Minerals
·
2021
·Vol. 11
·期 2
·105
·
IF 2.644
Yifan Yang,Shiyong Tao,Zhichun Dong,Jing Xu,Xiang Zhang,Guoyan Pan
Because of the diversification of industries in developing cities, the phenomenon of the simultaneous contamination of various kinds of pollutants is becoming common, and the environmental process of pollutants in multi-contaminated environmental mediums has attracted attention in recent years. In this study,p-arsanilic acid (ASA), a kind of organic arsenic feed additive that contains the arsenic group in a chemical structure, is used as a typical contaminant to investigate its adsorption on iron oxides and its implication for contaminated soils. The adsorption kinetics on all solids can be fitted to the pseudo-second-order kinetic model well. At the same mass dosage conditions, the adsorption amount per unit surface area on iron oxides follows the order α-FeOOH > γ-Fe2O3> α-Fe2O3, which is significantly higher than that for actual soil, because of the lower content of iron oxides in actual soil. Lower pH conditions favor ASA adsorption, while higher pH conditions inhibit its adsorption as a result of the electrostatic repulsion and weakened hydrophobic interaction. The presence of phosphate also inhibits ASA adsorption because of the competitive effect. Correlations between the amount of ASA adsorption in actual soil and the Fe2O3content, total phosphorus content, arsenic content, and organic matter content of actual soil are also investigated in this work, and a moderate positive correlation (R2= 0.630), strong negative correlation (R2= 0.734), insignificant positive correlation (R2= 0.099), and no correlation (R2= 0.006) are found, respectively. These findings would help evaluate the potential hazard of the usage of organic arsenic feed additives, as well as further the understanding of the geochemical processes of contaminants in complicated mediums.Keywords:p-arsanilic acid;iron oxides;soil contamination;adsorption
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Ze Yang,Songding Guo,Zhenglai Huan,Yongbing Zhu,Tingting Zhang,Shangyi Li
In this study, we dexterously constructed a unique in situ interface oxidation–adsorption dual-reaction platform through the self-excitation of ferrate (Fe(VI))/peroxymonosulfate (PMS) for phenylarsonic acid (PAA) and inorganic As(V) removal. When the molar ratio of Fe(VI)/PMS was 1:2, 80% degradation of PAA could be achieved within 180 min and the apparent constant value of the reaction rate ( k obs ) would reach up to 0.185 min −1 . 1 O 2 and Fe(IV) were the main active species for degradation of PAA in Fe(VI)/PMS reaction system. In addition, we explored the possible degradation intermediates and pathway of PAA. In situ Fe(III) oxides generated from Fe(VI) decomposition could adsorb arsenic pollutants through ligand exchange with inorganic As(V) through surface hydroxyl groups to form Fe-O-As bonds. The effect of coexisting anions on the removal performance of the system was investigated, and the results showed that the presence of PO 4 3− and CO 3 2− promoted the oxidative degradation of PAA owing to the activation of PMS by PO 4 3− and CO 3 2− , but Cl − can inhibit the PAA degradation through a free radical scavenging mechanism. PO 4 3− and SiO 3 2− affected the adsorption and removal of the released inorganic As(V) due to their competitive adsorption of in situ Fe(III) oxides. Density functional theory (DFT) calculations indicated an obvious electron transfer (1.83 e) between the in situ Fe(III) oxides and inorganic As(V) with a high adsorption energy of −10.30 eV. These results indicate that the combination of Fe(VI) and PMS can effectively control the total arsenic (total-As) in water bodies.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Yuliya E. Tyutereva,Petr S. Sherin,Evgeniya V. Polyakova,Olga S. Koscheeva,Vyacheslav P. Grivin,Victor F. Plyusnin,Olga V. Shuvaeva,Ivan P. Pozdnyakov
Organic arsenicals are important environment pollutants due to wide use in livestock and toxicity of degradation products . In this work we report about the efficient photodegradation of the p-arsanilic acid (p-ASA) and its decomposition products in the Fe(III)-oxalate assisted approach under nature-relevant conditions. At neutral pH under near-visible UV irradiation the Fe(III) oxalate complexes generate the primary oxidizing intermediate, OH radical (the quantum yield of ϕ OH ∼ 0.06), which rapidly reacts with p-ASA with high rate constant, (8.6 ± 0.5) × 10 9 M −1 s −1 . Subsequent radical reactions result in the complete photooxidation of both p-ASA and basic aromatic photoproducts with the predominant formation of inorganic arsenic species, mainly As(V), under optimal conditions. Comparing with the direct UV photolysis, the presented Fe(III)-oxalate mediated degradation of p-ASA has several advantages: higher efficiency at low p-ASA concentration and complete degradation of organic arsenic by-products without use of short-wavelength UV radiation. The obtained results illustrate that the Fe(III)-oxalate complexes are promising natural photosensitizers for the removal of arsenic pollutants from contaminated waters .
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2015
·Vol. 182
·期 7
·1247-1254
·
IF 3.741
Dai Hong,Gong Lingshan,Lu Shuangyan,Zhang Qingrong,Li Yilin,Zhang Shupei,Xu Guifang,Li Xiuhua,Lin Yanyu,Chen Guonan
We have developed a sensor for 4-aminophenylarsonic acid (4-APhAA) by coating a glassy carbon electrode (GCE) with a composite prepared from an ionic liquid and dahlia-like carbon nanohorns (CNHs). The good electric conductivity, large surface area and high pore volume of the CNHs, and the synergistic action of the ionic liquid (which is a good dispersant with excellent ion conductivity) result in efficient electrocatalysis towards oxidation of 4-APhAA. The effect was investigated by various electrochemical methods, and the electron transfer coefficient, diffusion coefficient, standard heterogeneous rate constant and thermodynamic activation energy were determined. The response range of 4-APhAA was evaluated using an i-t plot. If operated at a working voltage of 900 mV (vs Ag/AgCl), the sensor responds to 4-APhAA over the 0.5 μM to 3.5 M concentration range.
An electrochemical sensor for 4-aminophenylarsonic acid is presented that consists of a glassy carbon electrode modified with carbon nanohorns and ionic liquids.
研究领域:
分析化学
·
电化学
·
生物医学工程
·
纳米材料
·
环境监测
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2020
·
IF 9.13
Panxin Wang,Xu He,Wei Zhang,Jun Ma,Jin Jiang,Zhuangsong Huang,Haijun Cheng,Suyan Pang,Yang Zhou,Xuedong Zhai
As a common animal feed additive, p-arsanilic acid (p-AsA) is thought to be excreted with little uptake and unchanged chemical structure, threatening the environment by potentially releasing more toxic inorganic arsenic. We herein investigated the removal of arsenic by in situ formed ferric (oxyhydr)oxides with the promotion of p-AsA degradation in Fe(II)/peroxydisulfate (PDS) system. Results showed that under acid conditions, p-AsA degraded very quickly and over 99% of p-AsA (5 μM) was degraded within 10 min at the optimal dosage of Fe(II) (100 μM) and PDS (150 μM) at pH 3, while less than 66.4% of arsenic was removed at pH 3–5. Higher pH (3–7) would inhibit the degradation of p-AsA but promote the arsenic removal. At pH 6–7, over 98.5% of total arsenic was removed, while the degradation efficiency of p-AsA was lower than 52.4%. HPLC-ICP-MS results indicated that the arsenic group was cleaved from p-AsA in the form of As(III) and then rapidly oxidized to As(V). FTIR and XPS analysis indicated that both As(V) products and residual p-AsA were bonded to ferric (oxyhydr)oxides via hydroxyl groups. Common cations (e.g., Na + , Ca 2+ , Mg 2+ ) and anions such as Cl − , SO 4 2− , CO 3 2− had no significant influence on arsenic removal, while SiO 3 2− , PO 4 3− and HA inhibited the removal of total arsenic, mainly by affecting the zeta potential of iron particles. In summary, the Fe(II)/PDS process, as an efficient method for partial oxidation and simultaneous adsorption of p-AsA under near-neutral conditions, is expected to control the potential environmental risks of p-AsA.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2021
·
IF 4.291
Yuliya E. Tyutereva,Petr S. Sherin,Evgeniya V. Polyakova,Vyacheslav P. Grivin,Victor F. Plyusnin,Olga V. Shuvaeva,Jing Xu,Feng Wu,Ivan P. Pozdnyakov
The p-arsanilic acid (p-ASA) is widely used in agriculture as a food additive to control parasites. It leaves the body almost unchanged and is subsequently destroyed by environmental factors with the formation of toxic forms of inorganic arsenic. UVA irradiation of p-ASA with the addition of the Fe(III) oxalate complex leads to an effective photodegradation of the target compound. However, this method needs high concentrations of reagents and the keeping high [oxalate]:[Fe(III)] ratio to maintain proper efficiency of Fe(III) oxalate system. In this work, to overcome these problems, potassium persulfate (PS) was used as an additional oxidizer to improve Fe(III) oxalate system. It was found that the sulfate radical produced upon PS activation reacts readily with both neutral and monoanionic forms of p-ASA yielding corresponding organic cation radical, bimolecular rate constants are (7.3 ± 0.6) × 10 9 and (2.4 ± 0.4) × 10 9 M −1 s −1 , accordingly. Addition of 1 mM of PS reduces to one order (from 1.6 to 0.12 mM) the working concentration of oxalate and allows to achieve the complete degradation of both p-ASA and organic byproducts to inorganic As(V). Also the proposed approach demonstrates high efficiency in a wide range (from <0.5 to 3 ppm) of p-ASA concentrations.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2015
·
IF 4.099
A-nan Wang,Ying Teng,Xue-feng Hu,Long-hua Wu,Yu-juan Huang,Yong-ming Luo,Peter Christie
Diphenylarsinic acid (DPAA) is formed during the leakage of arsenic chemical weapons in sites and poses a high risk to biota. However, remediation methods for DPAA contaminated soils are rare. Here, the photocatalytic oxidation (PCO) process by nano-sized titanium dioxide (TiO 2 ) was applied to degrade DPAA in soil. The degradation pathway was firstly studied, and arsenate was identified as the final product. Then, an orthogonal array experimental design of L 9 (3) 4 , only 9 experiments were needed, instead of 81 experiments in a conventional one-factor-at-a-time, was used to optimize the operational parameters soil:water ratio, TiO 2 dosage, irradiation time and light intensity to increase DPAA removal efficiency. Soil:water ratio was found to have a more significant effect on DPAA removal efficiency than other properties. The optimum conditions to treat 4 g soil with a DPAA concentration of 20 mg kg − 1 were found to be a 1:10 soil: water ratio, 40 mW cm − 2 light intensity, 5% TiO 2 in soil, and a 3-hour irradiation time, with a removal efficiency of up to 82.7%. Furthermore, this method (except for a change in irradiation time from 3 to 1.5 h) was validated in nine different soils and the removal efficiencies ranged from 57.0 to 78.6%. Removal efficiencies were found to be negatively correlated with soil electrical conductivity, organic matter content, pH and total phosphorus content. Finally, coupled with electron spin resonance (ESR) measurement, these soil properties affected the generation of OH• by TiO 2 in soil slurry. This study suggests that TiO 2 photocatalytic oxidation is a promising treatment for removing DPAA from soil.
研究领域:
环境科学
·
化学工程
·
土壤学
✓ 已验证
DOI
PubMed
高影响因子
Applied Sciences-Basel
·
2018
·Vol. 8
·期 4
·615
·
IF 1.689
Xiangyi Shen,Jing Xu,Ivan P. Pozdnyakov,Zizheng Liu
Used as a kind of feed additive,p-arsanilic acid can pose a potential risk to organisms when abandoned in the environment. The photodegradation ofp-ASA was investigated under UV-C irradiation in the presence of persulfate (PS) in this work. The addition of PS facilitated the decomposition ofp-ASA and notably, the presence of 50 mmol PS brought about a nearly complete mineralization after 3 h, while an insignificant total organic carbon (TOC) removal was observed under UV irradiation (λ = 254 nm) only. Experimental results proved that sulfate radical (SO4•−) was responsible for the promotion effect. The cleavage of As-C bond released inorganic arsenic and caused the occurrence of various organic products, for example, hydroxybenzaldehyde, nitrobenzene, benzenediol sulfate, and biphenylarsinic acid. The application of PS with UV-C light may throw a light on thorough treatment forp-ASA containing wastewater.Keywords:p-arsanilic acid;photodegradation;UV/persulfate system;sulfate radical
研究领域:
环境科学
·
化学工程
·
水处理
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xiong Peng,Zhijia Luo,Hongmei Xie,Wanwen Liang,Jinlu Luo,Chengxiong Dang,Aili Wang,Lihua Hu,Xiwen Yu,Weiquan Cai
Phenylarsonic acids are deemed as emerging contaminants, and their removal by carbonaceous materials has aroused wide attentions. However, the adsorption behaviors and mechanisms on nitrogen doped carbon still remain unclear. Herein, nitrogen doped porous carbons (NC-x) for adsorbing p -arsanilic acid and roxarsone were fabricated by hydrothermal and following activation treatment of peanut shell. The results revealed that NC-750 which was activated at 750 °C exhibited high BET surface area of 1331.11 m 2 /g, total pore volume of 0.97 cm 3 /g and average pore size of 2.91 nm, and its maximum equilibrium capacities based on Sips model for p -arsanilic acid and roxarsone were 287.3 mg/g and 462.6 mg/g, respectively. The sufficient adsorption space, rich defect structure and high affinity of nitrogen-containing groups endow NC-750 with high adsorption capacities, and the adsorption mechanisms involve with pore-filling, hydrogen bonding and π-π interactions. Density functional theory (DFT) calculation demonstrated that p -arsanilic acid was electron donor while roxarsone was electron acceptor, and graphitic nitrogen was conducive to the π-π interactions while pyrrolic nitrogen and pyridinic nitrogen were preferential for hydrogen bonding interactions. This work can provide reference for understanding the adsorption behaviors and interfacial mechanisms between phenylarsonic acid and nitrogen doped carbonaceous materials.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·
IF 5.8
Sun Zuyou,Zhou Jiali,Zhang Hui,Liu Zufan,Tao Shiyong,Xu Jing
The widespread used organoarsenicals have drawn attention for decades due to their potential environment risks. In this study, a heterogeneous system of goethite/oxalate irradiated using UVA light ( λ = 365 nm) was applied for the removal of ASA, a kind of organoarsenicals used in animal feeding operations as additives, from the aqueous phase through photodegradation. Results showed that the presence of 5 mM of oxalate significantly enhanced the photodegradation efficiency of ASA in the 0.1 g/L of goethite suspended system from 28 to ~100% within 180 min reaction at pH 5. Acid conditions favored the photoreaction rate, compared with neutral and basic conditions. This reaction process was also influenced by the initial concentration of oxalate and ASA. Furthermore, the mechanism study was conducted by quenching experiments and revealed the important roles of ·OH in the degradation of ASA in the goethite/oxalate/UVA system. By analyzing the reaction products, both inorganic arsenic (As(III) and As(V)) and ammonia were detected during the photodegradation of ASA. These findings help to gain a better understanding of the geochemical behavior of ASA in surface water and can also provide a potential treatment method for the organoarsenicals contaminated water.
研究领域:
环境科学
·
水处理
·
光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science of Advanced Materials
·
2021
·Vol. 13
·期 4
·550-555
·
IF 1.474
Dou Mingyu,Zhao Wenli,Lin Jie,Huang Xianqiang,Li Dacheng
In this work, a novel 4-aminophenylarsonic acid functionalized polyoxovanadates (POVs) hybrid material, namely, (Me2NH2)4 ·[(L)8(H12V16O32)] (H2L = 4-NH2C6H4AsO3H2)
POVs 1 was solvothermally synthesized and fully characterized. The results revealed POVs 1 consists of four similar tetranuclear vanadium clusters bridged by eight organic 4-aminophenylarsonic acid ligands. Remarkably, functionalized hybrid POVs 1 was further investigated as a heterogeneous
stable catalyst in oxidation of sulfide derivatives, and exhibited high catalytic activities (yields up to 96.7%). Additionally, the functionalized hybrid polyoxovanadates catalyst can be reused without losing activities after three runs cycle.
研究领域:
材料科学
·
催化
·
无机化学
✓ 已验证
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
✓ 已验证
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）