【摘要】 为探究吸附法捕获CO₂过程中的微观机理和吸附剂材料间的作用关系，基于密度泛函理论方法，综合比较了典型吸附剂包括煤基官能团、Fe、限域离子液体、Na₂CO₃、SrTiO₃与CO₂的吸附过程和差异性.根据不同计算策略，着重分析比较了吸附能、结构优化参数、吸附构型以及原子分布等参数.结果表明，化学吸附中CO₂分子与吸附面呈平行关系时通常吸附能最大；在一种材料的同类型官能团中，吸附能大小与氧原子的数量呈正相关关系；吸附过程中C-O键的伸长活化会生成一种重要的中间产物CO₂^-.提出在探寻CO₂吸附材料时可以在含氧原子较多的官能团、活性金属表面等方面进一步探究.最后对基于密度泛函理论的CO₂的吸附机理的进一步研究方向进行了展望.更多还原

【Abstract】 In order to investigate the microscopic mechanism and the relationship between adsorbent materials in the process of CO₂ capture by adsorption, the adsorption processes and differences between typical adsorbents including coal-based functional groups, Fe, restricted ionic liquids, Na₂CO₃ and SrTiO₃ with CO₂ were compared based on the density flooding theory approach. According to different calculation strategies, the parameters of adsorption energy, structural optimization parameters, adsorption configuration and atomic distribution are analyzed and compared. The results show that the adsorption energy is usually highest when the CO₂ molecule is parallel to the adsorption surface in chemisorption; the adsorption energy is positively correlated with the number of oxygen atoms in the same type of functional group of a material; and the elongation activation of the C-O bond during adsorption produces an important intermediate product CO₂^-. It is proposed that the search for CO₂ adsorption materials can be further explored in terms of functional groups containing more oxygen atoms and reactive metal surfaces. Finally, further research on the adsorption mechanism of CO₂ based on density functional theory has been expected in this paper.更多还原