4.7 Article

Partitioning and transformation behavior of arsenic during Fe(III)-As(III)-As(V)-SO42- coprecipitation and subsequent aging process in acidic solutions: Implication for arsenic mobility and fixation

期刊

SCIENCE OF THE TOTAL ENVIRONMENT
卷 799, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.scitotenv.2021.149474

关键词

Arsenite; Arsenate; Sulfate; Coprecipitation; Transformation; Ferric arsenate; Scorodite

资金

  1. National Key Research and Development Program of China [2020YFC1807800]
  2. National Natural Science Foundation of China [41877393, 41530643]
  3. Liao Ning Revitalization Talents Program [XLYC1807185, XLYC1807025]

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The coprecipitation and aging of Fe(III)-As(III)-As(V)-SO4(2-) in acidic systems play a crucial role in controlling arsenic behavior. The study investigates the redistribution and transformation of arsenic in the system at different Fe/As molar ratios and pH values. Results show that As(III) contents in the solid products change with aging time and conditions, indicating the complex behavior of arsenic in the system.
The coprecipitation and subsequent aging of Fe(III)-As(III)-As(V)-SO42- play an important role in controlling As behavior in acidic systems, such as acid mine drainage and hydrometallurgical acid waste. In this study, we investigated the redistribution and transformation of As in the Fe(III)-As(III)-As(V)-SO42- system (As(III)/As(V) approximate to 1) at different Fe/As molar ratios (i.e., 0.25. 0.5, and 1) and pH (12 and 1.8) at 60 degrees C. The results showed that As(Ill) and SO42- can be incorporated into the amorphous ferric arsenate and scorodite host phases by forming a Fe(AsO4)(x)(AsO3)(y)(SO4)(z) solid solution. As(III) contents in the freshly coprecipitated solids increased with pH and initial As(III) concentrations. During aging process, As(III) contents in the solid products with Fe/As molar ratios of 0.5 and 1 increased with aging time at pH 1.8. In contrast, As(III) was gradually expelled from aging products with aging time at pH 1.2, regardless of Fe/As molar ratio. X-ray diffraction (XRD), scanning electron microscopy (SEM), attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), and Raman spectroscopy characterization results showed that an As(III)-SO42--doped scorodite was formed at Fe/As molar ratio <= 0.5 during the aging process. It was also found that As(III) had an inhibitory effect on the transformation of poorly crystalline ferric arsenate to scorodite. The present study may have important implications for understanding the geochemical cycle of As, Fe, and SO42- in acidic solutions and give further understanding on the mechanisms involved in As removal and fixation in hydrometallurgical unit operations. (C) 2021 Elsevier B.V. All rights reserved.

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