文献类型：期刊文献

英文题名：Molecularly Distorted Local Structure in Bi2CuO4 Oxide to Stabilize Lattice Oxygen for Efficient Formate Electrosynthesis

作者：Liu, Yuanwei[1,2];Lou, Zhen Xin[1];Wu, Xuefeng[1];Mei, Bingbao[3];Chen, Jiacheng[4];Zhao, Jia Yue[1];Li, Ji[2];Yuan, Hai Yang[1];Zhu, Minghui[4];Dai, Sheng[5,6];Sun, Chenghua[7];Liu, Peng Fei[1];Jiang, Zheng[2,3];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[3]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Key Lab Adv Mat, Sch Chem & Mol Engn, Inst Fine Chem, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Inst Fine Chem, Shanghai 200237, Peoples R China;[7]Swinburne Univ Technol, Ctr Translat Atomat, Dept Chem & Biotechnol, Hawthorn, Vic 3122, Australia

年份：2022

卷号：34

期号：39

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20223612696738);WOS:【SCI-EXPANDED(收录号:WOS:000848250600001)】；

基金：Y.L. and Z.X.L. contributed equally to this work. This work was financially supported by National Natural Science Funds for Distinguished Young Scholars (51725201), International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), Innovation Program of Shanghai Municipal Education Commission (E00014), the Science and Technology Commission of Shanghai Municipality (21DZ1207101, 22ZR1416400), the National Natural Science Foundation of China (51902105, 21902048) and Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400). Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry, and the crew of BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF) and 1W1B beamline at the Beijing Synchrotron Radiation Facility (BSRF) for the constructive assistance in the XAFS measurements and data analysis.

语种：英文

外文关键词：Bi; 2CuO; (4); carbon dioxide reduction; formate; lattice oxygen; local distortion

摘要：The electrochemical CO2 reduction reaction (CO2RR) provides an economically feasible way for converting green energy into valuable chemical feedstocks and fuels. Great progress has been achieved in the understanding and synthesis of oxidized-based precatalysts; however, their dynamical changes of local structure under operando conditions still hinder their further applications. Here a molecularly distorted Bi2CuO4 precatalyst for efficient CO2-to-formate conversion is reported. X-ray absorption fine structure (XAFS) results and theoretical calculations suggest that the distorted structure with molecularly like [CuO4](6-) unit rotation is more conducive to the structural stability of the sample. Operando XAFS and scanning transmission electron microscopy (STEM) results prove that quite a bit of lattice oxygen can remain in the distorted sample after CO2RR. Electrochemical measurements of the distorted sample show an excellent activity and selectivity with a high formate partial current density of 194.6 mA cm(-2) at an extremely low overpotential of -400 mV. Further in situ surface-enhanced infrared absorption spectroscopy (SEIRAS) and density functional theory (DFT) calculations illustrate that the retained oxygen can optimize the adsorption of *OCHO intermediate for the enhanced CO2RR performance.