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., ... 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
Latimer, Allegra A. ; Kulkarni, Ambarish R. ; Aljama, Hassan ; Montoya, Joseph H. ; Yoo, Jong Suk ; Tsai, Charlie ; Abild-Pedersen, Frank ; Studt, Felix ; Nørskov, Jens K. / Understanding trends in C-H bond activation in heterogeneous catalysis. In: Nature Materials. 2017 ; Vol. 16, No. 2. pp. 225-229.
@article{cd1f975c73264aa19514dd16ddfa3114,
title = "Understanding trends in C-H bond activation in heterogeneous catalysis",
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.",
author = "Latimer, {Allegra A.} and Kulkarni, {Ambarish R.} and Hassan Aljama and Montoya, {Joseph H.} and Yoo, {Jong Suk} and Charlie Tsai and Frank Abild-Pedersen and Felix Studt and N{\o}rskov, {Jens K.}",
year = "2017",
doi = "10.1038/nmat4760",
language = "English",
volume = "16",
pages = "225--229",
journal = "Nature Materials",
issn = "1476-1122",
publisher = "Nature Publishing Group",
number = "2",

}

Latimer, AA, Kulkarni, AR, Aljama, H, Montoya, JH, Yoo, JS, Tsai, C, Abild-Pedersen, F, Studt, F & Nørskov, JK 2017, 'Understanding trends in C-H bond activation in heterogeneous catalysis', Nature Materials, vol. 16, no. 2, pp. 225-229. https://doi.org/10.1038/nmat4760

Understanding trends in C-H bond activation in heterogeneous catalysis. / Latimer, Allegra A.; Kulkarni, Ambarish R.; Aljama, Hassan; Montoya, Joseph H.; Yoo, Jong Suk; Tsai, Charlie; Abild-Pedersen, Frank; Studt, Felix; Nørskov, Jens K.

In: Nature Materials, Vol. 16, No. 2, 2017, p. 225-229.

Research output: Contribution to journalLetterResearchpeer-review

TY - JOUR

T1 - Understanding trends in C-H bond activation in heterogeneous catalysis

AU - Latimer, Allegra A.

AU - Kulkarni, Ambarish R.

AU - Aljama, Hassan

AU - Montoya, Joseph H.

AU - Yoo, Jong Suk

AU - Tsai, Charlie

AU - Abild-Pedersen, Frank

AU - Studt, Felix

AU - Nørskov, Jens K.

PY - 2017

Y1 - 2017

N2 - 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.

AB - 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.

U2 - 10.1038/nmat4760

DO - 10.1038/nmat4760

M3 - Letter

C2 - 27723737

AN - SCOPUS:84991017458

VL - 16

SP - 225

EP - 229

JO - Nature Materials

JF - Nature Materials

SN - 1476-1122

IS - 2

ER -

Latimer AA, Kulkarni AR, Aljama H, Montoya JH, Yoo JS, Tsai C et al. Understanding trends in C-H bond activation in heterogeneous catalysis. Nature Materials. 2017;16(2):225-229. https://doi.org/10.1038/nmat4760