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
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
• 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.
Magnetic iron nanoparticles modified microfibrillated cellulose
[As(V)] = 50.9
0.957
51.307
0.005
319.823
Hokkanen et al., 2015
Lignin-based magnetic activated carbon
[p-AsA] = 50
0.9928
227.27
Wu et al., 2020
[ROX] = 50
0.9558
42.36
[PAA] = 50
0.9491
40.12
Tab.2
Fig.3
Fig.4
Fig.5
Fig.6
Sample
Path
CNb
Rc (Å)
ΔE0d (eV)
σ2e (Å2)
R factorf
Initial pH
Reference
Magnetite/ DPAA
As-O
2.0
1.69
10.9
0.0030
0.0084
6.0
This work
As-C1
2.0
1.89
–
0.0344
As-C2
4.0
2.79
–
0.0344
As-C3
4.0
4.31
–
0.0344
As-C4
2.0
4.73
–
0.0344
As-Fe
1.85
3.33
–
0.0030
Siderite/ DPAA
As-O
2.0
1.68
4.9
0.0030
0.0076
6.0
This work
As-C1 As-C2 As-C3 As-C4 As-Fe
2.0 4.0 4.0 2.0 1.11
1.89 2.79 4.31 4.72 3.27
– –
0.0030 0.0030 0.0030 0.0030 0.0030
Ferrihydrite/ DPAA
As-O
2.0
1.69
4.8
0.0012
4.0
Tanaka et al., 2014
As-C1
2.0
1.89
–
0.0020
As-C2
4.0
2.86
–
0.0026
As-C3
4.0
4.36
–
0.0048
As-C4
2.0
4.75
–
0.0027
As-Fe1
2.1
3.27
–
0.0076
As-Fe2
0.8
3.46
–
0.0076
Tab.3
Fig.7
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