How can the Dual-atom Catalyst FeCo-NC Surpass Singleatom Catalysts Fe-NC/Co-NC in CO_(2) RR?-CO Intermediate Assisted Promotion via a Synergistic Effect  

作　　者：Shoufu Cao Sainan Zhou Hongyu Chen Shuxian Wei Siyuan Liu Xiaojing Lin Xiaodong Chen Zhaojie Wang Wenyue Guo Xiaoqing Lu 

机构地区：[1]School of Materials Science and Engineering,China University of Petroleum,Qingdao Shandong 266580,China [2]College of Science,China University of Petroleum,Qingdao Shandong 266580,China

出　　处：《Energy & Environmental Materials》2023年第1期300-308,共9页能源与环境材料（英文）

基　　金：This work was supported by Shandong Natural Science Foundation,China(ZR2019MEM005,ZR2020ME053,and ZR2020QB027);the Major Scientific and Technological Projects of CNPC(ZD2019-184-001);the Fundamental Research Funds for the Central Universities(18CX02042A and 20CX05010A);the National Science Fund for Distinguished Young Scholars(22101300).

摘　　要：Atomically dispersed catalysts are widely adopted in CO_(2)reduction reaction(CO_(2)RR)due to maximal atomic utilization and high catalytic activity.Dual-atom catalysts(DACs),with more dispersed active sites and distinct electronic structures compared with single-atom catalysts(SACs),may exhibit diverse catalytic performance.Herein,the DAC FeCo-NC and SAC Fe-NC/Co-NC are employed as probes to explore DACs advantage in CO_(2)RR.Results show that the moderate interaction between the dual-atom center and N coordination balances structural stability and catalytic activity.CO is the only product on Fe-NC/Co-NC,and the high limiting potentials from−1.22 to−1.67 V inhibit further reduction.FeCo-NC assisted with CO intermediate exhibits low limiting potentials of−0.64 V for both CH_(3)OH and CH 4,comparable to those on Cu-based catalysts.Under circumstance of applied potentials,CO_(2)RR on FeCo-NC has greater advantages in yielding CH_(3)OH and CH 4 than that on Fe-NC/Co-NC,and hydrogen evolution reaction is severely inhibited.The intrinsic essence is that dual-atom center can provide large spin-polarization and multi-electron transfer capability,rendering CO intermediates as effective electronic and geometric modifiers in CO_(2)RR.This work highlights FeCo-NC as a high-performance CO_(2)RR catalyst toward deep-reduction C1 products and elucidates CO intermediate assisted promotion mechanism via a dual-atom synergistic effect.

关 键 词：dispersed LIMITING RENDERING 

分 类 号：O643.36[理学—物理化学]