文献类型：期刊文献

英文题名：Dynamic restructuring of epitaxial Au-Cu biphasic interface for tandem CO2-to-C2+ alcohol conversion

作者：Zhu, Chenyuan[1];Zhou, Lihui[2];Zhang, Zhibin[3];Yang, Chunlei[1];Shi, Guoshuai[1];Zhao, Siwen[1];Gu, Huoliang[1];Wu, Jing[1];Gao, Xinyang[1];Li, Yefei[1];Liu, Kaihui[3];Dai, Sheng[2];Zhang, Liming[1]

机构：[1]Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat iChEM, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200438, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Key Lab Adv Mat & Joint Int Res Lab Precis Chem &, Shanghai 200237, Peoples R China;[3]Peking Univ, Frontiers Sci Ctr Nanooptoelect, Sch Phys, State Key Lab Mesoscop Phys, Beijing 100871, Peoples R China

年份：2022

卷号：8

期号：12

起止页码：3288

外文期刊名：CHEM

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000906511200001)】；

基金：This research was supported by the National Natural Science Foundation of China (grants 21872039, 22072030, 51991340, 51991342, and 52025023), the Fundamental Research Funds for the Central Universities (20720220008 and JKVJ1221022), the Science and Technology Commission of Shanghai Municipality (grants 18JC1411700 and 19DZ2270100), the Beijing Natural Science Foundation (JQ19004), the Shanghai Rising-star Program (20QA1402400), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, and The Key R&D Program of Guangdong Province (2020B010189001, 2018B030327001). C.Z. thanks the funding support from the China Postdoctoral Science Foundation ( 2021M700810). Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at the East China University of Science and Technology.

语种：英文

摘要：Interfacing Cu with a secondary metal is an effective strategy to enhance the production of value-added C2+ fuels in CO2 electroreduction. However, such a biphasic interface generally suffers unclear dynamic reconstruction/phase transformation, rendering the structure-function correlation elusive. Here, we studied a model system of epitaxial Au-Cu heterostructure, which exhibits a similar to 150 mV more positive onset potential for C2+ alcohols and a 400-fold improved alcohols production over hydrocarbons, relative to primitive Cu. We unambiguously revealed a dynamic restructuring of such heterostructure, from phase-separated bimetals to alloy-supported core-shell nanoclusters, driven by the oxidation/reduction of Cu(0) at the interface. A distinct tandem mechanism was proposed, and the buildup of *CO was identified as crucial to keeping the production durability of C2+ alcohols. This work fills in the voids of direct observation on the dynamic restructuring of the bimetallic interface and establishes a paradigm to understand the tandem CO2-to-C2+ alcohols conversion from an atomic view.