Electroreduction of CO_(2) to C_(2)H_(4) Regulated by Spacing Effect:Mechanistic Insights from DFT Studies  

作　　者：Xinze Bi Yifan Yan Hongzhi Wang Yuezhu Zhao Jiatao Zhang Mingbo Wu 

机构地区：[1]College of New Energy,College of Chemical Engineering,State Key Laboratory of Heavy Oil Processing,China University of Petroleum(East China),Qingdao 266580,China [2]Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications,School of Chemistry and Chemical Engineer,Beijing Institute of Technology,Beijing 100081,China

出　　处：《Energy Material Advances》2023年第1期294-303,共10页能源材料前沿（英文）

基　　金：National Natural Science Foundation of China(Grant Nos.22208377,2213000238,and 52072409);Major Scientific and Technological Innovation Project of Shandong Province(2020CXGC010402);Natural Science Foundation of Shandong Province(ZR2021QE062);Qingdao postdoctoral applied research project(qdyy20200063);Taishan Scholar Project(ts201712020).

摘　　要：It is crucial to construct an efficient catalyst with high activity and excellent selectivity for realizing CO_(2) electroreduction reaction(CO_(2)ER)to high-value-added chemicals,especially the C2 products.Density functional theory(DFT)provides a powerful tool for investigating the promotional effect on C2 selectivity of finely tuned catalyst structures,which is currently difficult to control using experimental techniques,such as interatomic distances.In the work,5 Cu_(2)O catalyst models are constructed with different Cu-Cu atomic spacing(d_(Cu-Cu)).The results of DFT calculations show that adjusting the d_(Cu-Cu) can effectively tailor the electronic structures of active sites,enhance catalytic activity,and improve product selectivity.Specifically,the Cu atom pair spaced at d_(Cu-Cu)=2.5Åcould optimize the adsorption configuration of*CO and enhance the binding strength of*CO,thus improving*CO adsorption energy and reducing the energy barrier of C-C coupling.The work proves the feasibility of spacing effect in enhancing the C_(2)H_(4) selectivity of CO_(2) ER and provides a new idea for the catalyst modification for other reactions of polyprotons-coupled electrons.

关 键 词：CATALYST SELECTIVITY SPACING 

分 类 号：O64[理学—物理化学]