Reactivity descriptor in solid acid catalysis: Predicting turnover frequencies for propene methylation in zeotypes

Chuan Ming Wang, Rasmus Y. Brogaard, Bert M. Weckhuysen, Jens K. Nørskov, Felix Studt*

*Corresponding author for this work

Research output: Contribution to journalLetterResearchpeer-review

Abstract

Recent work has reported the discovery of metal surface catalysts by employing a descriptor-based approach, establishing a correlation between a few well-defined properties of a material and its catalytic activity. This theoretical work aims for a similar approach in solid acid catalysis, focusing on the reaction between propene and methanol catalyzed by Brønsted acidic zeotype catalysts. Experimentally, the ammonia heat of adsorption is often used as a measure of the strength of acid sites. Using periodic DFT calculations, we show that this measure can be used to establish scaling relations for the energy of intermediates and transition states, effectively describing the reactivity of the acid site. This allows us to use microkinetic modeling to predict a quantitative relation between the ammonia heat of adsorption and the rate of propene methylation from first principles. We propose that this is the first step toward descriptor-based design of solid acid catalysts.

Original languageEnglish
JournalJournal of Physical Chemistry Letters
Volume5
Issue number9
Pages (from-to)1516-1521
Number of pages6
ISSN1948-7185
DOIs
Publication statusPublished - 2014
Externally publishedYes

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