期刊
CHEM
卷 8, 期 12, 页码 3288-3301出版社
CELL PRESS
DOI: 10.1016/j.chempr.2022.08.016
关键词
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资金
- National Natural Science Foundation of China [21872039, 22072030, 51991340, 51991342, 52025023]
- Fundamental Research Funds for the Central Universities [20720220008, JKVJ1221022]
- Science and Technology Commission of Shanghai Municipality [18JC1411700, 19DZ2270100]
- Beijing Natural Science Foundation [JQ19004]
- Shanghai Rising-star Program [20QA1402400]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
- Key R&D Program of Guangdong Province [2020B010189001, 2018B030327001]
- China Postdoctoral Science Foundation [2021M700810]
- Frontiers Science Center for Materiobiology and Dynamic Chemistry
- Feringa Nobel Prize Scientist Joint Research Center at the East China University of Science and Technology
Interfacing Cu with a secondary metal can enhance the production of C2+ fuels in CO2 electroreduction. This study investigates the dynamic restructuring of an Au-Cu heterostructure and proposes a tandem mechanism to understand the conversion of CO2 to C2+ alcohols.
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.
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