skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on March 28, 2020

Title: Theory and experiments join forces to characterize the electrocatalytic interface

Abstract

Electrocatalysis is gaining impetus as a key technology in fuel cells and for the medium-term energy storage in the context of intermittent, renewable energy sources such as wind and solar power. Furthermore, electrocatalysis promises to convert rather inert molecules such as CO 2 and N 2 into reduced products such as CO and ammonia under relatively mild conditions (1, 2). Harnessing the full power of electrocatalysis is, however, hampered by a lack of understanding of the governing physical and chemical processes at the metal–electrolyte interface. In PNAS, Cheng et al. (3) bring key insight to the characterization of reaction intermediates during CO 2 electroreduction via firstprinciples molecular dynamics modeling. This reaction is timely and has, over the last few years, served as the playground for advanced atomistic modeling of electrocatalysis (4–9).

Authors:
 [1];  [2]; ORCiD logo [2]
  1. National Centre for Scientific Research (CNRS), Lyon (France)
  2. Univ. of California, Los Angeles, CA (United States)
Publication Date:
Research Org.:
Univ. of California, Los Angeles, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1567210
Grant/Contract Number:  
SC0019381
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 116; Journal Issue: 16; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electrocatalysis; electrical energy storage; defects; charge transport; mesoscale science; materials and chemistry by design; mesostructured materials; synthesis (novel materials); synthesis (scalable processing)

Citation Formats

Steinmann, Stephan N., Wei, Zi-Yang, and Sautet, Philippe. Theory and experiments join forces to characterize the electrocatalytic interface. United States: N. p., 2019. Web. doi:10.1073/pnas.1903412116.
Steinmann, Stephan N., Wei, Zi-Yang, & Sautet, Philippe. Theory and experiments join forces to characterize the electrocatalytic interface. United States. doi:10.1073/pnas.1903412116.
Steinmann, Stephan N., Wei, Zi-Yang, and Sautet, Philippe. Thu . "Theory and experiments join forces to characterize the electrocatalytic interface". United States. doi:10.1073/pnas.1903412116.
@article{osti_1567210,
title = {Theory and experiments join forces to characterize the electrocatalytic interface},
author = {Steinmann, Stephan N. and Wei, Zi-Yang and Sautet, Philippe},
abstractNote = {Electrocatalysis is gaining impetus as a key technology in fuel cells and for the medium-term energy storage in the context of intermittent, renewable energy sources such as wind and solar power. Furthermore, electrocatalysis promises to convert rather inert molecules such as CO2 and N2 into reduced products such as CO and ammonia under relatively mild conditions (1, 2). Harnessing the full power of electrocatalysis is, however, hampered by a lack of understanding of the governing physical and chemical processes at the metal–electrolyte interface. In PNAS, Cheng et al. (3) bring key insight to the characterization of reaction intermediates during CO2 electroreduction via firstprinciples molecular dynamics modeling. This reaction is timely and has, over the last few years, served as the playground for advanced atomistic modeling of electrocatalysis (4–9).},
doi = {10.1073/pnas.1903412116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 16,
volume = 116,
place = {United States},
year = {2019},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on March 28, 2020
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Catalysts for nitrogen reduction to ammonia
journal, July 2018

  • Foster, Shelby L.; Bakovic, Sergio I. Perez; Duda, Royce D.
  • Nature Catalysis, Vol. 1, Issue 7
  • DOI: 10.1038/s41929-018-0092-7

Theoretical Considerations on the Electroreduction of CO to C 2 Species on Cu(100) Electrodes
journal, June 2013

  • Calle-Vallejo, Federico; Koper, Marc T. M.
  • Angewandte Chemie International Edition, Vol. 52, Issue 28
  • DOI: 10.1002/anie.201301470

Identification of Possible Pathways for C–C Bond Formation during Electrochemical Reduction of CO 2 : New Theoretical Insights from an Improved Electrochemical Model
journal, April 2016

  • Goodpaster, Jason D.; Bell, Alexis T.; Head-Gordon, Martin
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 8
  • DOI: 10.1021/acs.jpclett.6b00358

Hydration of metal surfaces can be dynamically heterogeneous and hydrophobic
journal, February 2013

  • Limmer, David T.; Willard, Adam P.; Madden, Paul
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 11
  • DOI: 10.1073/pnas.1301596110

Insights into CC Coupling in CO 2 Electroreduction on Copper Electrodes
journal, January 2013

  • Montoya, Joseph H.; Peterson, Andrew A.; Nørskov, Jens K.
  • ChemCatChem, Vol. 5, Issue 3
  • DOI: 10.1002/cctc.201200564

The structure of interfacial water on gold electrodes studied by x-ray absorption spectroscopy
journal, October 2014


Ab initio molecular dynamics of solvation effects on reactivity at electrified interfaces
journal, August 2016

  • Herron, Jeffrey A.; Morikawa, Yoshitada; Mavrikakis, Manos
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 34
  • DOI: 10.1073/pnas.1604590113

Capturing Solvation Effects at a Liquid/Nanoparticle Interface by Ab Initio Molecular Dynamics: Pt 201 Immersed in Water
journal, August 2016

  • de Morais, Rodrigo Ferreira; Kerber, Torsten; Calle-Vallejo, Federico
  • Small, Vol. 12, Issue 38
  • DOI: 10.1002/smll.201601307

Assessing a First-Principles Model of an Electrochemical Interface by Comparison with Experiment
journal, January 2016

  • Steinmann, Stephan N.; Sautet, Philippe
  • The Journal of Physical Chemistry C, Vol. 120, Issue 10
  • DOI: 10.1021/acs.jpcc.6b01938

Electrochemical CO Reduction: A Property of the Electrochemical Interface
journal, December 2018

  • Bagger, Alexander; Arnarson, Logi; Hansen, Martin H.
  • Journal of the American Chemical Society, Vol. 141, Issue 4
  • DOI: 10.1021/jacs.8b08839

In situ nano- to microscopic imaging and growth mechanism of electrochemical dissolution (e.g., corrosion) of a confined metal surface
journal, August 2017

  • Merola, C.; Cheng, H. -W.; Schwenzfeier, K.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 36
  • DOI: 10.1073/pnas.1708205114

Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K
journal, February 2017

  • Cheng, Tao; Xiao, Hai; Goddard, William A.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 8
  • DOI: 10.1073/pnas.1612106114

High-rate electrochemical energy storage through Li+ intercalation pseudocapacitance
journal, April 2013

  • Augustyn, Veronica; Come, Jérémy; Lowe, Michael A.
  • Nature Materials, Vol. 12, Issue 6
  • DOI: 10.1038/nmat3601

Activity and Selectivity Control in CO 2 Electroreduction to Multicarbon Products over CuO x Catalysts via Electrolyte Design
journal, September 2018


Static and Dynamical Properties of Liquid Water from First Principles by a Novel Car−Parrinello-like Approach
journal, January 2009

  • Kühne, Thomas D.; Krack, Matthias; Parrinello, Michele
  • Journal of Chemical Theory and Computation, Vol. 5, Issue 2
  • DOI: 10.1021/ct800417q

Voltage-dependent ordering of water molecules at an electrode–electrolyte interface
journal, March 1994

  • Toney, Michael F.; Howard, Jason N.; Richer, Jocelyn
  • Nature, Vol. 368, Issue 6470
  • DOI: 10.1038/368444a0

Heterogeneous catalytic conversion of CO 2 : a comprehensive theoretical review
journal, January 2015

  • Li, Yawei; Chan, Siew Hwa; Sun, Qiang
  • Nanoscale, Vol. 7, Issue 19
  • DOI: 10.1039/C5NR00092K

Mechanism and Tafel Lines of Electro-Oxidation of Water to Oxygen on RuO 2 (110)
journal, December 2010

  • Fang, Ya-Hui; Liu, Zhi-Pan
  • Journal of the American Chemical Society, Vol. 132, Issue 51
  • DOI: 10.1021/ja1069272

Reaction intermediates during operando electrocatalysis identified from full solvent quantum mechanics molecular dynamics
journal, March 2019

  • Cheng, Tao; Fortunelli, Alessandro; Goddard, William A.
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 16
  • DOI: 10.1073/pnas.1821709116

Insights into Current Limitations of Density Functional Theory
journal, August 2008


Probing the Reaction Mechanism of CO 2 Electroreduction over Ag Films via Operando Infrared Spectroscopy
journal, December 2016


Force Field for Water over Pt(111): Development, Assessment, and Comparison
journal, April 2018

  • Steinmann, Stephan N.; Ferreira De Morais, Rodrigo; Götz, Andreas W.
  • Journal of Chemical Theory and Computation, Vol. 14, Issue 6
  • DOI: 10.1021/acs.jctc.7b01177