Key Laboratory of High-temperature and High-pressure Study of the Earth's Interior, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, 550081, China; University of Chinese Academy of Sciences, Beijing, 100039, China.
Key Laboratory of High-temperature and High-pressure Study of the Earth's Interior, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, 550081, China.
J Hazard Mater. 2020 Jun 15;392:122502. doi: 10.1016/j.jhazmat.2020.122502. Epub 2020 Mar 10.
In situ electrochemical techniques and surface analysis were used to investigate the weathering behavior of arsenopyrite in chlorine-containing brine. Cyclic voltammetry measurements showed that arsenopyrite weathering releases S°, As (III) and Fe (II) during the initial step, even contains different concentrations of H and Cl, and terminal transformation into SO, As (V) and Fe (III), respectively. Cl ions promote the arsenopyrite weathering through diffusion control or adsorption control when Cl- ions are at low or high concentrations. When C increased from 0.00 to 0.05 mol/L, As (III) release increases from 549.33 to 1135.86 g·m·y, and the promotion efficiency is 107 %; whereas from 0.20 to 0.40 mol/L, the promotion efficiency is only 15.1 %. H ions accelerate arsenopyrite weathering for O + 4H + 4e → 2HO, and the relationship between corrosion current density (i) and pH is i = -26.54 pH + 199.75. Raman spectra confirm that corrosion produces S° and As (V) and EDX shows the passivation layers are mainly composed of elements Fe, As, S and O, while the adsorption layer are mainly composed of elements Fe, As, S and Cl. The experimental results are of great significance for arsenopyrite geological environment assess and removal of arsenic ions.
采用电化学原位技术和表面分析方法研究了含氯盐水溶液中毒砂的风化行为。循环伏安测量表明,毒砂风化在初始阶段释放 S°、As(III)和 Fe(II),即使含有不同浓度的 H 和 Cl,最终分别转化为 SO、As(V)和 Fe(III)。Cl 离子通过扩散控制或吸附控制促进毒砂风化,当 Cl-离子浓度较低或较高时。当 C 从 0.00 增加到 0.05 mol/L 时,As(III)的释放量从 549.33 增加到 1135.86 g·m·y,促进效率为 107%;而从 0.20 增加到 0.40 mol/L 时,促进效率仅为 15.1%。H 离子加速毒砂风化,O + 4H + 4e → 2HO,腐蚀电流密度(i)与 pH 值的关系为 i = -26.54 pH + 199.75。拉曼光谱证实腐蚀产生 S°和 As(V),EDX 表明钝化层主要由 Fe、As、S 和 O 元素组成,而吸附层主要由 Fe、As、S 和 Cl 元素组成。实验结果对毒砂地质环境评估和去除砷离子具有重要意义。