Liakakou, Eleni T., Isaacs, Mark, Wilson, Karen, Lee, Adam F. and Heracleous, Eleni (2017). On the Mn promoted synthesis of higher alcohols over Cu derived ternary catalysts. Catalysis Science and Technology, 7 (4), pp. 988-999.
Abstract
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: | 30 Oct 2024 08:13 |
Date Deposited: | 24 Jan 2017 08:14 |
Full Text Link: | |
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 ( 0000-0003-4873-708X) Lee, Adam F. ( 0000-0002-2153-1391) Heracleous, Eleni |