文献类型：期刊文献

英文题名：Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy

作者：Zhang, Li[1,2];Yang, Xiaoju[1,2];Yuan, Qing[1,2];Wei, Zhiming[3];Ding, Jie[3];Chu, Tianshu[4];Rong, Chao[4];Zhang, Qiao[3];Ye, Zhenkun[1,2];Xuan, Fu-Zhen[4];Zhai, Yueming[3];Zhang, Bowei[4];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]Wuhan Univ, Inst Adv Studies, Wuhan 430072, Peoples R China;[4]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai Key Lab Intelligent Sensing & Detect Tec, Key Lab Pressure Syst & Safety,Minist Educ, Shanghai 200237, Peoples R China

年份：2023

卷号：14

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001125281300039)】；

基金：L.Z., XiaojuY., Q.Y., Z.Y. and XuanY. acknowledge the financial support from the National Natural Science Foundation of China (Grant. No. 22204054), the HUST Academic Frontier Youth Team grant (Grant No. 2019QYTD11), Knowledge Innovation Program of Wuhan-Shuguang, and Wuhan Talented Youth Program. T.C., C.R., F.-Z.X. and B.Z. thank the support from the National Natural Science Foundation of China (Grant. No. 52105145, No. 12274124) and the Shanghai pilot Program for Basic Research (Grant. No. 22TQ1400100-6). Z.W., J.D., Q.Z. and Y.Z. acknowledge the Center for Electron Microscopy at Wuhan University for their substantial supports to TEM characterizations. Thanks 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.

语种：英文

摘要：Understanding the structure-stability relationship of catalysts is imperative for the development of high-performance electrocatalytic devices. Herein, we utilize operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to quantitatively monitor the evolution of Cu single-atom catalysts (SACs) during the electrochemical reduction of CO2 (CO2RR). Cu SACs are converted into 2-nm Cu nanoparticles through a reconstruction process during CO2RR. The evolution rate of Cu SACs is highly dependent on the substrates of the catalysts due to the coordination difference. Density functional theory calculations demonstrate that the stability of Cu SACs is highly dependent on their formation energy, which can be manipulated by controlling the affinity between Cu sites and substrates. This work highlights the use of operando ATR-SEIRAS to achieve mechanistic understanding of structure-stability relationship for long-term applications.