文献类型：期刊文献

英文题名：In Operando Identification of In Situ Formed Metalloid Zincδ+ Active Sites for Highly Efficient Electrocatalyzed Carbon Dioxide Reduction

作者：Zhang, Xin Yu[1];Li, Wen Jing[1];Chen, Jiacheng[2];Wu, Xue Feng[1];Liu, Yuan Wei[1];Mao, Fangxin[1];Yuan, Hai Yang[1];Zhu, Minghui[2];Dai, Sheng[3];Wang, Hai Feng[4];Hu, P.[4,5];Sun, Chenghua[6];Liu, Peng Fei[1];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai Engn Res Ctr Hierarch Nanomat, Key Lab Ultrafine Mat,Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Key Lab Adv Mat & Feringa Nobel Prize,Scientist J, 130 Meilong Rd, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Ctr Computat Chem & Res Inst Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland;[6]Swinburne Univ Technol, Ctr Translat Atomat, Dept Chem & Biotechnol, Hawthorn, Vic 3122, Australia

年份：2022

卷号：61

期号：28

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20221912088742);WOS:【SCI-EXPANDED(收录号:WOS:000792448900001)】；

基金：This work was financially supported by the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), the National Natural Science Funds for Distinguished Young Scholars (51725201), the Innovation Program of Shanghai Municipal Education Commission (E00014), the National Natural Science Foundation of China (51902105, 21902048, 52103340), the Science and Technology Commission of Shanghai Municipality (21DZ1207101, 19YF1411600, 20QA1402400), the National Postdoctoral Program for Innovative Talents (BX20190113), and the 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. The authors also thank the crew of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF) and the 1W1B beamline of Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analyses.

语种：英文

外文关键词：CO2 Reduction Reaction; EA Global Optimization Method; Metalloid Zn8+; Operando EXAFS; Zinc Pyrophosphate

摘要：Electrochemical CO2-to-CO conversion provides a possible way to address problems associated with the greenhouse effect; however, developing low-cost electrocatalysts to mediate high-efficiency CO2 reduction remains a challenge on account of the limited understanding of the nature of the real active sites. Herein, we reveal the Zn delta+ metalloid sites as the real active sites of stable nonstoichiometric ZnOx structure derived from Zn2P2O2 through operando X-ray absorption fine structure analysis in conjunction with evolutionary-algorithm-based global optimization. Furthermore, theoretical and experimental results demonstrated that Zn delta+ metalloid active sites could facilitate the activation of CO2 and the hydrogenation of *CO2, thus accelerating the CO2-to-CO conversion. Our work establishes a critical fundamental understanding of the origin of the real active center in the zinc-based electrocatalysts for CO2 reduction reaction.