Understanding trends in C-H bond activation in heterogeneous catalysis

Allegra A. Latimer, Ambarish R. Kulkarni, Hassan Aljama, Joseph H. Montoya, Jong Suk Yoo, Charlie Tsai, Frank Abild-Pedersen, Felix Studt, Jens K. Nørskov

Research output: Contribution to journalLetterResearchpeer-review

Abstract

While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed. Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C-H activation barriers using a single universal descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.

Original languageEnglish
JournalNature Materials
Volume16
Issue number2
Pages (from-to)225-229
Number of pages5
ISSN1476-1122
DOIs
Publication statusPublished - 2017
Externally publishedYes

Cite this

Latimer, A. A., Kulkarni, A. R., Aljama, H., Montoya, J. H., Yoo, J. S., Tsai, C., Abild-Pedersen, F., Studt, F., & Nørskov, J. K. (2017). Understanding trends in C-H bond activation in heterogeneous catalysis. Nature Materials, 16(2), 225-229. https://doi.org/10.1038/nmat4760