Journal article
Understanding trends in C-H bond activation in heterogeneous catalysis
SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, 450 Serra Mall Stanford, California 94305, USA.1
Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, USA.2
SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA.3
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.
Language: | English |
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Publisher: | Nature Publishing Group |
Year: | 2017 |
Pages: | 225-229 |
ISSN: | 14764660 and 14761122 |
Types: | Journal article |
DOI: | 10.1038/nmat4760 |
ORCIDs: | Tsai, Charlie |