Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 25, Pages 13788-13792Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202103808
Keywords
carbon dioxide; catalytic reactions; mass spectrometry; methane; quantum chemistry calculations
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Funding
- K.C. Wong Education Foundation
- National Natural Science Foundation of China [92061115, 21973101]
- Youth Innovation Promotion Association CAS [2018041]
- Alexander von Humboldt Foundation
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [AS 133/4-1]
- Projekt DEAL
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The study identifies a promising active species for dry (CO2) reforming of methane to syngas, and emphasizes the importance of temperature control over elementary steps in practical catalysis. This may significantly alleviate the carbon deposition originating from the pyrolysis of methane.
Catalytic co-conversion of methane with carbon dioxide to produce syngas (2 H-2+2 CO) involves complicated elementary steps and almost all the elementary reactions are performed at the same high temperature conditions in practical thermocatalysis. Here, we demonstrate by mass spectrometric experiments that RhTiO2- promotes the co-conversion of CH4 and CO2 to free 2 H-2+CO and an adsorbed CO (COads) at room temperature; the only elementary step that requires the input of external energy is desorption of COads from the RhTiO2CO- to reform RhTiO2-. This study not only identifies a promising active species for dry (CO2) reforming of methane to syngas, but also emphasizes the importance of temperature control over elementary steps in practical catalysis, which may significantly alleviate the carbon deposition originating from the pyrolysis of methane.
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