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Media type:
E-Article
Title:
Quasi-graphitic carbon shell-induced Cu confinement promotes electrocatalytic CO2 reduction toward C2+ products
Contributor:
Kim, Ji-Yong;
Hong, Deokgi;
Lee, Jae-Chan;
Kim, Hyoung Gyun;
Lee, Sungwoo;
Shin, Sangyong;
Kim, Beomil;
Lee, Hyunjoo;
Kim, Miyoung;
Oh, Jihun;
Lee, Gun-Do;
Nam, Dae-Hyun;
Joo, Young-Chang
Published:
Springer Science and Business Media LLC, 2021
Published in:
Nature Communications, 12 (2021) 1
Language:
English
DOI:
10.1038/s41467-021-24105-9
ISSN:
2041-1723
Origination:
Footnote:
Description:
<jats:title>Abstract</jats:title><jats:p>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) - CO<jats:sub>2</jats:sub> (g) - C (s) equilibrium. The quasi-graphitic C shell-coated Cu was stable during the CO<jats:sub>2</jats:sub> reduction reaction and provided a platform for rational material design. C<jats:sub>2+</jats:sub> product selectivity could be additionally improved by doping <jats:italic>p</jats:italic>-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 C<jats:sub>2</jats:sub>H<jats:sub>4</jats:sub> at −0.55 V (vs RHE) and a C<jats:sub>2</jats:sub>H<jats:sub>4</jats:sub> cathodic power conversion efficiency of 44.0%. In the case of N-modified Cu, an improved C<jats:sub>2+</jats:sub> selectivity of 82.3% at a partial current density of 329.2 mA/cm<jats:sup>2</jats:sup> was acquired. Quasi-graphitic C shells, which enable surface stabilization and inner element doping, can realize stable CO<jats:sub>2</jats:sub>-to-C<jats:sub>2</jats:sub>H<jats:sub>4</jats:sub> conversion over 180 h and allow practical application of electrocatalysts for renewable energy conversion.</jats:p>