Influences and Mechanisms of As(V) Concentration and Environmental Factors on Hydrosulfate Green Rust Transformation

doi:10.6023/A17020046

Acta Chim. Sinica ›› 2017, Vol. 75 ›› Issue (6): 608-616.DOI: 10.6023/A17020046 Previous Articles Next Articles

Special Issue: 铁环境化学

Article

As(V)浓度和环境因子对硫酸盐绿锈转化的影响及其机制

王小明^a, 彭晶^a, 徐欢欢^a, 谭文峰^a, 刘凡^a, 黄巧云^a,b, 冯雄汉^a

a 华中农业大学资源与环境学院农业部长江中下游耕地保育重点实验室武汉 430070;
b 华中农业大学农业微生物国家重点实验室武汉 430070

投稿日期:2017-02-09 发布日期:2017-04-12
通讯作者: 冯雄汉 E-mail:fxh73@mail.hzau.edu.cn
基金资助:
项目受中国博士后科学基金（No.2016M590700）和国家自然科学基金（Nos.41601228，41471194）资助.

Influences and Mechanisms of As(V) Concentration and Environmental Factors on Hydrosulfate Green Rust Transformation

Wang Xiaoming^a, Peng Jing^a, Xu Huanhuan^a, Tan Wenfeng^a, Liu Fan^a, Huang Qiaoyun^a,b, Feng Xionghan^a

a Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture, College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China;
b State Key Laboratory of Agricultural Microbiology, Huazhong Agricultural University, Wuhan 430070, China

Received:2017-02-09 Published:2017-04-12
Contact: 10.6023/A17020046 E-mail:fxh73@mail.hzau.edu.cn
Supported by:
Project supported by the China Postdoctoral Science Foundation (No. 2016M590700) and National Natural Science Foundation of China (Nos. 41601228, 41471194).

1. Influences and Mechanisms of As(V) Concentration and Environmental Factors on Hydrosulfate Green Rust Transformation.PDF(2170KB)

Abstract

Green rusts can coexist with As(V) in some anoxic environments, such as soils, sediments, and groundwater, the interaction between them will affect the transformation of green rusts and the environmental behaviors of As(V), but the influences of As(V) on the processes and mechanisms of green rust transformation have not been fully understood. In this study, the effects of As(V) concentration, pH, temperature, and air rate on hydrosulfate green rust (GR2(SO₄^2-), GR) transformation have been systematically studied by solution chemistry methods combined with spectroscopic analysis, including synchrotron based X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and As K-edge X-ray absorption near edge structure (XANES) spectroscopy. GR shows extremely strong removal capability of As(V) via adsorption and co-precipitation during its transformation, meanwhile the presence of As(V) increases the stability of GR and significantly affects the crystallinity and phases of the transformation products and the transformation mechanisms. With increasing the As(V) concentration (0~20 mmol/L As) at pH 7.3 and 25℃ under open and stirring conditions, the mechanisms change from dissolution-oxidation-precipitation (DOP) to solid state oxidation (SSO), and the transformation products of GR change from mixed phases of goethite and lepidocrocite to pure lepidocrocite to mixed phases of poorly crystalline lepidocrocite, ferrihydrite, and ferric GR, and their crystallinity gradually decreases. The transformation processes of GR exhibit strong accumulation capability towards As(V), leading to the formation of amorphous FeAsO₄ surface precipitation at high As(V) concentrations (Fe/As molar ratio<24). When the molar ratio of Fe/As=24, lepidocrocite is the main product at the conditions of pH 6.5~9, temperature of 5~45℃, and air rate of 0~0.05 m³/h, its crystallinity decreases with increasing pH and air rate or decreasing temperature. High pH and air rate, and low temperature favors the formation of ferric GR (same structure with GR but only contains Fe(Ⅲ)) and ferrihydrite, while high temperature favors the formation of goethite. These new insights provide important implications for understanding the formation and transformation mechanisms of various iron oxides and the environmental behaviors of As(V).

Key words: green rust, As(V), pH, temperature, air rate, transformation

Cite this article

Wang Xiaoming, Peng Jing, Xu Huanhuan, Tan Wenfeng, Liu Fan, Huang Qiaoyun, Feng Xionghan. Influences and Mechanisms of As(V) Concentration and Environmental Factors on Hydrosulfate Green Rust Transformation[J]. Acta Chim. Sinica, 2017, 75(6): 608-616.

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As(V)浓度和环境因子对硫酸盐绿锈转化的影响及其机制

Influences and Mechanisms of As(V) Concentration and Environmental Factors on Hydrosulfate Green Rust Transformation

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