铜
密度泛函理论
选择性
煅烧
吸附
甲烷
材料科学
二氧化碳
选择性还原
二氧化碳电化学还原
化学
纳米技术
化学物理
催化作用
碳纤维
物理化学
计算化学
一氧化碳
复合数
有机化学
复合材料
冶金
作者
Qi Hu,Zhen Han,Xiaodeng Wang,Guomin Li,Ziyu Wang,Xiaowan Huang,Hengpan Yang,Xiangzhong Ren,Qianling Zhang,Jianhong Liu,Chuanxin He
标识
DOI:10.1002/anie.202009277
摘要
Previous density-functional theory (DFT) calculations show that sub-nanometric Cu clusters (i.e., 13 atoms) favorably generate CH4 from the CO2 reduction reaction (CO2 RR), but experimental evidence is lacking. Herein, a facile impregnation-calcination route towards Cu clusters, having a diameter of about 1.0 nm with about 10 atoms, was developed by double confinement of carbon defects and micropores. These Cu clusters enable high selectivity for the CO2 RR with a maximum Faraday efficiency of 81.7 % for CH4 . Calculations and experimental results show that the Cu clusters enhance the adsorption of *H and *CO intermediates, thus promoting generation of CH4 rather than H2 and CO. The strong interactions between the Cu clusters and defective carbon optimize the electronic structure of the Cu clusters for selectivity and stability towards generation of CH4 . Provided here is the first experimental evidence that sub-nanometric Cu clusters facilitate the production of CH4 from the CO2 RR.
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