文献类型：期刊文献

英文题名：Elucidating the roles of grain boundary and facet in electrochemical CO2 reduction

作者：Yuan, Qing[1,2];Wang, Xiaoyuan[3];Wu, Guangze[3];Li, Linfeng[3];Yang, Xiaoju[1,2];Zhang, Li[1,2];Zhang, Qiao[4];Wei, Zhiming[4];Zhai, Yueming[4];Xuan, Fu-Zhen[3];Zhai, Yanling[5,6];Zhang, Bowei[3];Yang, Xuan[1,2]

机构：[1]Huazhong Univ Sci & Technol, Key Lab Mat Chem Energy Convers & Storage, Wuhan 430074, Peoples R China;[2]Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Key Lab Bioinorgan Chem & Mat Med, Wuhan 430074, Peoples R China;[3]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai Key Lab Intelligent Sensing & Detect Tech, Shanghai 200237, Peoples R China;[4]Wuhan Univ, Inst Adv Studies, Wuhan 430072, Peoples R China;[5]Qingdao Univ, Inst Hybrid Mat, Coll Mat Sci & Engn, Coll Chem & Chem Engn, Qingdao 266071, Peoples R China;[6]Qingdao Univ, Inst Mol Metrol, Coll Chem & Chem Engn, Qingdao 266071, Peoples R China

年份：2026

卷号：19

期号：8

外文期刊名：NANO RESEARCH

收录：;EI(收录号：20263121207038);Scopus(收录号：2-s2.0-105046009310);WOS:【SCI-EXPANDED(收录号:WOS:001796878000008)】；

基金：Q. Y., X. J. Y., L. Z., and X. Y. acknowledge the financial support from the National Natural Science Foundation of China (Nos. 22204054, 22422405, and 224B2402), the HUST Academic Frontier Youth Team grant (No. 2019QYTD11), Knowledge Innovation Program of Wuhan-Shuguang, and Wuhan Talented Youth Program. X. Y. W., G. Z. W., L. F. L., F.-Z. X., and B. W. Z. thank the support from the National Natural Science Foundation of China (Nos. 52422505 and 12274124) and the Shanghai pilot Program for Basic Research (No. 22TQ1400100-6) . Q. Z., Z. M. W., and Y. M. Z. acknowledge the Center for Electron Microscopy at Wuhan University for their substantial supports to TEM characterizations. Thanks to engineer Wei Xu in Optoelectronic Micro&Nano Fabrication and Characterizing Facility, Wuhan National Laboratory for Optoelectronics of Huazhong University of Science and Technology for the support in device fabrication. Thanks to the supports from HUST Analytical and Testing Center.

语种：英文

外文关键词：grain boundary; structure-activity correlation; electrochemical reduction reaction of CO2 (CO2RR); in situ surface-enhanced infrared absorption spectroscopy (SEIRAS)

摘要：The electrochemical reduction reaction of CO2 (CO2RR) facilitates the sustainable synthesis of fuels and chemicals. Grain-boundary-rich nanoparticles show superior CO2RR performance, however, the nature of active sites remains elusive. Here, we utilized in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy to identify the active sites and achieve structure-activity correlations, by taking advantage of synthesizing colloidal nanoparticles with welldefined shapes. It indicates that grain boundaries selectively convert CO2 to CO during the CO2RR, and the terrace sites on Cu(100) facets are the active sites for the conversion of CO to C2+ products. Density functional theory calculations show that the optimal adsorption energies of CO2 and CO on grain boundaries facilitate the conversion of CO2 into CO, while the terrace sites on Cu(100) facets selectively convert CO to C2+ products by lowering the activation energy of C-C coupling process. This work provides experimental evidences for the rational design of highly selective catalysts to produce C2+ products via the CO2RR.