Exploration of Gas‑Dependent Self‑Adaptive Reconstruction Behavior of Cu_(2)O for Electrochemical CO_(2) Conversion to Multi‑Carbon Products  

作　　者：Chaoran Zhang Yichuan Gu Qu Jiang Ziyang Sheng Ruohan Feng Sihong Wang Haoyue Zhang Qianqing Xu Zijian Yuan Fang Song 

机构地区：[1]State Key Laboratory of Metal Matrix Composites,School of Materials Science and Engineering,Shanghai Jiao Tong University,Shanghai 200240,People’s Republic of China

出　　处：《Nano-Micro Letters》2025年第3期280-296,共17页纳微快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(Grant No.22479097);the Shanghai Science and Technology Committee(Grant No.23ZR1433000);the National High-Level Talent Program for Young Scholars,the Start-up Fund(F.S.)from Shanghai Jiao Tong University.

摘　　要：Structural reconstruction of electrocatalysts plays a pivotal role in catalytic performances for CO_(2)reduction reaction(CO_(2)RR),whereas the behavior is by far superficially understood.Here,we report that CO_(2)accessibility results in a universal self-adaptive structural reconstruction from Cu_(2)O to Cu@CuxO composites,ending with feeding gas-dependent microstructures and catalytic performances.The CO_(2)-rich atmosphere favors reconstruction for CO_(2)RR,whereas the CO_(2)-deficient one prefers that for hydrogen evolution reaction.With the assistance of spectroscopic analysis and theoretical calculations,we uncover a CO_(2)-induced passivation behavior by identifying a reductionresistant but catalytic active Cu(I)-rich amorphous layer stabilized by*CO intermediates.Additionally,we find extra CO production is indispensable for the robust production of C2H4.An inverse correlation between durability and FECO/FEC2H4 is disclosed,suggesting that the selfstabilization process involving the absorption of*CO intermediates on Cu(I)sites is essential for durable electrolysis.Guided by this insight,we design hollow Cu_(2)O nanospheres for durable and selective CO_(2)RR electrolysis in producing C2H4.Our work recognizes the previously overlooked passivation reconstruction and self-stabilizing behavior and highlights the critical role of the local atmosphere in modulating reconstruction and catalytic processes.

关 键 词：CO_(2)reduction reaction ELECTROCATALYSTS Cu_(2)O RECONSTRUCTION Self-adaptive electrocatalysis 

分 类 号：TQ426[化学工程] X701[环境科学与工程—环境工程]