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Facile Synthesis of Sub‐Nanometric Copper Clusters by Double Confinement Enables Selective Reduction of Carbon Dioxide to Methane
Author(s) -
Hu Qi,
Han Zhen,
Wang Xiaodeng,
Li Guomin,
Wang Ziyu,
Huang Xiaowan,
Yang Hengpan,
Ren Xiangzhong,
Zhang Qianling,
Liu Jianhong,
He Chuanxin
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202009277
Subject(s) - density functional theory , selectivity , copper , calcination , carbon fibers , adsorption , materials science , chemistry , chemical physics , nanotechnology , computational chemistry , catalysis , composite number , organic chemistry , composite material , metallurgy
Previous density‐functional theory (DFT) calculations show that sub‐nanometric Cu clusters (i.e., 13 atoms) favorably generate CH 4 from the CO 2 reduction reaction (CO 2 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 CO 2 RR with a maximum Faraday efficiency of 81.7 % for CH 4 . Calculations and experimental results show that the Cu clusters enhance the adsorption of *H and *CO intermediates, thus promoting generation of CH 4 rather than H 2 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 CH 4 . Provided here is the first experimental evidence that sub‐nanometric Cu clusters facilitate the production of CH 4 from the CO 2 RR.