Electron-deficient ZnO induced by heterointerface engineering as the dominant active component to boost CO_(2)-to-formate conversion  

作　　者：Qing Qin Zijian Li Yingzheng Zhang Haeseong Jang Li Zhai Liqiang Hou Xiaoqian Wei Zhe Wang Min Gyu Kim Shangguo Liu Xien Liu 

机构地区：[1]College of Chemical Engineering,Qingdao University of Science and Technology,Qingdao,China [2]Department of Chemistry,City University of Hong Kong,Hong Kong SAR,China [3]Department of Advanced Materials Engineering,Chung-Ang University,Anseong-si,Gyeonggi-do,Republic of Korea [4]Beamline Research Division,Pohang Accelerator Laboratory(PAL),Pohang,Republic of Korea

出　　处：《Carbon Energy》2024年第5期127-136,共10页碳能源（英文）

基　　金：National Natural Science Foundation of China,Grant/Award Number:22102079;Taishan Scholar Program of Shandong Province,China,Grant/Award Number:tsqn202211162;Natural Science Foundation of Shandong Province of China,Grant/Award Numbers:ZR2021YQ10,ZR2022QB163。

摘　　要：Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,but seldom do they exhibit excellent selectivity toward formate.In this article,we demonstrate that a heterointerface catalyst ZnO/ZnSnO3 with nanosheet morphology shows enhanced selectivity with a maximum Faradaic efficiency(FE)of 86%at−0.9 V versus reversible hydrogen electrode and larger current density for the conversion of CO_(2) to formate than pristine ZnO and ZnSnO3.In particular,the FEs of the C1 products(CO+HCOO−)exceed 98%over the potential window.The experimental measurements combined with theoretical calculations revealed that the ZnO in ZnO/ZnSnO3 heterojunction delivers the valence electron depletion and accordingly optimizes Zn d-band center,which results in moderate Zn-O hybridization of HCOO*and weakened Zn-C hybridization of competing COOH*,thus greatly boosting the HCOOH generation.Our study highlights the importance of charge redistribution in catalysts on the selectivity of electrochemical CO_(2) reduction.

关 键 词：charge redistribution CO_(2)reduction reaction ELECTROCATALYST heterointerfaces SELECTIVITY 

分 类 号：O64[理学—物理化学]