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Title: Accessing the C–C transition state energy on transition metals

Abstract

The search for catalysts that can efficiently convert large hydrocarbons has been an active area of research for decades. To gain insight into those reactions, electronic structure calculations are playing an increasing role but the screening efforts are impeded by the complexity of the reaction networks that can contain hundreds of elementary steps, presenting a large number of computationally expensive transition state barrier calculations. A large number of the sub reactions in the network involve C–C bond dissociation, a step that has been identified as rate determining in many studies. The purpose of this article is to present a methodology that allows for accurate and rapid assessment of transition state energies for C–C bond breaking in any hydrocarbon based on a small number of simple calculations. Our model significantly enhances the capability of expanding the search space for new and efficient catalysts.

Authors:
ORCiD logo [1]; ORCiD logo [1]
  1. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1605208
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 21; Journal Issue: 45; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Aljama, Hassan, and Abild-Pedersen, Frank. Accessing the C–C transition state energy on transition metals. United States: N. p., 2019. Web. https://doi.org/10.1039/c9cp04897a.
Aljama, Hassan, & Abild-Pedersen, Frank. Accessing the C–C transition state energy on transition metals. United States. https://doi.org/10.1039/c9cp04897a
Aljama, Hassan, and Abild-Pedersen, Frank. Tue . "Accessing the C–C transition state energy on transition metals". United States. https://doi.org/10.1039/c9cp04897a. https://www.osti.gov/servlets/purl/1605208.
@article{osti_1605208,
title = {Accessing the C–C transition state energy on transition metals},
author = {Aljama, Hassan and Abild-Pedersen, Frank},
abstractNote = {The search for catalysts that can efficiently convert large hydrocarbons has been an active area of research for decades. To gain insight into those reactions, electronic structure calculations are playing an increasing role but the screening efforts are impeded by the complexity of the reaction networks that can contain hundreds of elementary steps, presenting a large number of computationally expensive transition state barrier calculations. A large number of the sub reactions in the network involve C–C bond dissociation, a step that has been identified as rate determining in many studies. The purpose of this article is to present a methodology that allows for accurate and rapid assessment of transition state energies for C–C bond breaking in any hydrocarbon based on a small number of simple calculations. Our model significantly enhances the capability of expanding the search space for new and efficient catalysts.},
doi = {10.1039/c9cp04897a},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 45,
volume = 21,
place = {United States},
year = {2019},
month = {9}
}

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