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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Bimetallic heterostructures enhance selectivity in carbon dioxide (CO2) electroreduction to multi-carbon (C2+) products.
  • Understanding interfacial structures during electrolysis is key to controlling reaction pathways but remains challenging.

Purpose of the Study:

  • To investigate the relationship between interfacial structure and product selectivity in a well-defined Ag-Cu biphasic heterostructure for CO2 electroreduction.
  • To elucidate the mechanism of structure evolution and its impact on C2+ product formation.

Main Methods:

  • Fabrication of a tunable Ag-Cu biphasic heterostructure.
  • Electrochemical characterization of CO2 electroreduction performance.
  • In-situ/operando analysis to probe interfacial restructuring and intermediate formation.

Main Results:

  • Cu-rich interfaces favor ethylene production, while increasing Ag content shifts selectivity towards alcohols and then CO.
  • A *CO intermediate-regulated restructuring mechanism was identified, involving Cu atom migration onto Ag surfaces.
  • Altered interfacial oxyphilicity due to restructuring dictates CO2 hydrogenation energetics and C2+ product distribution.

Conclusions:

  • The evolving interfacial structure in Ag-Cu heterostructures directly correlates with distinct C2+ product pathways.
  • This work provides design principles for developing bimetallic electrocatalysts with enhanced and selective C2+ yields from CO2 reduction.