NDLI: Catalytic selectivity of Rh/TiO<sub>2</sub> catalyst in syngas conversion to ethanol: probing into the mechanism and functions of TiO<sub>2</sub> support and promoter

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Catalytic selectivity of Rh/TiO₂ catalyst in syngas conversion to ethanol: probing into the mechanism and functions of TiO₂ support and promoter

Content Provider	Royal Society of Chemistry (RSC)
Author	Peng, Mao Zhang, Riguang Wang, Baojun
Copyright Year	2017
Abstract	The catalytic selectivity, the functions of a TiO2 support and promoter, and the mechanism of ethanol synthesis from syngas on a Rh/TiO2 model catalyst have been fully identified. Our results show that all species preferentially interact with Rh7 clusters of a Rh/TiO2 catalyst, rather than the support and cluster–support interface. CO → CHO → CH2O → CH3O is an optimal pathway. CH3 formed via the CH3O → CH3 + O route is the most favored CHx (x = 1–3) monomer, and this route is more favorable than methanol formation by CH3O hydrogenation; CO insertion into CH3 can then form CH3CO, followed by successive hydrogenation to ethanol. Methane is formed by CH3 hydrogenation. The Rh/TiO2 catalyst exhibits better catalytic activity and selectivity toward CH3 than CH3OH formation. Starting from the CH3 species, CH4 formation is more favorable than CH3CO formation; thus, ethanol productivity and selectivity on a Rh/TiO2 catalyst with a support is determined only by CH4 formation, which is similar to that on a pure Rh catalyst without a support. Introducing an Fe promoter into the Rh/TiO2 catalyst effectively suppresses methane production, and promotes CH3CO formation. Therefore, compared to a pure Rh catalyst without a support, the TiO2 support serves only to promote the activity and selectivity of CH3 formation, and provide more CH3 species for ethanol formation; methane formation is independent of the Rh catalyst support, and depends only on the promoter. In order to achieve high ethanol productivity and selectivity, an effective Rh-based catalyst must contain a suitable combination of supports and promoters, in which the promoter, M, should have characteristics that draw the d-band center of the MRh/TiO2 catalyst closer to the Fermi level compared to the Rh7/TiO2 catalyst; as a result, the MRh/TiO2 catalyst can suppress CH4 production and facilitate C2 oxygenate formation.
Starting Page	1073
Ending Page	1085
Page Count	13
File Format	HTM / HTML PDF
ISSN	20444753
Volume Number	7
Issue Number	5
Journal	Catalysis Science & Technology
DOI	10.1039/c6cy02350a
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Methane Ethanol Fermi level Interaction CO Monomer Hydrogenation Syngas Methanol
Content Type	Text
Resource Type	Article
Subject	Catalysis

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