APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Hongbo Lu,Chunli Wang,Xueming Liu,Jing Zhang,Zhang Lin,Zhengping Hao,Gang Pan
Arsenic sulfide sludge (ASS) is a typical precipitation product of acid smelting wastewater. Previous study reported that when exposed to sunlight, the release and oxidation of As(III) in ASS were markedly accelerated. However, the key factor to trigger the photocatalytic transformation of ASS is still unclear. Herein, we revealed that the coexisting Fe(II)/Fe(III) ions were critical to promote the photo-oxidation of released As(III) under visible light. We further validated that Fe(II)-stimulated photo-oxidation mechanism of As(III) in ASS was pH-dependent. In acid conditions, OH and SO 4 − were promoted by Fe(II)/Fe(III) cycling catalysis with the assistance of the reductive sulfur species from ASS, e.g. S 2− and SO 3 2− , and thus accelerated the oxidation of As(III). While in neutral conditions, the nascent ferric hydroxide colloids enhanced the oxidation rate of As(III) via photo-induced ligand-to-metal-charge transfer (LMCT) mechanism. These findings help in predicting and controlling the fate of real arsenic-containing sludge in sunlit environments.
研究领域:
环境科学
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化学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 11
·5206-5217
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IF 3.925
Yajie Wang,Xianhe Gong,Xin Dong,Xiuzhen Tao,Yingchun Luo
In this study, the kinetics of arsenite (As(III)) removal in a ferrihydrite/oxalate system under irradiation was investigated, and the effects of pH, ferrihydrite dosage, As(III) initial concentration, and oxalate concentration were evaluated. Ultraviolet A (UVA) irradiation significantly promoted As(III) removal in the presence of ferrihydrite and oxalate. The greatest removal efficiency of As(III) (92.5%) was observed under the following conditions: pH 3.0, 100.0 μg L−1 As(III), 0.0125 g L−1 ferrihydrite, 0.1 mmol L−1 oxalate, and after 90 min under UVA irradiation. The removal of As(III) in the ferrihydrite/oxalate system was strongly pH-dependent. Mechanistic investigations indicated that HO˙ was the primary oxidant for As(III) photo-oxidation in the ferrihydrite/oxalate system. Surface adsorbed hydroxyl radical (HOads˙) was the dominant oxidant over the entire pH range in the presence of oxalate, and the hydroxyl radical in aqueous solution (HOaq˙) made only a small contribution under acidic conditions. The sources of HO˙ were also strongly dependent on pH; HO2˙/O2˙− was the precursor of HO˙ under acidic conditions, while photo-generated holes gradually became the main source of HO˙ as the pH increased. The photo-oxidation of As(III) mainly occurred on the surface of ferrihydrite. Although some ferrihydrite transformed into goethite during the removal process, the iron oxides showed good reusability for up to five regeneration cycles. The findings indicate that As(III) can be efficiently removed by the ferrihydrite/oxalate system and provide guidance for developing effective treatment strategies for As(III)-contaminated waters.
研究领域:
环境科学
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化学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2025
·
IF 0
Qin Chuan,Jiao Yanni,Yang Luping,Wang Lin,Kong Zhengqiao,Jiang Dafeng,Zhang Jiacheng,Zhang Tianliang,Gao Xibao
Arsenic species were quantified to further explore the biotransformation of arsenic and better explain the potential health risks. In this research, the levels of six arsenic species (AsB, AsC, MMA, DMA, As 3+ , and As 5+ ) were determined in 160 squid samples by HPLC-ICP-MS. AsB was the most predominant speciation in squid tissues. The arsenic species, including AsB, AsC, and MMA, were found in all samples, followed by DMA (49.38%), As 3+ (21.25%), and As 5+ (2.5%). Results indicated squid samples from offshore had higher levels of AsB, AsC, MMA, and DMA. Pearson’s correlation analysis found correlations between As-MMA, DMA-As 5+ , and AsB-MMA, which showed a clear methylation pathway. The levels of inorganic arsenic were below the standard, and no potential health risks were identified. Therefore, the application of total arsenic in our previous study to assess health risks may be biased. In future, there is a need to optimize food safety monitoring of arsenic and comprehensively grasp the basic status and change law of marine ecological environment.
研究领域:
食品安全
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环境科学
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毒理学
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DOI
PubMed
JOURNAL OF MOLECULAR STRUCTURE
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2024
·
IF 4
Yue Yin,Yanming Xu,Ya-Nan Luan,Zhuo Zhao,Yihua Xiao,Changqing Liu
A novel porous Fe-Mn chitosan bead (PFMB) was fabricated through the freeze-drying technique for the enhanced oxidation and adsorption of arsenite (As(Ⅲ)) from aqueous solution. The porous internal structure of PFMB provided a significantly higher As(Ⅲ) oxidation and adsorption rate than solid Fe-Mn chitosan bead (FMB). The experimental results showed that FMB and PFMB exhibited the theoretical maximum As(Ⅲ) adsorption capacities of 27.42 and 49.80 mg/g, respectively. The real-time oxidation and adsorption progress of As(Ⅲ) onto PFMB was deeply evaluated: PFMB effectively oxidized As(Ⅲ) to As(Ⅴ) and the generated As(Ⅴ) was subsequently adsorbed. The operational parameters (initial pH, adsorbent dosage, ionic strength, and HA concentration) were thoroughly investigated and had no significant influence on As(Ⅲ) removal by PFMB. Finally, the regeneration experiment showed that PFMB can be easily regenerated and the recycled PFMB can successfully remove As(Ⅲ) in the following 5 cycles. Column experiments suggested that the column device could effectively remove the As(Ⅲ) in more than 3830 bed volume with the influent velocity at 0.5 mL/min before effluent concentration reached 0.05 mg/L. These results revealed the enhanced oxidation and adsorption performance of As(Ⅲ) onto PFMB and provided a reference for the future application of PFMB in 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
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Na Chen,Yichao Wan,Guangming Zhan,Xiaobing Wang,Meiqi Li,Lizhi Zhang
Solar light driven organoarsenicals degradation and simultaneous inorganic arsenic immobilization with naturally abundant hematite is very promising for organoarsenicals remediation, but suffers from the fast electron-hole charge recombination of hematite. Herein, we report that oxalate, widely existed in soil and water environments, can greatly enhance the photocatalytic molecular oxygen activation of hematite to degrade a typical organoarsenical roxarsone and immobilize the resulted inorganic arsenic. It was found that oxalate could chelate with surface Fe(III) of hematite to generate plenty of •OH via a surface Fe(III)/Fe(II) cycle mediated oxygen molecular activation process under a simulated solar light, and thus induced 85.1% of roxarsone transformation into inorganic arsenic species, mainly As(V), within 6 h. The generated As(V) could be further adsorbed on hematite surface with prolonging the reaction time to 24 h in dark, avoiding secondary pollution. More importantly, hematite was reusable for the simulated solar light driven roxarsone degradation and As(V) immobilization in the presence of oxalate. This study offers a green and effective strategy for organoarsenicals remediation, and also sheds light on the environmental effects of iron oxides and oxalate.
研究领域:
环境科学
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光化学
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DOI
高影响因子
ANALYTICA CHIMICA ACTA
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2012
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IF 4.555
Dongyue Li,Jing Li,Xiaofang Jia,Yanchao Han,Erkang Wang
A simple, rapid and sensitive sensing platform for the detection of As(III) has been fabricated in neutral media based on the mercaptoethylamine modified Au electrode. A wide detection range of 0.2–300 μg L −1 and a low detection limit of 0.02 μg L −1 were obtained with a preconcentration time of 100 s under optimal conditions. Compared with previous studies, this work shows obvious advantages that it not only suppresses the Cu(II) interference, but also can detect the As(III) in natural water samples at the original pH avoiding high concentration acidic media. Moreover, the practical application of the proposed method was verified in the lake water sample determination.
研究领域:
分析化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2020
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IF 6.785
Pei-Hua Li,Meng Yang,Yi-Xiang Li,Zong-Yin Song,Jin-Huai Liu,Chu-Hong Lin,Jie Zeng,Xing-Jiu Huang
Achieving highly sensitive and selective detection of trace-level As(III) and clarifying the underlying mechanism is still a intractable problem. The electroanalysis of As(III) relies on the electrocatalytic ability of the sensing interface. Herein, we first adopt single-atom catalysts as the electrocatalyst in As(III) detection. Cobalt single-atoms anchored on nitrogen-doped carbon material (Co SAC) were found to have an extraordinary sensitivity of 11.44 μA ppb–1 with excellent stability and repeatability, which so far is the highest among non-noble metal nanomaterials. Co SAC also exhibited a superior selectivity toward As(III) compared with some bivalent heavy metal ions (HMIs). Combining X-ray absorption spectroscopy (XAFS), density functional theory (DFT) calculation, and reaction kinetics simulation, we demonstrated that Co single atoms stabilized in N2C2 support serve as active sites to catalyze H3AsO3 reduction via the formation of Co–O hybridization bond, leading to a lower energy barrier, promoting the breakage of As–O bonds. Importantly, the first electron transfer is the rate-limiting step of arsenic reduction and is found to be more favorable on Co-SAC both thermodynamically and kinetically. This work not only expands the potential applicaiton of single-atom catalysts in the detection and treatment of As(III), but also provides atomic-level catalytic insights into HMIs sensing interfaces.
研究领域:
环境科学
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材料科学
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分析化学
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DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 4
·1185-1190
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IF 4.58
Gong Lingling,Du Bibai,Pan Long,Liu Qingju,Yang Kunhao,Wang Wei,Zhao Hong,Wu Li,He Yujian
The authors describe a colorimetric assay for the determination of As(III) in aqueous solution using citrate capped gold nanoparticles (AuNPs) which, in the presence of As(III), undergo aggregation due to the interaction of citrate ion with As(III). This results in an easily detectable color change from wine-red to blue. The ratio of the absorbances at 661 and 519 nm is linearly related to the As(III) concentration in the 4 to 100 ppb range, with a detection limit as low as 1.8 ppb (at 3σ) which is below the guideline value of 10 ppb. The method is rather simple in that it does not require the surface of the AuNPs to be modified. It was successfully applied to the determination of As(III) in spiked drinking water where it gave adequate recoveries.
The ratio of the absorbances at 661 and 519 nm is linearly related to the As(III) concentration in the 4 to 100 ppb range, with a detection limit as low as 1.8 ppb (at 3σ) which is below the guideline value of 10 ppb.
研究领域:
分析化学
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环境科学
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产品关联
DOI
高影响因子
APPLIED GEOCHEMISTRY
·
2022
·
IF 3.841
Peiwen Zhang,Shaofeng Wang,Danni Zhang,Yumeng Wang,Yu Song,Yongfeng Jia
Thioarsenic species are widely existed in transitional environments with varying redox potential such as hot springs and paddy fields , where arsenite , sulfide and thioarsenites may be exposed to ambient air. However, arsenic speciation, especially the kinetics of arsenic transformation in such scenarios are not well studied. Here we present results from both kinetic experiments and computational information on the formation mechanisms of thioarsenic species from the sulfide-driven oxidation of arsenite (13.3 μM) under air atmosphere at circumneutral pH (6.5–10.5, covering the usual groundwater pH range). Ion chromatography-hydride generation atomic fluorescence spectrometry (IC-HG-AFS) was used for the determination of non-thiolated arsenic and thioarsenate species as well as indirect identification of thioarsenites at environmentally relevant As concentration. Results showed that the ambient air facilitated the thiolation and oxidation of arsenite, during which thioarsenites were served as intermediates. It was supported by our ab initio DFT calculation showing that the activity towards oxidation was in the order of: monothioarsenite > dithioarsenite > trithioarsenite > arsenite. The thiolation of arsenite was decreased with pH with a rate constant of 0.2–1.7 h −1 ; while the oxidation of thioarsenites by air was increased with pH with a rate constant of 0.1–0.45 h −1 . The results of this study shall improve our mechanistic understanding on the formation of thioarsenic, and shed light on the potential intermediate roles played by thioarsenites in environments with varying redox potential or intermittent anoxia, such as paddy fields, peatlands , hot springs etc.
研究领域:
环境科学
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化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhuoyao Fang,Siyuan Pan,Xiaolin Zhang,Lu Lv,Bingcai Pan
Efficient removal of As(III) from groundwater remains an urgent but still challenging task. The X-Mn (X = Fe, Zr, Al…) binary oxide nanoparticles enable simultaneous oxidation and sequestration of As(III), yet facing the challenges in facile synthesis of the ultra-small nanoparticles with extraordinary decontamination reactivity, and in effective regeneration of oxidation capability. Herein, we prepared a novel nanocomposite Zr-Mn@N201 by conducting stepwise precipitation of hydrated oxides of zirconium (HZO) and manganese (HMO) inside the commercial gel-type anion exchanger N201, i.e. , the quaternary ammoniated poly(styrene-co-divinylbenzene) bead. Owing to restriction of nanopores, the HZO/HMO inside N201 possessed an ultra-small size around 4.78 nm. The kinetics and spectroscopic results suggested that As(III) was transformed into As(V) by HMO prior to adsorption onto HZO, and the negatively charged HMO captured most of the produced Mn 2+ ions. Alkaline treatment could regenerate Zr-Mn@N201 through simultaneously desorbing As(V) and transforming Mn 2+ into HMO again. During a 10-cyclic adsorption-regeneration assay, Zr-Mn@N201 could steadily reduce As(III) from 500 μg/L to < 10 μg/L with negligible HMO loss (<0.3%) in each run. In fixed-bed assays, the integration of HMO increased the effective treatment amounts of the Zr-Mn@N201 column toward the realistic groundwater by ∼ 11.5 times over the single nano-HZO ( i.e. , HZO@N201) column, reaching to ∼ 4600 bed volume with < 1% HMO loss.
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
ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Dun Fu,Tonni Agustiono Kurniawan,Heng Li,Haitao Wang,Yuanpeng Wang,Qingbiao Li
A highly efficient, eco-friendly and relatively low-cost catalyst is necessary to tackle bottlenecks in the treatment of industrial wastewater laden with heavy metals and antibiotic such as livestock farm and biogas liquids. This study investigated co-oxidative removal of arsenite (As(III)) and tetracycline (TC) by iron nanoparticles (Fe NP)-impregnated carbons based on heterogeneous Fenton-like reactions. The composites included Fe NP@biochar (BC), Fe NP@hydrochar (HC), and Fe NP@HC-derived pyrolysis char (HDPC). The functions of N and S atoms and the loading mass of the Fe NP in the Fe NP@BC in heterogeneous Fenton-like reactions were studied. To sustain its cost-effectiveness, the spent Fe NP@BC was regenerated using NaOH. Among the composites, the Fe NP@BC achieved an almost complete removal of As(III) and TC under optimized conditions (1.0 g/L of dose; 10 mM H 2 O 2 ; pH 6; 4 h of reaction; As(III): 50 μM; TC: 50 μM). The co-oxidative removal of As(III) and TC by the Fe NP@ BC was controlled by the synergistic interactions between the Fe NPs and the active N and S sites of the BC for generating reactive oxygen species (ROS). After four consecutive regeneration cycles, about 61 and 95% of As(III) and TC removal were attained. This implies that the spent carbocatalyst still has reasonable catalytic activities for reuse. Overall, this suggests that adding technological values to unused biochar as a carbocatalyst like Fe NP@BC was promising for co-oxidative removal of As(III) and TC from contaminated water .
研究领域:
环境科学
·
水处理工程
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DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 22
·13661-13670
·
IF 3.945
Si-Yuan Yu,Ying Liu,Hai-Tao Ren,Zhao-Yu Liu,Xu Han
Photooxidation of As(III) by TiO2 is a complicated process in which the oxidation mechanisms are always controversial. In this study, the enhanced photooxidation rates of As(III) with increasing pH values from 8.0 to 11.0 indicate the high photocatalytic reactivity of TiO2 under alkaline conditions. Moreover, As(III) improves the production of H2O2, indicating H-abstraction from As(III) (soluble or adsorbed) for H2O2 production. Although O2˙−, h+, ˙OH and –OOH are always regarded as the reactive oxygen species in the UV-TiO2 system, the superoxo and peroxo species formed on the surface of TiO2 also contribute to As(III) oxidation. The As(III)–O–Ti(IV) surface complexes formed on TiO2, as well as the decreased bandgaps of TiO2 with increasing concentrations of As(III) indicate that the ligand-to-metal charge transfer (LMCT) pathway also contributes to the oxidation of As(III) under alkaline conditions. Electrochemical analyses further reveal that As(III) enhances the electron density on the surface of TiO2, thereby improving the catalytic reactivity of TiO2. We therefore suggest that H-abstraction from As(III) or H2O to the formed superoxo and peroxo species results in the formation of H2O2, accompanied by the oxidation of As(III). This enriches our knowledge on the oxidation of As(III), as well as other contaminants rich in –OH groups during the photocatalytic oxidation processes.
研究领域:
环境科学
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化学
✓ 已验证
DOI
PubMed
高影响因子
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