Brooks, A., Jenkins, S., Wrabetz, S. et al. (2 more authors) (2022) The dehydrogenation of butane on metal-free graphene. Journal of Colloid & Interface Science, 619. pp. 377-387. ISSN 0021-9797
Abstract
The dehydrogenation of alkane feedstock to produce alkenes is a significant and energy intensive industrial process, generally occurring on metals and metal oxides. Here, we investigate a catalytic mechanism for the dehydrogenation of butane on single-layer, metal-free graphene using a combination of ab initio quantum chemical calculations and Adsorption Microcalorimetry. Dispersion-corrected Density Functional Theory (DFT) is employed to calculate transition states and energy minima that describe the reaction pathways connecting butane to the two possible products, but-1-ene and but-2-ene. The deprotonations occur with moderate energy barriers in the 0.54 eV ÷ 0.69 eV range. A strong agreement is observed between the results of the adsorption energies calculated by DFT (0.40 eV) and the measured differential heat of adsorption of n-butane on graphitic overlayer. We conclude that the active-site for this catalytic reaction is a metal-free graphene vacancy, created by removing a carbon atom from a single-layer graphene sheet.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2022 The Author(s). Published by Elsevier Inc. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). |
Keywords: | graphene catalysis; dehydrogenation; metal-free catalysis; graphene vacancy; density functional theory |
Dates: |
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Institution: | The University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Engineering (Sheffield) > Department of Chemical and Biological Engineering (Sheffield) |
Depositing User: | Symplectic Sheffield |
Date Deposited: | 05 Apr 2022 15:26 |
Last Modified: | 20 Apr 2022 09:03 |
Status: | Published |
Publisher: | Elsevier Inc |
Refereed: | Yes |
Identification Number: | 10.1016/j.jcis.2022.03.128 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:185346 |