Generic approach to access barriers in dehydrogenation reactions

Yu, Liang; Vilella, Laia; Abild-Pedersen, Frank

doi:10.1038/s42004-017-0001-z

Title: Generic approach to access barriers in dehydrogenation reactions

Abstract

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:

^[1]; Vilella, Laia ^[2]; Abild-Pedersen, Frank ^[3]

Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., Stanford, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: Thu Mar 08 00:00:00 EST 2018

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1457169

Grant/Contract Number:: AC02-76SF00515

Resource Type:: Accepted Manuscript

Journal Name:: Communications Chemistry

Additional Journal Information:: Journal Volume: 1; Journal Issue: 1; Journal ID: ISSN 2399-3669

Publisher:: Springer Nature

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Yu, Liang, Vilella, Laia, and Abild-Pedersen, Frank. Generic approach to access barriers in dehydrogenation reactions.  United States: N. p., 2018. 
Web.  doi:10.1038/s42004-017-0001-z.

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                    Yu, Liang, Vilella, Laia, & Abild-Pedersen, Frank. Generic approach to access barriers in dehydrogenation reactions.  United States.  https://doi.org/10.1038/s42004-017-0001-z

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                    Yu, Liang, Vilella, Laia, and Abild-Pedersen, Frank. Thu .  
"Generic approach to access barriers in dehydrogenation reactions".  United States.  https://doi.org/10.1038/s42004-017-0001-z.  https://www.osti.gov/servlets/purl/1457169.

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@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         = {Thu Mar 08 00:00:00 EST 2018},

  month        = {Thu Mar 08 00:00:00 EST 2018}

}

Copy to clipboard

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Works referencing / citing this record:

Accessing the C–C transition state energy on transition metals
journal, January 2019

Aljama, Hassan; Abild-Pedersen, Frank
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Similar Records

Title: Generic approach to access barriers in dehydrogenation reactions

Abstract

Citation Formats

Concepts in Theoretical Heterogeneous Catalytic Reactivity journal, November 1995

Inertia and driving force of chemical reactions journal, January 1938

Universal Brønsted-Evans-Polanyi Relations for C–C, C–O, C–N, N–O, N–N, and O–O Dissociation Reactions journal, November 2010

Computational high-throughput screening of electrocatalytic materials for hydrogen evolution journal, October 2006

On Shustorovich's Bond-Order conservation method as applied to chemisorption journal, January 1990

Introducing structural sensitivity into adsorption–energy scaling relations by means of coordination numbers journal, April 2015

Special points for Brillouin-zone integrations journal, June 1976

Computational catalyst screening: Scaling, bond-order and catalysis journal, September 2016

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal, September 2009

Kinetic Modeling of Pt Catalyzed and Computation-Driven Catalyst Discovery for Ethylene Glycol Decomposition journal, August 2011

The UBI-QEP method: A practical theoretical approach to understanding chemistry on transition metal surfaces journal, January 1998

Heat of molecular chemisorption from bond-order-conservation viewpoint: Why morse potentials are so efficient journal, March 1987

Metal effects in the Fischer-Tropsch synthesis: Bond-order-conservation-morse-potential approach journal, January 1991

Scaling Properties of Adsorption Energies for Hydrogen-Containing Molecules on Transition-Metal Surfaces journal, July 2007

Alloy catalysts designed from first principles journal, October 2004

Chemisorption phenomena: Analytic modeling based on perturbation theory and bond-order conservation journal, July 1986

Ammonia Synthesis from First-Principles Calculations journal, January 2005

Overcoming Limitation in the Design of Selective Solid Catalysts by Manipulating Shape and Size of Catalytic Particles: Epoxidation Reactions on Silver journal, August 2010

Theory of surface chemical reactivity journal, August 2007

Soft self-consistent pseudopotentials in a generalized eigenvalue formalism journal, April 1990

Bond Order Conservation Strategies in Catalysis Applied to the NH 3 Decomposition Reaction journal, December 2016

A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal, December 2000

Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation journal, June 2012

Towards the computational design of solid catalysts journal, April 2009

The theory of reactions involving proton transfers journal, April 1936

Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points journal, December 2000

The Brønsted–Evans–Polanyi relation and the volcano curve in heterogeneous catalysis journal, May 2004

Examining the Linearity of Transition State Scaling Relations journal, May 2015

Scaling relations between adsorption energies for computational screening and design of catalysts journal, January 2014

Brønsted−Evans−Polanyi Relation of Multistep Reactions and Volcano Curve in Heterogeneous Catalysis journal, February 2008

Alloys of platinum and early transition metals as oxygen reduction electrocatalysts journal, September 2009

Computational-based catalyst design for thermochemical transformations journal, March 2011

Ammonia Synthesis from First-Principles Calculations. journal, April 2005

Heat of molecular chemisorption from bond-order-conservation viewpoint: Why morse potentials are so efficient journal, March 1987

Alloy Catalysts Designed from First Principles. journal, January 2005

Accessing the C–C transition state energy on transition metals journal, January 2019

Concepts in Theoretical Heterogeneous Catalytic Reactivity
journal, November 1995

Inertia and driving force of chemical reactions
journal, January 1938

Universal Brønsted-Evans-Polanyi Relations for C–C, C–O, C–N, N–O, N–N, and O–O Dissociation Reactions
journal, November 2010

Computational high-throughput screening of electrocatalytic materials for hydrogen evolution
journal, October 2006

On Shustorovich's Bond-Order conservation method as applied to chemisorption
journal, January 1990

Introducing structural sensitivity into adsorption–energy scaling relations by means of coordination numbers
journal, April 2015

Special points for Brillouin-zone integrations
journal, June 1976

Computational catalyst screening: Scaling, bond-order and catalysis
journal, September 2016

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

Kinetic Modeling of Pt Catalyzed and Computation-Driven Catalyst Discovery for Ethylene Glycol Decomposition
journal, August 2011

The UBI-QEP method: A practical theoretical approach to understanding chemistry on transition metal surfaces
journal, January 1998

Heat of molecular chemisorption from bond-order-conservation viewpoint: Why morse potentials are so efficient
journal, March 1987

Metal effects in the Fischer-Tropsch synthesis: Bond-order-conservation-morse-potential approach
journal, January 1991

Scaling Properties of Adsorption Energies for Hydrogen-Containing Molecules on Transition-Metal Surfaces
journal, July 2007

Alloy catalysts designed from first principles
journal, October 2004

Chemisorption phenomena: Analytic modeling based on perturbation theory and bond-order conservation
journal, July 1986

Ammonia Synthesis from First-Principles Calculations
journal, January 2005

Overcoming Limitation in the Design of Selective Solid Catalysts by Manipulating Shape and Size of Catalytic Particles: Epoxidation Reactions on Silver
journal, August 2010

Theory of surface chemical reactivity
journal, August 2007

Soft self-consistent pseudopotentials in a generalized eigenvalue formalism
journal, April 1990

Bond Order Conservation Strategies in Catalysis Applied to the NH ₃ Decomposition Reaction
journal, December 2016

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation
journal, June 2012

Towards the computational design of solid catalysts
journal, April 2009

The theory of reactions involving proton transfers
journal, April 1936

Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
journal, December 2000

The Brønsted–Evans–Polanyi relation and the volcano curve in heterogeneous catalysis
journal, May 2004

Examining the Linearity of Transition State Scaling Relations
journal, May 2015

Scaling relations between adsorption energies for computational screening and design of catalysts
journal, January 2014

Brønsted−Evans−Polanyi Relation of Multistep Reactions and Volcano Curve in Heterogeneous Catalysis
journal, February 2008

Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
journal, September 2009

Computational-based catalyst design for thermochemical transformations
journal, March 2011

Ammonia Synthesis from First-Principles Calculations.
journal, April 2005

Heat of molecular chemisorption from bond-order-conservation viewpoint: Why morse potentials are so efficient
journal, March 1987

Alloy Catalysts Designed from First Principles.
journal, January 2005

Accessing the C–C transition state energy on transition metals
journal, January 2019