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

Ji-Yong Kim, Deokgi Hong, Jae-Chan Lee, Hyoung Gyun Kim, Sungwoo Lee, Sangyong Shin, Beomil Kim, Hyunjoo Lee, Miyoung Kim, Jihun Oh, Gun-Do Lee (), Dae-Hyun Nam () and Young-Chang Joo ()
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Ji-Yong Kim: Seoul National University
Deokgi Hong: Seoul National University
Jae-Chan Lee: Seoul National University
Hyoung Gyun Kim: Seoul National University
Sungwoo Lee: Seoul National University
Sangyong Shin: Korea Advanced Institute of Science and Technology
Beomil Kim: Korea Advanced Institute of Science and Technology
Hyunjoo Lee: Korea Advanced Institute of Science and Technology
Miyoung Kim: Seoul National University
Jihun Oh: Korea Advanced Institute of Science and Technology
Gun-Do Lee: Seoul National University
Dae-Hyun Nam: Daegu Gyeongbuk Institute of Science and Technology (DGIST)
Young-Chang Joo: Seoul National University

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract 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 −0.55 V (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 329.2 mA/cm2 was acquired. Quasi-graphitic C shells, which enable surface stabilization and inner element doping, can realize stable CO2-to-C2H4 conversion over 180 h and allow practical application of electrocatalysts for renewable energy conversion.

Date: 2021
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DOI: 10.1038/s41467-021-24105-9

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