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过程工程学报 ›› 2021, Vol. 21 ›› Issue (7): 836-846.DOI: 10.12034/j.issn.1009-606X.220175

• 过程与工艺 • 上一篇    下一篇

盐酸在黄铜矿表面吸附机制的第一性原理计算

李小亮1,2， 田国才1,2*   

  1. 1. 昆明理工大学省部共建复杂有色金属资源清洁利用国家重点实验室，云南昆明650093
    2. 昆明理工大学冶金与能源工程学院，云南昆明650093
  • 收稿日期:2020-06-08 修回日期:2020-09-03 出版日期:2021-07-28 发布日期:2021-07-27
  • 通讯作者: 田国才 tiangc01@163.com
  • 基金资助:
    燃煤超细微粒的生成与控制机理研究;云南省中青年学术技术带头人后备人才培养项目

First-principles calculation of adsorption mechanism of hydrochloric acid on chalcopyrite surface

Xiaoliang LI1,2, Guocai TIAN1,2*   

  1. 1. State Key Laboratory of Complex Non-ferrous Metal Resource Clean Utilization, Kunming University of Science and Technology,
    Kunming, Yunnan 650093, China
    2. Faculty of Metallurgy and Energy Engineering, Kunming University of Science and Technology, Kunming, Yunnan 650093, China
  • Received:2020-06-08 Revised:2020-09-03 Online:2021-07-28 Published:2021-07-27

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摘要： 采用第一性原理对盐酸在黄铜矿表面不同位点的吸附及反应机理进行研究。结果表明，黄铜矿(001)-S表面重构后形成了二硫化物S22?。盐酸以解离形式在黄铜矿的(001)硫终止面(001)-S上吸附，浸出过程中H+在黄铜矿(001)-S表面上S位点的吸附都会破坏黄铜矿表面所形成的S22-。Cl-的吸附对黄铜矿(001)-S表面结构也会造成一定的破坏，吸附过程中H+和Cl-与黄铜矿表面发生化学反应生成了FeCl2和H2S，这些都有利于黄铜矿的浸出。

关键词: 黄铜矿, 盐酸, 表面吸附, 第一性原理

Abstract: The leaching of chalcopyrite has always been the core of copper sulfide hydrometallurgy, but chalcopyrite is a sulfide mineral that is difficult to be oxidized and decomposed. At present, a large number of macroscopic phenomena are obtained by focusing on experimental research, and the mechanism is mostly inferred. However, the lack of information on atomic or molecular level hinders the clear and effective explanation to these macroscopic phenomena. Therefore, it is necessary to study the surface interaction between liquid medium and chalcopyrite and the influence of medium on the formation of surface products by means of atomic or molecular level calculation and analysis, which are of great significance to reveal the reaction mechanism of leaching process and improve or develop a green hydrometallurgical technology of chalcopyrite. As a common leaching agent, hydrochloric acid can be used in the leaching of chalcopyrite, and it has been widely studied because of its advantages of recyclable leaching agent, high solubility of metal ions, good oxidation reduction performance and fast leaching rate. In this work, the adsorption and reaction mechanism of hydrochloric acid on different sites of chalcopyrite surface were studied with first-principles calculation. It was shown that the reconstructed sulfur terminated chalcopyrite (001) surface [labeled as (001)-S surface] led to the formation of disulphide S22-. Hydrochloric acid was adsorbed on the sulfur terminated surface (001)-S of chalcopyrite in the form of dissociation. In the process of leaching, the adsorption of H+ on sulfur terminated surface (001)-S of chalcopyrite destroyed the S22- formed on the surface. The surface structure of chalcopyrite (001)-S was destroyed by adsorption of chloride ion Cl-. During the adsorption process, the chemical reactions between H+ and Cl- with the surface of chalcopyrite produce the FeCl2 and H2S, which were both beneficial to the leaching of chalcopyrite. The results can provide a theoretical basis and guidance for future research.

Key words: chalcopyrite, hydrochloric acid, surface adsorption, the first principles