Catalytic Co-Conversion of CH 4 and CO 2 Mediated by Rhodium-Titanium Oxide Anions RhTiO 2 .

Autor: Yang Y; State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China.; University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.; Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190, P.R. China., Li YK; Wilhelm-Ostwald Institut für Physikalische und Theoretische Chemie, Universität Leipzig, Linnéstrasse 2, 04103, Leipzig, Germany.; Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany., Zhao YX; State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China.; Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190, P.R. China., Wei GP; State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China.; University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.; Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190, P.R. China., Ren Y; State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China., Asmis KR; Wilhelm-Ostwald Institut für Physikalische und Theoretische Chemie, Universität Leipzig, Linnéstrasse 2, 04103, Leipzig, Germany., He SG; State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China.; University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.; Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190, P.R. China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2021 Jun 14; Vol. 60 (25), pp. 13788-13792. Date of Electronic Publication: 2021 May 17.
DOI: 10.1002/anie.202103808
Abstrakt: 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 RhTiO 2 - promotes the co-conversion of CH 4 and CO 2 to free 2 H 2 +CO and an adsorbed CO (CO ads ) at room temperature; the only elementary step that requires the input of external energy is desorption of CO ads from the RhTiO 2 CO - to reform RhTiO 2 - . This study not only identifies a promising active species for dry (CO 2 ) 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.
(© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE