How Rh surface breaks CO2 molecules under ambient pressure

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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 OCO* with ordered intermediates structure formation of (2x2)-CO on an atomically flat Rh(111) surface at room temperature. Direct observation of carbon dioxide dissociation provides an origin of catalytic conversion for industrial chemical reactions. Here, the authors reveal their molecular interactions on the rhodium catalyst at near-ambient pressure by interface science techniques and computational calculations.
Publisher
NATURE RESEARCH
Issue Date
2020-11
Language
English
Article Type
Article
Citation

NATURE COMMUNICATIONS, v.11, no.1

ISSN
2041-1723
DOI
10.1038/s41467-020-19398-1
URI
http://hdl.handle.net/10203/279275
Appears in Collection
CH-Journal Papers(저널논문)
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