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
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
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
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
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wen-Qing Ding,Lei Xu,Xiao-Ying Li,Ming-Lai Fu,Baoling Yuan
Metal–organic frameworks (MOFs) are emerging as advanced nanoporous materials to remove phenylarsenic acid, p-arsanilic acid (p-ASA), and roxarsone (ROX) in the aqueous solution, while MOFs are often present as powder state and encounter difficulties in recovery after adsorption, which greatly limit their practical application in the aqueous environments. Herein, MIL-101 (Fe), a typical MOF, was mixed with sodium alginate and gelatin to prepare MIL-101@CAGE by three-dimensional (3D) printing technology, which was then used as a separatable adsorbent to remove phenylarsenic acid in the aqueous solution. The structure of 3D-printed MIL-101@CAGE was first characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FTIR), and thermogravimetry and differential thermogravimetry (TG-DTG). The octahedral morphology of MIL-101 (Fe) was found unchanged during the 3D printing process. Then, the adsorption process of MIL-101@CAGE on phenylarsenic acids was systematically investigated by adsorption kinetics, adsorption isotherms, adsorption thermodynamics, condition experiments, and cyclic regeneration experiments. Finally, the adsorption mechanism between MIL-101@CAGE and phenylarsenic acid was further investigated. The results showed that the Langmuir, Freundlich, and Temkin isotherms were well fit, and according to the Langmuir fitting results, the maximum adsorption amounts of MIL-101@CAGE on p-ASA and ROX at 25 °C were 106.98 and 120.28 mg/g, respectively. The removal of p-ASA and ROX by MIL-101@CAGE remained stable over a wide pH range and in the presence of various coexisting ions. The regeneration experiments showed that the 3D-printed MIL-101@CAGE could still maintain a more than 90% removal rate after five cycles. The adsorption mechanism of this system might include π–π stacking interactions between the benzene ring on the phenylarsenic acids and the organic ligands in MIL-101@CAGE, hydrogen-bonding, and ligand-bonding interactions (Fe–O–As). This study provides a new idea for the scale preparation of a separatable and recyclable adsorbent based on MOF material for the efficient removal of phenylarsenic acid in the aqueous solution.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yuxin Li,Li Liu,Zeming Wang,Lixiang Zhou,Yeqing Lan,Cheng Chen
4-aminophenylarsonic acid ( p -ASA) is usually employed as feed antibiotics which can kill bacteria, protozoa and spirochetes. When p -ASA is released into the environment by biological metabolism, it could be broken down to produce hypertoxic inorganic arsenic, including arsenite (AsO 3 3- ) and arsenate (AsO 4 3- ). In this study, cobalt and lanthanum composites loaded on rice straw biochar labelled as Co 3 O 4 -La 2 CO 5 @RSBC was obtained. The material was used as an efficient catalyst for peroxymonosulfate (PMS) activation and adsorbent to achieve the simultaneous degradation of p -ASA and adsorption of arsenic. 100% decomposition of p -ASA (50 μmol L -1 ) could be realized within 30 min, coupled with nearly complete removal of inorganic arsenic during 80 min at initial pH = 7. Co 3 O 4 -La 2 CO 5 @RSBC also possessed superior reusability and stability. Even in the third cycle, more than 95% of p -ASA was decomposed and meanwhile 92.5% of inorganic arsenic was removed. No cobalt ions were detected, and the concentration of lanthanum ions in the three cycles ranged from 8.05 to 9.90 mg L -1 , which was much lower than those reported in previous studies. A series of the material characterizations, electron paramagnetic resonance technology and scavenger tests were utilized to unveil the possible catalytic mechanism and the transformation pathways of p -ASA and arsenic. It was confirmed that 1 O 2 , O 2 ∙ - , OH ∙ , and SO 4 ∙ - generated from the PMS activation were responsible for the degradation of p -ASA and the oxidation of As(III) to As(V). Meanwhile, As(V) was rapidly adsorbed by Co 3 O 4 -La 2 CO 5 @RSBC. This study provides us with a novel and efficient approach to control p -ASA pollution in aqueous solution.
研究领域:
环境科学
·
催化材料
·
污染控制
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2018
·Vol. 6
·期 1
·207-215
·
IF 6.087
Miao Peng,Guijian Guan,Hong Deng,Bin Han,Chen Tian,Junyang Zhuang,Yunyun Xu,Weizhen Liu,Zhang Lin
Considering p-arsanilic acid (p-ASA) as an organoarsenic pollutant, monitoring concentration of p-ASA is significant to maintain environmental security. Photoelectrochemical (PEC) detection is promisingly applied in environmental monitoring for its lower cost and simpler operation, compared to traditional techniques. However, general electrode materials of PEC sensors need to be modified with biological probes due to lack of specific binding sites to analytes, which may lead to complicated sensor fabrication and bio-recognizers inactivation during storage. Herein, a porphyrinic metal–organic framework/reduced graphene oxide (PCN-224/rGO) nanocomposite with simultaneously excellent photoelectric activity and strong binding characteristics was prepared and used to fabricate a PEC sensor for p-ASA detection avoiding the modification of bio-recognizers. Benefiting from the high conductivity of rGO, the separation efficiency of charge carriers was improved in PCN-224/rGO and thereby photocurrent gained an amplification of about 12 times. The PCN-224/rGO nanocomposite had strong affinity to p-ASA via Zr–O–As coordination and π–π stacking. Significantly, the binding of p-ASA could adjust the band position of PCN-224/rGO and facilitate oxygen reduction by releasing more photogenerated electrons, achieving photocurrent enhancement. The developed PEC sensor had a wide detection range, from 10 ng L−1 to 10 mg L−1, with a detection limit of 5.47 ng L−1. Furthermore, the sensor was successfully applied to monitor p-ASA in simulated natural water and swine manure lixivium. This study paved the way for the design of more efficient PEC sensors for environmental monitoring.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）