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Title: Generic approach to access barriers in dehydrogenation reactions

The introduction of linear energy correlations, which explicitly relate adsorption energies of reaction intermediates and activation energies in heterogeneous catalysis, has proven to be a key component in the computational search for new and promising catalysts. A simple linear approach to estimate activation energies still requires a significant computational effort. To simplify this process and at the same time incorporate the need for enhanced complexity of reaction intermediates, we generalize a recently proposed approach that evaluates transition state energies based entirely on bond-order conservation arguments. Here, we show that similar variation of the local electronic structure along the reaction coordinate introduces a set of general functions that accurately defines the transition state energy and are transferable to other reactions with similar bonding nature. With such an approach, more complex reaction intermediates can be targeted with an insignificant increase in computational effort and without loss of accuracy.
Authors:
ORCiD logo [1] ;  [2] ;  [3]
  1. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Stanford Univ., Stanford, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Communications Chemistry
Additional Journal Information:
Journal Volume: 1; Journal Issue: 1; Journal ID: ISSN 2399-3669
Publisher:
Springer Nature
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1457169

Yu, Liang, Vilella, Laia, and Abild-Pedersen, Frank. Generic approach to access barriers in dehydrogenation reactions. United States: N. p., Web. doi:10.1038/s42004-017-0001-z.
Yu, Liang, Vilella, Laia, & Abild-Pedersen, Frank. Generic approach to access barriers in dehydrogenation reactions. United States. doi:10.1038/s42004-017-0001-z.
Yu, Liang, Vilella, Laia, and Abild-Pedersen, Frank. 2018. "Generic approach to access barriers in dehydrogenation reactions". United States. doi:10.1038/s42004-017-0001-z.
@article{osti_1457169,
title = {Generic approach to access barriers in dehydrogenation reactions},
author = {Yu, Liang and Vilella, Laia and Abild-Pedersen, Frank},
abstractNote = {The introduction of linear energy correlations, which explicitly relate adsorption energies of reaction intermediates and activation energies in heterogeneous catalysis, has proven to be a key component in the computational search for new and promising catalysts. A simple linear approach to estimate activation energies still requires a significant computational effort. To simplify this process and at the same time incorporate the need for enhanced complexity of reaction intermediates, we generalize a recently proposed approach that evaluates transition state energies based entirely on bond-order conservation arguments. Here, we show that similar variation of the local electronic structure along the reaction coordinate introduces a set of general functions that accurately defines the transition state energy and are transferable to other reactions with similar bonding nature. With such an approach, more complex reaction intermediates can be targeted with an insignificant increase in computational effort and without loss of accuracy.},
doi = {10.1038/s42004-017-0001-z},
journal = {Communications Chemistry},
number = 1,
volume = 1,
place = {United States},
year = {2018},
month = {3}
}

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