CO2在高岭石(001)晶面吸附的第一性原理计算

doi:10.7523/j.ucas.2022.005

摘要/Abstract

摘要： 吸附是封存CO₂的一种重要手段，也是降低CO₂温室效应的一种有效途径。高岭石作为主要的黏土矿物，不仅具有较大的比表面积，而且分布广，封存CO₂后不污染环境，是CO₂的天然吸附剂。基于密度泛函理论的第一性原理计算CO₂在高岭石（001）晶面的吸附，讨论吸附后的稳定构型、电子转移情况、密立根布居和分波态密度。结果表明在Top （1~3），Bridge （1~3）和Hollow （1~6）不同位点的吸附构型中，Hollow4-X构型最稳定，其吸附能为-0.41 eV。在Hollow4-X吸附构型中，CO₂的O原子与晶面的H原子形成H—O键，其中CO₂的O原子的2p轨道对成键贡献较大；高岭石（001）晶面H原子的电子转移到CO₂的O原子上。

关键词: 吸附, 高岭石, 二氧化碳, 第一性原理计算

Abstract: Adsorption is an important means of storing CO₂, and it is also an effective way to reduce the greenhouse effect caused by CO₂. Kaolinite, the main clay mineral, is one of the potential media to adsorb CO₂due to its large specific surface area, wide distribution and no pollution after CO₂ adsorption. In this paper, the first-principle calculations based on density functional theory were used to study the CO₂ adsorption on the kaolinite(001) surface. The stable configuration, electron transfer, Milliken population and partial density of states after adsorption are discussed. These results show that Hollow4-X is the most stable configuration with adsorption energy -0.41 eV in the adsorption configurations at different sites of Top(1-3), Bridge(1-3) and Hollow(1-6). In the stable adsorption configuration Hollow4-X, the hydrogen atom of the kaolinite(001) surface bonds with the oxygen atom of the CO₂, which leads to the formation of H-O bond. Moreover, the 2p orbital of the oxygen atom of CO₂ has a great contribution to the formation of H-O bond, and the electrons of the H atom of the kaolinite(001) surface transfer to the O atom of CO₂. Our calculations illustrate the mechanism of CO₂ adsorption on the kaolinite(001) surface from the atomic scale, and provide a basis for further research and utilization of kaolinite to store CO₂.

Key words: adsorption, kaolinite, CO₂, first-principle calculations

中图分类号:

P574.1

梁家新, 刘善琪, 李永兵. CO₂在高岭石(001)晶面吸附的第一性原理计算[J]. 中国科学院大学学报, 2023, 40(6): 751-760.

LIANG Jiaxin, LIU Shanqi, LI Yongbing. First-principle calculations of CO₂ adsorption on the kaolinite (001) surface[J]. Journal of University of Chinese Academy of Sciences, 2023, 40(6): 751-760.

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CO₂在高岭石(001)晶面吸附的第一性原理计算

First-principle calculations of CO₂ adsorption on the kaolinite (001) surface

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