Cu纳米粒催化CO_(2)还原反应机理的理论研究

Theoretical study on the mechanism of CO_(2)reduction catalyzed by Cu nanoparticles

此文采用密度泛函理论,研究了Cu_(38)纳米粒催化剂模型,分别研究了CO_(2)和H_(2)O分子在催化剂上不同吸附位,确了稳定的吸附构型,并进一步研究了CO_(2)催化还原反应机理,确定催化剂的活性.本文主要研究催化CO_(2)还原生成CO_(2)过程,研究了两条可行的反应路径,路径I为水分子的H原子直接转移到CO_(2)上,路径II为H原子先迁移到Cu_(38)纳米粒上再转移到CO_(2)上,研究结果发现此步反应机理路径I优先.从微观角度解释了实验研究结果.

In this paper,the Cu_(38) nanoparticle catalyst model was studied by using density functional theory,the different adsorption sites of CO_(2) and H_(2)O molecules on the catalyst were studied respectively,the stable adsorption configuration was determined,the mechanism of CO_(2) catalytic reduction was further studied,and the activity of the catalyst was determined.This paper mainly studies the process of catalytic CO_(2) reduction to CO and two feasible reaction paths.Path I is the direct transfer of H atom of water molecule to CO_(2),and path II is the first transfer of H atom to Cu_(38) nanoparticles and then to CO_(2).The results show that the reaction mechanism path I is preferred.The experimental results are explained from the microscopic point of view.