GEODERMA
·
2015
·
IF 2.772
Meng Zhu,Chen Tu,Haibo Zhang,Yongming Luo,Peter Christie
A solvent extraction method coupled to high-performance liquid chromatography with tandem mass spectrometry detection (HPLC–MS/MS) was developed and validated for the simultaneous determination of soil diphenylarsinic acid (DPAA) and phenylarsinic acid (PAA). Several extraction solvents were evaluated with respect to the degree of soil extract-induced matrix effects and the recovery values for DPAA and PAA in the four studied soil matrices. Validation data showed that solvent extraction had a negligible impact on the accurate quantification of DPAA. In contrast, only with disodium hydrogen phosphate extraction did the method give both limited matrix effects (102–107%) with a coefficient of variation < 3% ( n = 4) and efficient recoveries (77–109%) at two spiking levels (20 and 50 mg kg − 1 ) for PAA. The selection of an appropriate extractant was the approach to reduce matrix effects while guaranteeing satisfactory recoveries of soil DPAA and PAA. Chromatographic separation was completed in 37 min and the analytes were detected in positive mode using selected reaction monitoring . MS/MS operating conditions were optimized for both electrospray ionization (ESI) and atmospheric pressure chemical ionization (APCI) sources. Under optimal conditions the detection limit was 0.01 and 1.00 μg L − 1 for DPAA and PAA. The method detection limits (MDLs) obtained ranged from 2.52 to 3.42 μg kg − 1 for DPAA and from 0.23 to 0.33 mg kg − 1 for PAA depending on the soil types, and the intraday and interday precision was less than 5% for both analytes at two different concentrations. The method was successfully applied for the simultaneous determination of DPAA and PAA in one-month aged soils, satisfactory recoveries (> 74.03%) were obtained for both analytes. The results show that the proposed solvent extraction method coupled to HPLC–MS/MS analysis can provide accurate and reliable determinations of DPAA and PAA in soil samples.
研究领域:
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
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
ENVIRONMENT INTERNATIONAL
·
2024
·
IF 10.3
Yizhao Wu,Song-Ge Deng,Yunxiang Xu,Yifan Zhang,Puguo Hao,Qi Zhao,Jibao Jiang,Yinsheng Li
The organoarsenical feed additive roxarsone (ROX) is a ubiquitous threat due to the unpredictable levels of arsenic (As) released by soil bacteria. The earthworms representing soil fauna communities provide hotspots for As biotransformation genes (ABGs). Nonetheless, the role of gut bacteria in this regard is unclear. In this study, the changes in As speciation, bacterial ABGs, and communities were analyzed in a ROX-contaminated soil (50 mg/kg As in ROX form) containing the earthworm Eisenia feotida . (RE vs. R treatment). After 56 d, earthworms reduced the levels of both ROX and total As by 59 % and 17 %, respectively. The available As content was 10 % lower in the RE than in R treatment. Under ROX stress, the total ABG abundance was upregulated in both earthworm gut and soil, with synergistic effects observed following RE treatment. Besides, the enrichment of arsM and arsB genes in earthworm gut suggested that gut bacteria may facilitate As removal by enhancing As methylation and transport function in soil. However, the bacteria carrying ABGs were not associated with the ABG abundance in earthworm gut indicating the unique strategies of earthworm gut bacteria compared with soil bacteria due to different microenvironments. Based on a well-fit structural equation model (P = 0.120), we concluded that gut bacteria indirectly contribute to ROX transformation and As detoxification by modifying soil ABGs. The positive findings of earthworm-induced ROX transformation shed light on the role of As biomonitoring and bioremediation in organoarsenical-contaminated environments.
研究领域:
环境科学
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers of Environmental Science & Engineering
·
2020
·Vol. 14
·期 4
·1-12
·
IF 4.053
Zhu Meng,Luo Yongming,Yang Ruyi,Zhou Shoubiao,Zhang Juqin,Zhang Mengyun,Christie Peter,Rylott Elizabeth L.
Diphenylarsinic acid (DPAA) is a phenyl arsenic compound derived from chemical warfare weapons. Macroscopic and microscopic work on DPAA sorption will provide useful information in predicting the partitioning and mobility of DPAA in the soil-water environment. Here, batch experiments and extended X-ray absorption fine structure (EXAFS) spectroscopy were used to investigate the sorption mechanisms of DPAA. The DPAA sorption data from 11 soil types was found to fit the Freundlich equation, and the sorption capacity, K f , was significantly and positively correlated with oxalate-extractable Fe 2 O 3 . The K f values of eight of the 11 untreated soils (1.51–113.04) significantly decreased upon removal of amorphous metal (hydr)oxides (0.51–13.37). When both amorphous and crystalline metal (hydr)oxides were removed from the untreated soils, the K f values either decreased or slightly increased (0.65–3.09). Subsequent removal of soil organic matter from these amorphous and crystalline metal (hydr)oxide-depleted samples led to further decreases in K f to 0.02–1.38, with only one exception (Sulfic Aquic-Orthic Halosols). These findings strongly suggest that ligand exchange reactions with amorphous metal (hydr)oxides contribute most to DPAA sorption on soils. EXAFS data provide further evidence that DPAA primarily formed bidentate binuclear ( 2 C ) and monodentate mononuclear ( 1 V ) coring-sharing complexes with As-Fe distances of 3.34 and 3.66 Å, respectively, on Fe (hydr)oxides. Comparison of these results with earlier studies suggests that 2 C and 1 V complexes of DPAA may be favored under low and high surface coverages, respectively, with the formation of 1 V bonds possibly conserving the sorption sites or decreasing the steric hindrance derived from phenyl substituents.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 27
·期 14
·16646-16655
·
IF 3.056
Zhu Meng,Luo Yongming,Cheng Nannan,Yang Ruyi,Zhang Juqin,Zhang Mengyun,Christie Peter
Diphenylarsinic acid (DPAA) is an emerging phenylarsenic compound derived from chemical warfare agents. It has been suggested that biostimulation of sulfate reduction decreases the concentrations of DPAA in soils. However, biostimulation often induces Fe(III) reduction which may affect the mobility and thereby the transformation of DPAA. Here, a soil incubation experiment was carried out to elucidate the impact of Fe(III) reduction on the mobilization and transformation of DPAA in a biostimulated Acrisol with the addition of sulfate and lactate. DPAA was significantly mobilized and then thionated in the sulfide soil (amended with sulfate and sodium lactate) compared with the anoxic soil (without addition of sulfate or sodium lactate). At the start of the incubation period, 41.8% of the total DPAA in sulfide soil was mobilized, likely by the addition of sodium lactate, and DPAA was then almost completely released into the solution after 2 weeks of incubation, likely due to Fe(III) reduction. The relatively low fraction of oxalate-extractable Fe in Acrisol, which contributes significantly to DPAA sorption and is more active and reduction-susceptible, may explain the observation that only < 40% of the Fe(III) (hydr)oxides were reduced when DPAA was completely released into the solution. A more rapid and final enhanced elimination of DPAA was observed in sulfide soil and the fraction of total DPAA decreased to 60.1 and 91.0%, respectively, at the end of the incubation in sulfide soil and anoxic soil. The difference appears to result from increased DPAA mobilization and sulfate reduction in sulfide soil. On the other hand, the formation of FeS precipitate, a product of Fe and sulfate reduction, may reduce the efficiency of DPAA thionation. Accordingly, the potentially contrasting effects of Fe(III) reduction on DPAA thionation need be considered when planning biostimulated sulfate reduction strategies for DPAA-contaminated soils.
研究领域:
环境科学
·
土壤学
·
污染修复
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Hepeng Zhou,Fanxin Xie,Xianping Luo,Boyuan Zhang,Siqi Yang,Yongbing Zhang
In this paper, the effect of benzyl arsenic acid (BAA) and sodium oleate (NaOl) on mineral flotation was studied for the first time from the perspective of the difference of solidophilic atom. Compared with NaOl, the solidophilic O atoms of BAA had stronger electronegativity and the bonding strength of As-O was lower than that of C O. Thus, when BAA adsorbed on the mineral surfaces, the bonding strength of the solidophilic O atoms with the adsorption sites would be higher. The DFT calculation of adsorption model indicated that after activation by Ca(OH) + , the adsorption capacity of BAA on spodumene surface was significantly higher than that of NaOl, while the adsorption strength on feldspar was similar to that of NaOl. This result was corroborated by flotation experiment and adsorption capacity test. Thus, compared with NaOl, BAA could separate and recover spodumene more effectively.
研究领域:
矿物加工工程
·
材料科学与工程
✓ 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
BIORESOURCE TECHNOLOGY
·
2017
·
IF 5.651
Wei Sun,Xun Qian,Jie Gu,Xiao-Juan Wang,Li Zhang,Ai-Yun Guo
High concentrations of residual arsanilic acid occur in pig manure due to its use in feed to promote growth and control diseases. This study compared the effects of arsanilic acid at three concentrations (0, 325, and 650 mg/kg dry pig manure) on the abundance of antibiotic resistance genes (ARGs) and the microbial community during anaerobic digestion. Addition of 650 mg/kg arsanilic acid enhanced the absolute abundances of tetC , sul2 , ermB , and gyrA more than twofold in the digestion product. Redundancy analysis indicated that the change in the microbial community structure was the main driver of variation in the ARGs profile. The As resistance gene arsC co-occurred with four ARGs and intI1 , possibly causing the increase in ARGs under pressure by arsanilic acid. High arsanilic acid concentrations can increase the risk of ARGs occurring in anaerobic digestion products. The amount of arsanilic acid used as a feed additive should be controlled.
研究领域:
环境科学
·
微生物学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED AND ENVIRONMENTAL MICROBIOLOGY
·
2022
·Vol. 88
·期 6
·
IF 5.005
Ke Huang,Wei Liu,Yuanhe Li,Sha Zeng,Fang-Jie Zhao
Methylarsenate (MAs(V)) is a product of microbial arsenic (As) biomethylation and has also been widely used as an herbicide. Some microbes are able to reduce nontoxic MAs(V) to highly toxic methylarsenite (MAs(III)) possibly as an antibiotic. The mechanism of MAs(V) reduction in microbes has not been elucidated. Here, we found that the bacterium Enterobacter sp. CZ-1 isolated from an As-contaminated paddy soil has a strong ability to reduce MAs(V) to MAs(III). Using a MAs(III)-responsive biosensor to detect MAs(V) reduction in E. coli Trans5α transformants of a genomic library of Enterobacter sp. CZ-1, we identified gshA, encoding a glutamate-cysteine ligase, as a key gene involved in MAs(V) reduction. Heterologous expression of gshA increased the biosynthesis of glutathione (GSH) and MAs(V) reduction in E. coli Trans5α. Deletion of gshA in Enterobacter sp. CZ-1 abolished its ability to synthesize GSH and decreased its MAs(V) reduction ability markedly, which could be restored by supplementation of exogenous GSH. In the presence of MAs(V), Enterobacter sp. CZ-1 was able to inhibit the growth of Bacillus subtilis 168; this ability was lost in the gshA-deleted mutant. In addition, deletion of gshA greatly decreased the reduction of arsenate to arsenite. These results indicate that GSH plays an important role in MAs(V) reduction to generate MAs(III) as an antibiotic.IMPORTANCE Arsenic is a ubiquitous environmental toxin. Some microbes detoxify inorganic arsenic through biomethylation, generating relatively nontoxic pentavalent methylated arsenicals, such as methylarsenate. Methylarsenate has also been widely used as an herbicide. Surprisingly, some microbes reduce methylarsenate to highly toxic methylarsenite possibly to use the latter as an antibiotic. How microbes reduce methylarsenate to methylarsenite is unknown. Here, we show that gshA encoding a glutamate-cysteine ligase in the glutathione biosynthesis pathway is involved in methylarsenate reduction in Enterobacter sp. CZ-1. Our study provides new insights into the crucial role of glutathione in the transformation of a common arsenic compound to a natural antibiotic.
研究领域:
微生物学
·
环境科学
·
毒理学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Meng Zhu,Yuan Li,Xiaobao Wei,Zhenqi Yan,Lu Yang,Ruyi Yang
Iron reduction impacts the mobilization and thionation of diphenylarsinic acid (DPAA) in soil, but the contribution of crystalline and non-crystalline iron remains unknown. A paddy soil deficient in non-crystalline iron (P-Fe o ), crystalline and non-crystalline iron (P-Fe d ) were incubated with sulfate-plus-lactate, and the results were compared with paddy soil (P) in our previous study. For treatments without ferrous sulfide (FeS) precipitation, the solution-to-solid ratio ( R L/S ) of DPAA increased slightly and dramatically with iron reduction, respectively, for P-Fe o and P, suggesting that the reduction of non-crystalline iron contributes more to DPAA mobilization than crystalline iron. The R L/S was > 0.667 and ≤ 0.667 for treatments without and with FeS, respectively, in P and P-Fe o but not P-Fe d , indicating that crystalline, rather than non-crystalline iron contributes more to DPAA sequestration through reduction and the subsequent FeS precipitation. The degree to which iron reduction facilitates DPAA mobilization or sequestration is likely determined by the composition and amount of iron in paddy soil, respectively. For treatments with FeS, the DPAA transformation rate was < 44 % and 74–86 %, respectively, in P-Fe o and P-Fe d after 90 days, with the maximum value comparable to those without FeS in P after 30 days. This suggests that the crystalline iron in P-Fe o and the residual, small amount of non-crystalline iron in P-Fe d could reduce DPAA thionation by forming FeS, and such effect seems to depend on both the composition and the amount of iron in paddy soil. The results would deepen our understanding of the “As-Fe-S” interactions in soil.
研究领域:
土壤科学
·
环境化学
✓ 已验证
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Guanbao Yao,Rui Tang,Haiping Luo,Shoujun Yuan,Wei Wang,Liwen Xiao,Xiangqian Chu,Zhen-Hu Hu
Zero-valent iron (ZVI) can enhance anaerobic digestion , and has great potential to alleviate/eliminate methanogenesis inhibition. Little is known about the feasibility of utilizing ZVI to alleviate methanogenesis inhibition that is caused by typical animal feed additive roxarsone in livestock wastewater. In this study, the role of ZVI on alleviating roxarsone-induced methanogenic inhibition and its mechanisms were investigated. With the increase of roxarsone concentration from 5 to 50 mg/L, the inhibition of methanogenesis increased from 3.0% to 65.7%. This inhibition was alleviated by 80.7% and 57.2% when 1.0 and 10.0 g/L ZVI were added, respectively. Due to ZVI addition, an efficient arsenic immobilization onto ZVI (45.4–85.8%) was achieved mainly through the formation of FeAsO 4 precipitate and adsorption by ZVI. Under the function of ZVI, hydrogenotrophic methanogenic activity was obviously restored. The microbial community analysis indicates that the ZVI-regulated alleviation on the methanogenesis inhibition was attributed to the enrichment of Methanobacterium and Methanosarcina . The findings from this study demonstrate that ZVI addition is an effective way for treatment of organoarsenic-contaminated wastewater.
研究领域:
环境科学
·
微生物学
✓ 已验证
DOI
PubMed
高影响因子
ELECTROPHORESIS
·
2020
·Vol. 42
·期 6
·719-724
·
IF 3.081
Evgeniya V. Polyakova,Olga V. Shuvaeva,Olga S. Koshcheeva,Yuliya E. Tyutereva,Ivan P. Pozdnyakov
Arsenic aromatic compounds including p-arsanylic acid (pASA) are still widely used in a number of countries as the feed additives in animal breeding resulting in its entering the environment. Under the influence of oxidizing agents or UV radiation, pASA undergoes transformations leading to generation of inorganic arsenic species that are more mobile and toxic than organic ones. On the one hand, an approach based on the treatment of contaminated waters by UV irradiation seems perspective for their detoxification, but the feasibility of this approach depends on the composition of the products forming as a result of photodegradation. In the present work, a CZE was applied for the study of the pASA degradation process during stationary (308 nm) photolysis in the presence of Fe(III)-oxalate complex. A developed assay allowed controlling the parent compounds and also As-containing products of pASA degradation, presented mainly by arsenate and arsenite ions. It was found that the main inorganic derivatives of the pASA photolytic conversions are presented by arsenate and arsenite ions whose ratio depends on the initial amount of pASA and reaction conditions.
研究领域:
环境科学
·
分析化学
✓ 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）