How Rh surface breaks CO2 molecules under ambient pressure

Jeongjin Kim, Hyunwoo Ha, Won Hui Doh, Kohei Ueda, Kazuhiko Mase, Hiroshi Kondoh, Bongjin Simon Mun (), Hyun You Kim () and Jeong Young Park ()
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Jeongjin Kim: Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
Hyunwoo Ha: Chungnam National University
Won Hui Doh: Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)
Kohei Ueda: Keio University
Kazuhiko Mase: SOKENDAI (The Graduate University for Advanced Studies)
Hiroshi Kondoh: Keio University
Bongjin Simon Mun: Gwangju Institute of Science and Technology (GIST)
Hyun You Kim: Chungnam National University
Jeong Young Park: Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS)

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Utilization of carbon dioxide (CO2) molecules leads to increased interest in the sustainable synthesis of methane (CH4) or methanol (CH3OH). The representative reaction intermediate consisting of a carbonyl or formate group determines yields of the fuel source during catalytic reactions. However, their selective initial surface reaction processes have been assumed without a fundamental understanding at the molecular level. Here, we report direct observations of spontaneous CO2 dissociation over the model rhodium (Rh) catalyst at 0.1 mbar CO2. The linear geometry of CO2 gas molecules turns into a chemically active bent-structure at the interface, which allows non-uniform charge transfers between chemisorbed CO2 and surface Rh atoms. By combining scanning tunneling microscopy, X-ray photoelectron spectroscopy at near-ambient pressure, and computational calculations, we reveal strong evidence for chemical bond cleavage of O‒CO* with ordered intermediates structure formation of (2 × 2)-CO on an atomically flat Rh(111) surface at room temperature.

Date: 2020
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DOI: 10.1038/s41467-020-19398-1

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