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

Autor: Kim J; Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 34141, Republic of Korea.; Chemistry Division, Brookhaven National Laboratory, Upton, NY, 11973, US., Yu Y; Department of Physics and Photon Science, School of Physics and Chemistry, Gwangju Institute of Science and Technology (GIST), Gwangju, 61005, Republic of Korea.; Center for Advanced X-ray Science, GIST, Gwangju, 61005, Republic of Korea., Go TW; Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 34141, Republic of Korea., Gallet JJ; Laboratoire de Chimie Physique-Matière et Rayonnement, CNRS, Sorbonne Université, Paris, 75005, France.; Synchrotron SOLEIL, Saint-Aubin, Gif sur Yvette, 91192, France., Bournel F; Laboratoire de Chimie Physique-Matière et Rayonnement, CNRS, Sorbonne Université, Paris, 75005, France.; Synchrotron SOLEIL, Saint-Aubin, Gif sur Yvette, 91192, France., Mun BS; Department of Physics and Photon Science, School of Physics and Chemistry, Gwangju Institute of Science and Technology (GIST), Gwangju, 61005, Republic of Korea. bsmun@gist.ac.kr.; Center for Advanced X-ray Science, GIST, Gwangju, 61005, Republic of Korea. bsmun@gist.ac.kr., Park JY; Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 34141, Republic of Korea. jeongypark@kaist.ac.kr.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2023 Jun 06; Vol. 14 (1), pp. 3273. Date of Electronic Publication: 2023 Jun 06.
DOI: 10.1038/s41467-023-38928-1
Abstrakt: 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.
(© 2023. The Author(s).)
Databáze: MEDLINE
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