Journal article
The Challenge of CO Hydrogenation to Methanol: Fundamental Limitations Imposed by Linear Scaling Relations
Recent developments in computational catalysis have allowed the routine reduction of the dimensionality of complex reaction networks to a few descriptors based on linear scaling relations. Despite this convenient benefit, linear scaling relations fundamentally limit the activity and selectivity of a given class of materials towards a given reaction.
Here, we show an example by offering a novel description of the fundamental limits on the activity of CO hydrogenation to methanol; a reaction that offers a sustainable route to obtaining value-added chemicals from syngas. First, we show that there is a strong linear correlation between the formation energy of CO* (where * denotes an adsorbed species) and those of the transition states of a number of elementary steps along the methanol synthesis pathway on these surfaces.
Using microkinetic modeling, we cast this information into activity volcano plots with the formation energies of a given transition state and CO* as independent descriptors. This analysis reveals the fundamental limits on activity imposed by the aforementioned linear scaling relations, and invites a vigorous search for novel materials that escape these linear scaling relations as a necessary condition for achieving improved activity towards methanol from CO hydrogenation.
Specifically, we point out the transition states H–CO* and CH3O–H* as key transition states to be stabilized independently of CO* for improved activity and selectivity towards methanol synthesis.
Language: | English |
---|---|
Publisher: | Springer US |
Year: | 2020 |
Pages: | 635-648 |
ISSN: | 15729028 and 10225528 |
Types: | Journal article |
DOI: | 10.1007/s11244-020-01283-2 |
ORCIDs: | Elnabawy, Ahmed O. , 0000-0002-4041-0165 and Nørskov, Jens K. |