On the Mn promoted synthesis of higher alcohols over Cu derived ternary catalysts


This work provides insight into the promotional effect of Mn on the synthesis of higher alcohols over Cu-based ternary catalysts through XPS and in situ DRIFTS and powder XRD. These revealed that the surface of K-CuZnAl, an active catalyst for CO hydrogenation to methanol, possesses Cu+ sites able to adsorb CO associatively and Cu0 sites for H2 dissociation. Here we show that exchanging Zn with Mn induces a strong interaction between Cu and Mn that decreases the overall copper surface area and increases the Cu+/Cu0 ratio. In situ DRIFTS showed that electronic modification of Cu+ sites by proximate Mn favors dissociative CO chemisorption, resulting in the formation of C and O adspecies that are precursors to higher alcohol formation. The decrease in metallic copper limits available sites for H2 dissociation, and hence retards the hydrogenation of oxygen-containing intermediates, thereby further promoting carbon-chain growth. Mn also increases the dispersion of K promoter over the catalyst surface, providing abundant basic sites for aldol-type condensation reactions to branched oxygenates.

Publication DOI: https://doi.org/10.1039/C7CY00018A
Dataset DOI: https://doi.org/10.17036/researchdata.aston.ac.uk.00000189
Divisions: College of Engineering & Physical Sciences
College of Engineering & Physical Sciences > School of Infrastructure and Sustainable Engineering > Chemical Engineering & Applied Chemistry
College of Engineering & Physical Sciences > Energy and Bioproducts Research Institute (EBRI)
Additional Information: This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
Uncontrolled Keywords: Catalysis
Publication ISSN: 2044-4761
Last Modified: 08 Jan 2024 08:19
Date Deposited: 24 Jan 2017 08:14
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Related URLs: http://www.scop ... tnerID=8YFLogxK (Scopus URL)
PURE Output Type: Article
Published Date: 2017-02-21
Published Online Date: 2017-01-23
Accepted Date: 2017-01-21
Authors: Liakakou, Eleni T.
Isaacs, Mark
Wilson, Karen (ORCID Profile 0000-0003-4873-708X)
Lee, Adam F. (ORCID Profile 0000-0002-2153-1391)
Heracleous, Eleni



Version: Published Version

License: Creative Commons Attribution

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