Quasi-graphitic carbon shell-induced Cu confinement promotes electrocatalytic CO2 reduction toward C2+ products

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For steady electroconversion to value-added chemical products with high efficiency, electrocatalyst reconstruction during electrochemical reactions is a critical issue in catalyst design strategies. Here, we report a reconstruction-immunized catalyst system in which Cu nanoparticles are protected by a quasi-graphitic C shell. This C shell epitaxially grew on Cu with quasi-graphitic bonding via a gas-solid reaction governed by the CO (g) - CO2 (g) - C (s) equilibrium. The quasi-graphitic C shell-coated Cu was stable during the CO2 reduction reaction and provided a platform for rational material design. C2+ product selectivity could be additionally improved by doping p-block elements. These elements modulated the electronic structure of the Cu surface and its binding properties, which can affect the intermediate binding and CO dimerization barrier. B-modified Cu attained a 68.1% Faradaic efficiency for C2H4 at -0.55V (vs RHE) and a C2H4 cathodic power conversion efficiency of 44.0%. In the case of N-modified Cu, an improved C2+ selectivity of 82.3% at a partial current density of 329.2mA/cm(2) was acquired. Quasi-graphitic C shells, which enable surface stabilization and inner element doping, can realize stable CO2-to-C2H4 conversion over 180h and allow practical application of electrocatalysts for renewable energy conversion. Surface reconstruction of electrocatalysts is an important issue for electroconversion of carbon dioxide to value-added chemical products. Here the authors address this issue by using copper nanoparticles protected by self-formed quasi graphitic carbon shell for stable CO2 to C2H4 conversion.
Publisher
NATURE RESEARCH
Issue Date
2021-06
Language
English
Article Type
Article
Citation

NATURE COMMUNICATIONS, v.12, no.1, pp.3765

ISSN
2041-1723
DOI
10.1038/s41467-021-24105-9
URI
http://hdl.handle.net/10203/286563
Appears in Collection
CBE-Journal Papers(저널논문)MS-Journal Papers(저널논문)
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