文献类型：期刊文献

英文题名：Synergistic Cr2O3@Ag Heterostructure Enhanced Electrocatalytic CO2 Reduction to CO

作者：Fu, Huai Qin[1];Liu, Junxian[1];Bedford, Nicholas M.[2];Wang, Yun[1];Sun, Ji Wei[3];Zou, Yu[1];Dong, Mengyang[1];Wright, Joshua[4];Diao, Hui[5];Liu, Porun[1];Yang, Hua Gui[3];Zhao, Huijun[1]

机构：[1]Griffith Univ, Ctr Catalysis & Clean Energy, Gold Coast Campus, Southport, Qld 4222, Australia;[2]Univ New South Wales, Sch Chem Engn, Sydney, NSW 2052, Australia;[3]East China Univ Sci & Technol, Sch Mat Sci & Engn, Minist Educ, Key Lab Ultrafine Mat, Shanghai 200237, Peoples R China;[4]IIT, Dept Phys, Chicago, IL 60616 USA;[5]Univ Queensland, Ctr Microscopy & Microanal, St Lucia, Qld 4072, Australia

年份：2022

卷号：34

期号：29

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20222412216364);WOS:【SCI-EXPANDED(收录号:WOS:000809072600001)】；

基金：This work was financially supported by Australian Research Council Discovery Project (DP200100965). Ag K-edge and Cr K-edge XAS measurements were performed at the 10-ID-B beamline of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility, operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Operations at 10-ID-B are further supported by members of the Materials Research Collaborative Access Team. C and O K-edge measurements were performed at the SXR beamline of the Australian Synchrotron, part of the Australian Nuclear Science and Technology Organisation.

语种：英文

外文关键词：carbon dioxide reduction; Cr2O3; Ag heterostructures; metal; metal oxides (MMO) heterostructures; synergetic promotional effect

摘要：The electrocatalytic CO2RR to produce value-added chemicals and fuels has been recognized as a promising means to reduce the reliance on fossil resources; it is, however, hindered due to the lack of high-performance electrocatalysts. The effectiveness of sculpturing metal/metal oxides (MMO) heterostructures to enhance electrocatalytic performance toward CO2RR has been well documented, nonetheless, the precise synergistic mechanism of MMO remains elusive. Herein, an in operando electrochemically synthesized Cr2O3-Ag heterostructure electrocatalyst (Cr2O3@Ag) is reported for efficient electrocatalytic reduction of CO2 to CO. The obtained Cr2O3@Ag can readily achieve a superb FECO of 99.6% at -0.8 V (vs RHE) with a high J(CO) of 19.0 mA cm(-2). These studies also confirm that the operando synthesized Cr2O3@Ag possesses high operational stability. Notably, operando Raman spectroscopy studies reveal that the markedly enhanced performance is attributable to the synergistic Cr2O3-Ag heterostructure induced stabilization of CO2 center dot-/*COOH intermediates. DFT calculations unveil that the metallic-Ag-catalyzed CO2 reduction to CO requires a 1.45 eV energy input to proceed, which is 0.93 eV higher than that of the MMO-structured Cr2O3@Ag. The exemplified approaches in this work would be adoptable for design and development of high-performance electrocatalysts for other important reactions.