In-situ electrochemical study on the effects of Fe(III) on kinetics of pyrite acidic pressure oxidation

IF 1.4 4区 地球科学 Q3 GEOCHEMISTRY & GEOPHYSICS Acta Geochimica Pub Date : 2024-04-17 DOI:10.1007/s11631-024-00685-3
Yu Zhang, Can Cui, Sen Lin, Heping Li, Lian Yang, Yadian Xie, Hailiang Hu, Lingyun Zhou, Huanjiang Wang, Chunyan Li
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Abstract

Fe(III) has been proved to be a more effective oxidant than dissolved oxygen at ambient temperature, however, the role of Fe(III) in pyrite acidic pressure oxidation was rarely discussed so far. In this paper, in-situ electrochemical investigation was performed using a flow-through autoclave system in acidic pressure oxidation environment. The results illustrated that increasing Fe(III) concentrations led to raising in redox potential of the solution, and decreased passivation of pyrite caused by deposition of elemental sulfur. Reduction of Fe(III) at pyrite surface was a fast reaction with low activation energy, it was only slightly promoted by rising temperatures. While, the oxidation rate of pyrite at all investigated Fe(III) concentrations increased obviously with rising temperatures, the anodic reaction was the rate-limiting step in the overall reaction. Activation energy of pyrite oxidation decreased from 47.74 to 28.79 kJ/mol when Fe(III) concentration was increased from 0.05 to 0.50 g/L, showing that the reaction kinetics were limited by the rate of electrochemical reaction at low Fe(III) concentrations, while, it gradually turned to be diffusion control with increasing Fe(III) concentrations.

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铁(III)对黄铁矿酸性压力氧化动力学影响的原位电化学研究
事实证明,在常温下,Fe(III)是比溶解氧更有效的氧化剂,但迄今为止,Fe(III)在黄铁矿酸性压力氧化中的作用还很少被讨论。本文在酸性压力氧化环境下,使用流动高压釜系统进行了原位电化学研究。结果表明,Fe(III) 浓度的增加会导致溶液氧化还原电位的升高,元素硫的沉积会降低黄铁矿的钝化。黄铁矿表面的铁(III)还原反应速度快,活化能低,只有在温度升高时才稍有促进作用。在所有研究的铁(III)浓度下,黄铁矿的氧化速率都随着温度的升高而明显增加,阳极反应是整个反应的限速步骤。当铁(III)浓度从 0.05 g/L 增加到 0.50 g/L 时,黄铁矿氧化的活化能从 47.74 kJ/mol 下降到 28.79 kJ/mol,这表明反应动力学在低铁(III)浓度时受到电化学反应速率的限制,而随着铁(III)浓度的增加,反应动力学逐渐转为扩散控制。
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来源期刊
Acta Geochimica
Acta Geochimica GEOCHEMISTRY & GEOPHYSICS-
CiteScore
2.80
自引率
6.20%
发文量
1134
期刊介绍: Acta Geochimica serves as the international forum for essential research on geochemistry, the science that uses the tools and principles of chemistry to explain the mechanisms behind major geological systems such as the Earth‘s crust, its oceans and the entire Solar System, as well as a number of processes including mantle convection, the formation of planets and the origins of granite and basalt. The journal focuses on, but is not limited to the following aspects: • Cosmochemistry • Mantle Geochemistry • Ore-deposit Geochemistry • Organic Geochemistry • Environmental Geochemistry • Computational Geochemistry • Isotope Geochemistry • NanoGeochemistry All research articles published in this journal have undergone rigorous peer review. In addition to original research articles, Acta Geochimica publishes reviews and short communications, aiming to rapidly disseminate the research results of timely interest, and comprehensive reviews of emerging topics in all the areas of geochemistry.
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