Sorption mechanisms of diphenylarsinic acid on natural magnetite and siderite: Evidence from sorption kinetics, sequential extraction and extended X-ray absorption fine-structure spectroscopy analysis

doi:10.1007/s11783-022-1547-2

Front. Environ. Sci. Eng.

2022, Vol. 16

Issue (9) : 115 https://doi.org/10.1007/s11783-022-1547-2

RESEARCH ARTICLE

Sorption mechanisms of diphenylarsinic acid on natural magnetite and siderite: Evidence from sorption kinetics, sequential extraction and extended X-ray absorption fine-structure spectroscopy analysis

Meng Zhu^1,^3,^4,⁵, Yuhuan He¹, Xiaobao Wei¹, Haoran Qi¹, Yunpeng Zhang¹, Yijun Zhang¹, Ruyi Yang^1,^4,⁵, Yongming Luo^2,^3,⁴(

)

¹. School of Ecology and Environment, Anhui Normal University, Wuhu 241002, China
². Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China
³. Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003, China
⁴. Anhui Provincial Engineering Laboratory of Water and Soil Pollution Control and Remediation, Anhui Normal University, Wuhu 241002, China
⁵. Center of Cooperative Innovation for Recovery and Reconstruction of Degraded Ecosystem in Wanjiang City Belt, Anhui Normal University, Wuhu 241002, China

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Abstract

• DPAA sorption followed pseudo-secondary and intra-particle diffusion models.

• Chemical bonding and intra-particle diffusion were dominant rate-limiting steps.

• DPAA simultaneously formed inner- and outer-sphere complexes on siderite.

• DPAA predominantly formed occluded inner-sphere complexes on magnetite.

• Bidentate binuclear bond was identified for DPAA on siderite and magnetite.

Diphenylarsinic acid (DPAA) is both the prime starting material and major metabolite of chemical weapons (CWs). Because of its toxicity and the widespread distribution of abandoned CWs in burial site, DPAA sorption by natural Fe minerals is of considerable interest. Here we report the first study on DPAA sorption by natural magnetite and siderite using macroscopic sorption kinetics, sequential extraction procedure (SEP) and microscopic extended X-ray absorption fine-structure spectroscopy (EXAFS). Our results show that the sorption pseudo-equilibrated in 60 minutes and that close to 50% and 20%–30% removal can be achieved for magnetite and siderite, respectively, at the initial DPAA concentrations of 4–100 mg/L. DPAA sorption followed pseudo-secondary and intra-particle diffusion kinetics models, and the whole process was mainly governed by intra-particle diffusion and chemical bonding. SEP and EXAFS results revealed that DPAA mainly formed inner-sphere complexes on magnetite (>80%), while on siderite it simultaneously resulted in outer-sphere and inner-sphere complexes. EXAFS analysis further confirmed the formation of inner-sphere bidentate binuclear corner-sharing complexes (²C) for DPAA. Comparison of these results with previous studies suggests that phenyl groups are likely to impact the sorption capacity and structure of DPAA by increasing steric hindrance or affecting the way the central arsenic (As) atom maintains charge balance. These results improve our knowledge of DPAA interactions with Fe minerals, which will help to develop remediation technology and predict the fate of DPAA in soil-water environments.

Keywords Diphenylarsinic acid (DPAA) Sorption Magnetite Siderite Sequential extraction EXAFS

Corresponding Author(s): Yongming Luo

About author:

Tongcan Cui and Yizhe Hou contributed equally to this work.

Issue Date: 24 January 2022

Cite this article:

Meng Zhu,Yuhuan He,Xiaobao Wei, et al. Sorption mechanisms of diphenylarsinic acid on natural magnetite and siderite: Evidence from sorption kinetics, sequential extraction and extended X-ray absorption fine-structure spectroscopy analysis[J]. Front. Environ. Sci. Eng., 2022, 16(9): 115.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-022-1547-2
https://academic.hep.com.cn/fese/EN/Y2022/V16/I9/115

Fig.1 X-ray diffraction (XRD) (a, M represents magnetite and S represents siderite) and scanning electron microscope (SEM) images of magnetite (b) and siderite (c).

Tab.1 Properties of magnetite and siderite

Fig.2 DPAA sorption kinetics on magnetite (a) and siderite (b) and modeling the sorption envelop using the pseudo-second-order rate equation (sorbent dosage: 25 g/ L; initial DPAA concentrations: 4, 10, 20 and 100 mg/L; initial pH: 6.0; temperature: 25 °C). All results are expressed as mean±standard deviation, n = 2.

Tab.2 Kinetic parameters for DPAA, inorganic and phenyl arsenic sorption on magnetite and siderite

Fig.3 Pseudo-second-order sorption kinetics of DPAA on natural magnetite (a) and siderite (b) at various initial concentrations. Slopes and intercepts of the graphs were used to determine sorption rate constant K_f, and amount of DPAA sorbed in equilibrium Q_e. All results are expressed as means of duplicate samples.

Fig.4 Intra-particle diffusion linear plots of DPAA sorption kinetic data on natural magnetite (a) and siderite (b) based on the Weber-Morris model. According to this model, the plot of Q_t against t^0.5 should yield a straight line if intra-particle diffusion is the only rate-limiting step, whereas the sorption is controlled by multi-steps (Weber and Morris, 1963). All results are expressed as mean±standard deviation, n = 2.

Fig.5 Sequential extraction procedure applied to sorbed DPAA on magnetite (a) and siderite (b). All results are expressed as mean±standard deviation (n = 2) and presented as percentage (%) of the total extracted DPAA concentration present in the spiked minerals.

Fig.6 Arsenic K-edge XAFS data for DPAA-sorbed magnetite and siderite: XANES data (a), k³-weighted χ(k) EXAFS (b) and Fourier transformed spectra (c) (initial DPAA concentration: 100 mg/L) and molecular configurations of DPAA on Fe₂(OH)₂(H₂O)₈ (d). Experimental and calculated spectra are displayed as solid and dotted lines, respectively. O atoms are red-colored, As atoms are yellow-colored, Fe atoms are blue-colored, C atoms are gray-colored and H atoms are white-colored. The XANES data of DPAA were extracted from Zhu et al. (2019).

Tab.3 EXAFS parameters for DPAA sorption in this work and reference ^a

Fig.7 Partial k³-weighted χ(k) EXAFS functions of first (a), second and third (b) shells for DPAA-sorbed magnetite and siderite. Fourier back-transformed data were obtained using a Hanning window between 1.1 and 2.3 for the first-shell peak and between 2.3 and 3.7 for the second- and third-shell peaks. Experimental and calculated spectra are displayed as solid and dotted lines, respectively.

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