. This study thus provided an effective strategy for the treatment and safe disposal of ASS and revealed the mechanisms underlying arsenic stabilization via johnbaumite.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yuxin Li,Zhimin Wang,Yuanfeng Wei,Ting Wang,Maosong Zhao,Jie Luo,Jun Zhou,Zhaoshuang Li,Kai Yin,Chengbin Liu
Water decontamination from arsenic-contaminated groundwater is critical to the health of millions of households worldwide. However, efficiently removing the low-adsorbing As(III) remains challenging. Herein, a multifunctional biocomposite bead UiO-66-NH 2 -Cl@PCB integrating defects, oxidation and adsorption properties was prepared to effectively remove As(III). The N -chlorosulfonamide bound within the embedded UiO-66-NH 2 -Cl oxidizes the lower-adsorbing As(III) to As(V), which could be effectively adsorbed by the defect-rich MOF, while the porous chitosan bead (PCB) host ensures the utilisation of the reactive sites of UiO-66-NH 2 -Cl. Using 1 g/L of UiO-66-NH 2 -Cl@PCB, 1 mg/L of As(III) can be reduced to under 10 μg/L in 300 min. Furthermore, similar As(III) removal efficiencies were achieved across a wide pH spectrum (3–9) or in the presence of interfering substances (anions, cations, organic matter). High concentrations of phosphate will inhibit its performance. As(III) removal followed the Freundlich isotherm modal, and its maximum removal capacity reached 58.09 mg/g at pH 7. Furthermore, at equilibrium concentrations of 10 μg/L, its As(III) removal capacity exceeded 10 mg/g. UiO-66-NH 2 -Cl@PCB can purify the As(III)-spiked groundwater to meet the drinking standard level. Using NaOH solution for regeneration, the removal efficiency maintained above 70 % in the fifth cycle. Additional chlorination treatment can significantly improve reusability. 2.4 g of UiO-66-NH 2 -Cl@PCB packed fixed-bed column was capable of purifying 3820 BV of groundwater containing 100 μg/L of As(III). The proposed UiO-66-NH 2 -Cl@PCB has the potential to be an easy-to-use and reliable material for efficient As(III) removal.
研究领域:
环境科学
·
材料科学
·
水处理技术
·
化学工程
·
吸附与催化
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产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2018
·
IF 4.358
Jian Zhang,Wei Li,Ying Li,Lixiang Zhou,Yeqing Lan
Schwertmannite (SCH) has strong adsorption ability to As(III). However, there are few reports on the stability of SCH load with As(III) (SCH-As(III)). In this study, the effects of tartaric acid (TA), pH and coexisting ions including K + , Ca 2+ , Al 3+ and CO 3 2− on the photoreductive dissolution of SCH- As(III) and the release of the adsorbed As (III) were investigated. The results showed that under UV irradiation TA could greatly enhance the release of total Fe and total As from SCH-As(III). Nevertheless, the total Fe and total As in the solution decreased when TA was consumed up. Compared to SCH, the reductive dissolution of SCH-As(III) was obviously suppressed. In the dark, TA could slowly enhance the dissolution of SCH-As(III), but its effect on the release of adsorbed As(III) was weak. Low pH was conducive to the release of iron and arsenic. Ca 2+ , K + , and CO 3 2− promoted the decrease of the dissolved total Fe in the later reaction. However, Al 3+ inhibited the decrease of the dissolved total Fe and total As. The analyses of FTIR and XRD demonstrated that the mineralogical phase of SCH-As(III) after reaction changed. With light, the dissolved total Fe and total As existed mainly as Fe(II) and As(V), respectively. This is because Fe(II) was generated via ligand to metal charge transfer and As(III) was oxidized to As(V) by ·OH produced during the reaction. Thus, this study provides us with a comprehensive understanding of the stability of SCH-As(III) and the release of adsorbed As(III) in natural environments.
研究领域:
环境科学
·
矿物学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）