镍
密度泛函理论
二氧化碳电化学还原
碳纤维
石墨氮化碳
材料科学
氢
分子
化学
电子转移
光化学
计算化学
催化作用
有机化学
光催化
复合材料
复合数
一氧化碳
作者
Jihuai Wu,Guanqi Wang,Qizhen Liu,Yang Ling,Ruitao Zhang,Ningchao Sun,Yingchao Gao,Zhihao Chen,Yijing Sun,Yunfei Gao
摘要
Abstract In many photocatalytic reaction paths, the breaking of the first CO bond in a CO 2 molecule is often the key step that becomes the rate‐controlled reaction step. In this paper, a graphitic carbon nitride (g‐C 3 N 4 ) supported nickel single‐atom catalyst (Ni@g‐C 3 N 4 ) was successfully constructed, and the mechanism of CO 2 catalytic reduction was systematically studied based on density functional theory (DFT). The introduction of nickel promotes the adsorption of small molecules, especially for the CO 2 activation. According to density of states (DOS) and frontier orbital analysis, the photogenerated carriers tend to jump from nitrogen atoms to carbon atoms, forming an electron transfer in real space, after g‐C 3 N 4 is excited by light. With the appearance of nickel‐doped levels, the DOS of Ni@g‐C 3 N 4 is no longer symmetric with respect to the spin up and down, especially around the original band gap of g‐C 3 N 4 . Single‐atom nickel has abundant frontier orbitals and high activity and is a favourable place for chemical reactions. The presence of surface hydrogen can promote the recovery of CO 2 , and the energy barrier of Ni@g‐C 3 N 4 with hydrogen is only 15% of the clean g‐C 3 N 4 surface. This paper provides a new idea for the development of efficient single‐atom catalysts for CO 2 reduction.
科研通智能强力驱动
Strongly Powered by AbleSci AI