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DOE OSTI · 2470983

Revealing CO 2 dissociation pathways at vicinal copper (997) interfaces

Kim, Jeongjin·Yu, Youngseok·Go, Tae Won·Gallet, Jean-Jacques·Bournel, Fabrice·Mun, Bongjin Simon·Park, Jeong Young
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Abstract

Size- and shape-tailored copper (Cu) nanocrystals can offer vicinal planes for facile carbon dioxide (CO 2 ) activation. Despite extensive reactivity benchmarks, a correlation between CO 2 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 CO 2 (g). The CO 2 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 CO 2 conversion to renewable energy sources during C 1 chemical reactions.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYCharacterization and analytical techniquesChemical physicsScanning probe microscopyScience & Technology - Other TopicsStructural properties

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Kim, Jeongjin, Yu, Youngseok, Go, Tae Won, Gallet, Jean-Jacques, Bournel, Fabrice, Mun, Bongjin Simon, Park, Jeong Young. 2023-06-06. Revealing CO 2 dissociation pathways at vicinal copper (997) interfaces. https://doi.org/10.1038/s41467-023-38928-1

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