Revealing CO2 dissociation pathways at vicinal copper (997) interfaces

Jeongjin Kim, Youngseok Yu, Tae Won Go, Jean-Jacques Gallet, Fabrice Bournel, Bongjin Simon Mun () and Jeong Young Park ()
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Jeongjin Kim: Korea Advanced Institute of Science and Technology (KAIST)
Youngseok Yu: Gwangju Institute of Science and Technology (GIST)
Tae Won Go: Korea Advanced Institute of Science and Technology (KAIST)
Jean-Jacques Gallet: CNRS, Sorbonne Université
Fabrice Bournel: CNRS, Sorbonne Université
Bongjin Simon Mun: Gwangju Institute of Science and Technology (GIST)
Jeong Young Park: Korea Advanced Institute of Science and Technology (KAIST)

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Size- and shape-tailored copper (Cu) nanocrystals can offer vicinal planes for facile carbon dioxide (CO2) activation. Despite extensive reactivity benchmarks, a correlation between CO2 conversion and morphology structure has not yet been established at vicinal Cu interfaces. Herein, ambient pressure scanning tunneling microscopy reveals step-broken Cu nanocluster evolutions on the Cu(997) surface under 1 mbar CO2(g). The CO2 dissociation reaction produces carbon monoxide (CO) adsorbate and atomic oxygen (O) at Cu step-edges, inducing complicated restructuring of the Cu atoms to compensate for increased surface chemical potential energy at ambient pressure. The CO molecules bound at under-coordinated Cu atoms contribute to the reversible Cu clustering with the pressure gap effect, whereas the dissociated oxygen leads to irreversible Cu faceting geometries. Synchrotron-based ambient pressure X-ray photoelectron spectroscopy identifies the chemical binding energy changes in CO-Cu complexes, which proves the characterized real-space evidence for the step-broken Cu nanoclusters under CO(g) environments. Our in situ surface observations provide a more realistic insight into Cu nanocatalyst designs for efficient CO2 conversion to renewable energy sources during C1 chemical reactions.

Date: 2023
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DOI: 10.1038/s41467-023-38928-1

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