Speciation and sorption structure of diphenylarsinic acid in soil clay mineral fractions using sequential extraction and EXAFS spectroscopy

Zhu, Meng; Hu, Xuefeng; Tu, Chen; Luo, Yongming; Yang, Ruyi; Zhou, Shoubiao; Cheng, Nannan; Rylott, Elizabeth L.

doi:10.1007/s11368-019-02431-2

Cited by 8 publications

(10 citation statements)

References 62 publications

(73 reference statements)

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“…3(b)) in contrast to the DPAA standard, and the second shell was fitted with four C atoms at As-C 2 (the second-nearest C) distance of 2.79 Å (Table 4). The fitted As-O, As-C 1 and As-C 2 distances in the present study correspond well with the EXAFS data (Tanaka et al, 2014;Zhu et al, 2019aZhu et al, , 2019b and density functional theory (DFT) calculations (Tanaka et al, 2014) reported in the literature.…”

Section: Resultssupporting

confidence: 89%

“…The two fitting approaches yielded similar results, which are listed in Table 4. The k 3 -weighted EXAFS spectra of DPAA, together with the contributions of the first and second shells, can be found in our previous study (Zhu et al, 2019a). When the RDF of the highly DPAA-contaminated soil (Fig.…”

Section: Resultsmentioning

confidence: 72%

“…The fitted As-Fe distances at 3.34 and 3.66 Å correspond to As linked to the surface of Fe (hydr)oxides by forming 2 C and 1 V complexes, respectively, according to Fendorf et al (1997). These types of DPAA complexes have been observed in DPAA sorption onto various Fe minerals (Tanaka et al, 2014;Zhu et al, 2019b) and clay mineral fractions of soils (Zhu et al, 2019a).…”

Section: Resultsmentioning

confidence: 83%

“…When the RDF of the highly DPAA-contaminated soil (Fig. 3(b)) was compared with that of the DPAA standard (Zhu et al, 2019a), both yielded an intense peak at 1-2 Å, which is related to the contributions of As-O and As-C 1 (the nearest C) in the mixed, first-neighbor shell. The fitted inter-atomic distances for As-O and As-C 1 (Table 4) were 1.69 and 1.89 Å, respectively.…”

Section: Resultsmentioning

confidence: 99%

“…These results suggest that DPAA sorption on soils may be due mainly to ligand exchange reactions with hydroxyl groups on metal (hydr)oxides rather than hydrophobic interactions with SOM. A recent finding is that DPAA exists predominantly as amorphous and crystalline Fe/Al (hydr) oxide associated forms in clay mineral fractions of soils (Zhu et al, 2019a). However, the contributions of Fe/Al (hydr)oxides and their different degrees of crystallinity to DPAA sorption on soils are still unknown.…”

Section: Introductionmentioning

confidence: 99%

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Diphenylarsinic acid sorption mechanisms in soils using batch experiments and EXAFS spectroscopy

Zhu

Luo

Yang

et al. 2020

Front. Environ. Sci. Eng.

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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 oxalateextractable 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.

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Section: Resultssupporting

confidence: 89%

Section: Resultsmentioning

confidence: 72%

Section: Resultsmentioning

confidence: 83%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Diphenylarsinic acid sorption mechanisms in soils using batch experiments and EXAFS spectroscopy

Zhu

Luo

Yang

et al. 2020

Front. Environ. Sci. Eng.

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Contrasting effects of iron reduction on thionation of diphenylarsinic acid in a biostimulated Acrisol

Zhu

Luo

Cheng

et al. 2020

Environ Sci Pollut Res

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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.

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Stability and transport of titanium dioxide nanoparticles in three variable-charge soils

Zhang

et al. 2019

J Soils Sediments

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Purpose The exposure pathways and environmental impacts of titanium dioxide nanoparticles (TiO 2 NPs) released into soils could be significantly influenced by their stability and transport behaviors. The aim of this study was to investigate the stability and transport of TiO 2 NPs in three variable-charge soils and to determine the key factors controlling these behaviors. Materials and methods Three surface (0~15 cm) variable-charge soils derived from quaternary red clay, humid ferralsols and stagnic anthrosols collected from Yingtan, Jiangxi Province (YT-H and YT-S, respectively), and humid ferralsols collected from Fuyang, Zhejiang Province (FY-H), were used in this study. Batch sedimentation experiments of TiO 2 NPs in soil suspensions were performed for 10 h to quantify their stability. Transport of TiO 2 NPs in soil columns was conducted with and without the presence of fulvic acid (FA). Results and discussion Apart from soil organic matter (SOM) and iron oxides, there was no significant difference between the tested soils. Batch experiments showed that TiO 2 NPs were more stable in the YT-S soil suspension with high dissolved organic matter than in the YT-H and FY-H soil suspensions. In the column experiments, all TiO 2 NPs were retained in YT-H and YT-S, while 11% of the TiO 2 NPs were eluted from FY-H with a low amorphous iron oxide content. The significant retention of TiO 2 NPs in the soils could be attributed to the straining and adsorption of TiO 2 NPs on the surface of soil particles. FA enhanced the transport of TiO 2 NPs in YT-H and FY-H by dispersing the TiO 2 NPs and reducing their adsorption onto soil particles, while all the TiO 2 NPs dispersed in the FA solution were still deposited in YT-S with a high amorphous iron oxide content. Conclusions The stability of TiO 2 NPs in three variable-charge soil suspensions was dependent on the SOM. However, the mobility of TiO 2 NPs in soils was not directly related to their stability in the soil suspensions. The difference in amorphous iron oxide content could induce the disparity in mobility of TiO 2 NPs in soils.

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Speciation and sorption structure of diphenylarsinic acid in soil clay mineral fractions using sequential extraction and EXAFS spectroscopy

Cited by 8 publications

References 62 publications

Diphenylarsinic acid sorption mechanisms in soils using batch experiments and EXAFS spectroscopy

Diphenylarsinic acid sorption mechanisms in soils using batch experiments and EXAFS spectroscopy

Contrasting effects of iron reduction on thionation of diphenylarsinic acid in a biostimulated Acrisol

Stability and transport of titanium dioxide nanoparticles in three variable-charge soils

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