Atomic scale simulations of heterogeneous electrocatalysis: recent advances

Egill Skúlason; Hannes Jónsson

doi:10.1080/23746149.2017.1308230

Atomic scale simulations of heterogeneous electrocatalysis: recent advances

Egill Skúlason, Hannes Jónsson

University of Iceland

Research output: Contribution to journal › Review article › peer-review

Abstract

The methodology for atomic scale calculations of electrocatalysis in order to identify mechanisms and estimate reaction rates is reviewed. These include: (1) the application of an external electrical field or potential in density functional theory calculations, (2) the thermochemical model for estimating the onset potential of an electrochemical reaction, and (3) calculations of transition paths in atomic scale models of the electrical double layer. Hydrogen evolution reaction, oxygen reduction reaction as well as CO₂ and N₂ electrochemical reduction to form methane and ammonia are taken as examples. Calculations of reaction rates based on the estimation of the activation energy of elementary steps from minimum energy paths and transition state theory have been shown to provide accurate estimates of rates even for complex reactions and competing reaction mechanisms. There is room, however, for further improvements and some of those are also mentioned at the end of this mini-review.

Original language	English
Pages (from-to)	481-495
Number of pages	15
Journal	Advances in Physics: X
Volume	2
Issue number	3
DOIs	https://doi.org/10.1080/23746149.2017.1308230
Publication status	Published - 4 May 2017

Bibliographical note

Funding Information: This work was funded by the Nordic Energy Research [grant NISFD project]; Icelandic Research Fund [grant administered by RANNIS]; and the Academy of Finland [FiDiPro grant number 263294]. Funding Information: This work was funded by the Nordic Energy Research [grant NISFD project]; Icelandic Research Fund [grant administered by RANNIS]; and the Academy of Finland [FiDiPro grant number 263294]. We would like to thank our numerous collaborators, in particular Jens K. Nørskov, Jan Rossmeisl, Vladimir Tripković and Maarten E. Björketun, as well as Andrew Peterson and our Ph.D. students at the University of Iceland who carried out some of the calculations reviewed here, Sigrídur Gudmundsdóttir and Javed Hussain. Publisher Copyright: © 2017, © 2017, © 2017 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.

Other keywords

31.15.Ew Density functional theory
68.35.Md Surface thermodynamics, surface energies
73.20.-r Electron states at surfaces and interfaces
73.30.+y Surface double layers, Schottky barriers, and work functions
Electrocatalysis
rate estimation
reaction mechanism
simulation

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10.1080/23746149.2017.1308230

Cite this

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title = "Atomic scale simulations of heterogeneous electrocatalysis: recent advances",

abstract = "The methodology for atomic scale calculations of electrocatalysis in order to identify mechanisms and estimate reaction rates is reviewed. These include: (1) the application of an external electrical field or potential in density functional theory calculations, (2) the thermochemical model for estimating the onset potential of an electrochemical reaction, and (3) calculations of transition paths in atomic scale models of the electrical double layer. Hydrogen evolution reaction, oxygen reduction reaction as well as CO2 and N2 electrochemical reduction to form methane and ammonia are taken as examples. Calculations of reaction rates based on the estimation of the activation energy of elementary steps from minimum energy paths and transition state theory have been shown to provide accurate estimates of rates even for complex reactions and competing reaction mechanisms. There is room, however, for further improvements and some of those are also mentioned at the end of this mini-review.",

keywords = "31.15.Ew Density functional theory, 68.35.Md Surface thermodynamics, surface energies, 73.20.-r Electron states at surfaces and interfaces, 73.30.+y Surface double layers, Schottky barriers, and work functions, Electrocatalysis, rate estimation, reaction mechanism, simulation",

author = "Egill Sk{\'u}lason and Hannes J{\'o}nsson",

note = "Funding Information: This work was funded by the Nordic Energy Research [grant NISFD project]; Icelandic Research Fund [grant administered by RANNIS]; and the Academy of Finland [FiDiPro grant number 263294]. Funding Information: This work was funded by the Nordic Energy Research [grant NISFD project]; Icelandic Research Fund [grant administered by RANNIS]; and the Academy of Finland [FiDiPro grant number 263294]. We would like to thank our numerous collaborators, in particular Jens K. N{\o}rskov, Jan Rossmeisl, Vladimir Tripkovi{\'c} and Maarten E. Bj{\"o}rketun, as well as Andrew Peterson and our Ph.D. students at the University of Iceland who carried out some of the calculations reviewed here, Sigr{\'i}dur Gudmundsd{\'o}ttir and Javed Hussain. Publisher Copyright: {\textcopyright} 2017, {\textcopyright} 2017, {\textcopyright} 2017 The Author(s). Published by Informa UK Limited, trading as Taylor \& Francis Group.",

year = "2017",

month = may,

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doi = "10.1080/23746149.2017.1308230",

language = "English",

volume = "2",

pages = "481--495",

journal = "Advances in Physics: X",

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T2 - recent advances

AU - Skúlason, Egill

AU - Jónsson, Hannes

N1 - Funding Information: This work was funded by the Nordic Energy Research [grant NISFD project]; Icelandic Research Fund [grant administered by RANNIS]; and the Academy of Finland [FiDiPro grant number 263294]. Funding Information: This work was funded by the Nordic Energy Research [grant NISFD project]; Icelandic Research Fund [grant administered by RANNIS]; and the Academy of Finland [FiDiPro grant number 263294]. We would like to thank our numerous collaborators, in particular Jens K. Nørskov, Jan Rossmeisl, Vladimir Tripković and Maarten E. Björketun, as well as Andrew Peterson and our Ph.D. students at the University of Iceland who carried out some of the calculations reviewed here, Sigrídur Gudmundsdóttir and Javed Hussain. Publisher Copyright: © 2017, © 2017, © 2017 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.

PY - 2017/5/4

Y1 - 2017/5/4

N2 - The methodology for atomic scale calculations of electrocatalysis in order to identify mechanisms and estimate reaction rates is reviewed. These include: (1) the application of an external electrical field or potential in density functional theory calculations, (2) the thermochemical model for estimating the onset potential of an electrochemical reaction, and (3) calculations of transition paths in atomic scale models of the electrical double layer. Hydrogen evolution reaction, oxygen reduction reaction as well as CO2 and N2 electrochemical reduction to form methane and ammonia are taken as examples. Calculations of reaction rates based on the estimation of the activation energy of elementary steps from minimum energy paths and transition state theory have been shown to provide accurate estimates of rates even for complex reactions and competing reaction mechanisms. There is room, however, for further improvements and some of those are also mentioned at the end of this mini-review.

AB - The methodology for atomic scale calculations of electrocatalysis in order to identify mechanisms and estimate reaction rates is reviewed. These include: (1) the application of an external electrical field or potential in density functional theory calculations, (2) the thermochemical model for estimating the onset potential of an electrochemical reaction, and (3) calculations of transition paths in atomic scale models of the electrical double layer. Hydrogen evolution reaction, oxygen reduction reaction as well as CO2 and N2 electrochemical reduction to form methane and ammonia are taken as examples. Calculations of reaction rates based on the estimation of the activation energy of elementary steps from minimum energy paths and transition state theory have been shown to provide accurate estimates of rates even for complex reactions and competing reaction mechanisms. There is room, however, for further improvements and some of those are also mentioned at the end of this mini-review.

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JO - Advances in Physics: X

JF - Advances in Physics: X

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ER -

Atomic scale simulations of heterogeneous electrocatalysis: recent advances

Abstract

Bibliographical note

Other keywords

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