Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Chlorine evolution reaction electrocatalysis on RuO2(110) and IrO2(110) grown using molecular-beam epitaxy

Abstract

Herein, we report the electrocatalysis of the chlorine evolution reaction (CER) on well-defined RuO2(110) and IrO2(110) surfaces. RuO2 and IrO2 are known for their capabilities to catalyze the CER. Until now, the CER measurements have only been reported on well-defined RuO2 surfaces and only at high Cl- concentrations. We present the CER measurement and the role of Cl- at lower concentration on single-orientation RuO2(110) and IrO2(110) films. We find that RuO2(110) is two orders of magnitude more active than IrO2(110). Moreover, we observe the correlation between the CER activity and the Oad formation potential on RuO2 and IrO2, supporting the prior suggestion that the Oad is the active site for the CER. We further use the reaction order analysis to support the Volmer-Heyrovsky mechanism of the CER, which was previously suggested from the Tafel slope analysis. Our finding highlights the importance of the surface Oad species on oxides for the CER electrocatalysis and suggests the electrochemical formation of Clad on Oad (for example, Cl- + Oad ↔ OClad + e-) as the crucial step in the CER electrocatalysis.

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Cornell Univ., Ithaca, NY (United States)
Publication Date:
Research Org.:
Cornell Univ., Ithaca, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Taiwan Government
OSTI Identifier:
1612818
Grant/Contract Number:  
SC0018029; DGE-1650441; ECCS1542081
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 150; Journal Issue: 4; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics; Surface and interface chemistry; Epitaxy; Transition metal oxides; Density functional theory; Reaction rate constants; Catalyst; Electron diffraction; Electrolytes

Citation Formats

Kuo, Ding-Yuan, Paik, Hanjong, Nelson, Jocienne N., Shen, Kyle M., Schlom, Darrell G., and Suntivich, Jin. Chlorine evolution reaction electrocatalysis on RuO2(110) and IrO2(110) grown using molecular-beam epitaxy. United States: N. p., 2019. Web. doi:10.1063/1.5051429.
Copy to clipboard
Kuo, Ding-Yuan, Paik, Hanjong, Nelson, Jocienne N., Shen, Kyle M., Schlom, Darrell G., & Suntivich, Jin. Chlorine evolution reaction electrocatalysis on RuO2(110) and IrO2(110) grown using molecular-beam epitaxy. United States. https://doi.org/10.1063/1.5051429
Copy to clipboard
Kuo, Ding-Yuan, Paik, Hanjong, Nelson, Jocienne N., Shen, Kyle M., Schlom, Darrell G., and Suntivich, Jin. Fri . "Chlorine evolution reaction electrocatalysis on RuO2(110) and IrO2(110) grown using molecular-beam epitaxy". United States. https://doi.org/10.1063/1.5051429. https://www.osti.gov/servlets/purl/1612818.
Copy to clipboard
@article{osti_1612818,
title = {Chlorine evolution reaction electrocatalysis on RuO2(110) and IrO2(110) grown using molecular-beam epitaxy},
author = {Kuo, Ding-Yuan and Paik, Hanjong and Nelson, Jocienne N. and Shen, Kyle M. and Schlom, Darrell G. and Suntivich, Jin},
abstractNote = {Herein, we report the electrocatalysis of the chlorine evolution reaction (CER) on well-defined RuO2(110) and IrO2(110) surfaces. RuO2 and IrO2 are known for their capabilities to catalyze the CER. Until now, the CER measurements have only been reported on well-defined RuO2 surfaces and only at high Cl- concentrations. We present the CER measurement and the role of Cl- at lower concentration on single-orientation RuO2(110) and IrO2(110) films. We find that RuO2(110) is two orders of magnitude more active than IrO2(110). Moreover, we observe the correlation between the CER activity and the Oad formation potential on RuO2 and IrO2, supporting the prior suggestion that the Oad is the active site for the CER. We further use the reaction order analysis to support the Volmer-Heyrovsky mechanism of the CER, which was previously suggested from the Tafel slope analysis. Our finding highlights the importance of the surface Oad species on oxides for the CER electrocatalysis and suggests the electrochemical formation of Clad on Oad (for example, Cl- + Oad ↔ OClad + e-) as the crucial step in the CER electrocatalysis.},
doi = {10.1063/1.5051429},
journal = {Journal of Chemical Physics},
number = 4,
volume = 150,
place = {United States},
year = {Fri Jan 04 00:00:00 EST 2019},
month = {Fri Jan 04 00:00:00 EST 2019}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.5051429
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 31 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

The Kinetics of Chlorine Evolution and Reduction on Titanium-Supported Metal Oxides Especially RuO[sub 2] and IrO[sub 2]
journal, January 1973

  • Kuhn, A. T.; Mortimer, C. J.
  • Journal of The Electrochemical Society, Vol. 120, Issue 2
  • DOI: 10.1149/1.2403425

Sustainable chlorine recycling via catalysed HCl oxidation: from fundamentals to implementation
journal, January 2011

  • Pérez-Ramírez, Javier; Mondelli, Cecilia; Schmidt, Timm
  • Energy & Environmental Science, Vol. 4, Issue 12
  • DOI: 10.1039/c1ee02190g

Electrocatalysis and Chlorine Evolution Reaction at Ruthenium Dioxide Deposited on Conductive Diamond
journal, March 2002

  • Ferro, Sergio; De Battisti, Achille
  • The Journal of Physical Chemistry B, Vol. 106, Issue 9
  • DOI: 10.1021/jp012195i

Electrocatalysis and the chlorine evolution reaction—II. Comparison of anode materials
journal, February 1984

Chlorine Evolution Reaction on RuO2(110): Ab initio Atomistic Thermodynamics Study - Pourbaix Diagrams
journal, February 2014

Selectivity of Nanocrystalline IrO2-Based Catalysts in Parallel Chlorine and Oxygen Evolution
journal, October 2014

Towards identifying the active sites on RuO 2 (110) in catalyzing oxygen evolution
journal, January 2017

  • Rao, Reshma R.; Kolb, Manuel J.; Halck, Niels Bendtsen
  • Energy & Environmental Science, Vol. 10, Issue 12
  • DOI: 10.1039/c7ee02307c

Full Kinetics from First Principles of the Chlorine Evolution Reaction over a RuO 2 (110) Model Electrode
journal, May 2016

  • Exner, Kai S.; Anton, Josef; Jacob, Timo
  • Angewandte Chemie International Edition, Vol. 55, Issue 26
  • DOI: 10.1002/anie.201511804

Chlor-alkali electrolysis with oxygen depolarized cathodes: history, present status and future prospects
journal, May 2008

  • Moussallem, Imad; Jörissen, Jakob; Kunz, Ulrich
  • Journal of Applied Electrochemistry, Vol. 38, Issue 9
  • DOI: 10.1007/s10800-008-9556-9

RuO2–TiO2 coated titanium anodes obtained by the sol–gel procedure and their electrochemical behaviour in the chlorine evolution reaction
journal, October 1999

  • Panić, V. V.; Dekanski, A.; Milonjić, S. K.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 157, Issue 1-3
  • DOI: 10.1016/s0927-7757(99)00094-1

Problems in interfacial electrochemistry that have been swept under the carpet
journal, April 2011

Some oxide catalysts for the anodic evolution of chlorine: reaction mechanism and catalytic activity
journal, January 1978

Milestones of the development of kinetics of electrode reactions
journal, January 2011

Orientation-Dependent Oxygen Evolution Activities of Rutile IrO 2 and RuO 2
journal, April 2014

  • Stoerzinger, Kelsey A.; Qiao, Liang; Biegalski, Michael D.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 10
  • DOI: 10.1021/jz500610u

Progress in the understanding of the mechanism of chlorine evolution at oxide electrodes
journal, March 1987

Full Kinetics from First Principles of the Chlorine Evolution Reaction over a RuO 2 (110) Model Electrode
journal, May 2016

Surface and electrocatalytic properties of well-defined and vicinal RuO2 single crystal faces
journal, January 2005

  • Guerrini, Edoardo; Consonni, Valerio; Trasatti, Sergio
  • Journal of Solid State Electrochemistry, Vol. 9, Issue 5
  • DOI: 10.1007/s10008-004-0602-1

Chlorine and oxygen evolution on various compositions of RuO2/TiO2 electrodes
journal, June 1978

Measurements of Oxygen Electroadsorption Energies and Oxygen Evolution Reaction on RuO 2 (110): A Discussion of the Sabatier Principle and Its Role in Electrocatalysis
journal, November 2018

  • Kuo, Ding-Yuan; Paik, Hanjong; Kloppenburg, Jan
  • Journal of the American Chemical Society, Vol. 140, Issue 50
  • DOI: 10.1021/jacs.8b09657

Electrocatalysis in the anodic evolution of oxygen and chlorine
journal, November 1984

Full Free Energy Diagram of an Electrocatalytic Reaction over a Single-Crystalline Model Electrode
journal, August 2017

  • Exner, Kai S.; Sohrabnejad-Eskan, Iman; Anton, Josef
  • ChemElectroChem, Vol. 4, Issue 11
  • DOI: 10.1002/celc.201700687

Mechanism of chlorine evolution on oxide anodes study of pH effects
journal, August 1987

  • Consonni, V.; Trasatti, S.; Pollak, F.
  • Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 228, Issue 1-2
  • DOI: 10.1016/0022-0728(87)80119-5

Flow Batteries: Current Status and Trends
journal, September 2015

  • Soloveichik, Grigorii L.
  • Chemical Reviews, Vol. 115, Issue 20
  • DOI: 10.1021/cr500720t

Influence of Surface Adsorption on the Oxygen Evolution Reaction on IrO 2 (110)
journal, February 2017

  • Kuo, Ding-Yuan; Kawasaki, Jason K.; Nelson, Jocienne N.
  • Journal of the American Chemical Society, Vol. 139, Issue 9
  • DOI: 10.1021/jacs.6b11932

Measurement of competition between oxygen evolution and chlorine evolution using rotating ring-disk electrode voltammetry
journal, June 2018

Selectivity between Oxygen and Chlorine Evolution in the Chlor-Alkali and Chlorate Processes
journal, February 2016

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Atomically dispersed Pt–N4 sites as efficient and selective electrocatalysts for the chlorine evolution reaction
    journal, January 2020

    Special Topic on Interfacial Electrochemistry and Photo(electro)catalysis
    journal, January 2019

    • Lian, Tianquan; Koper, Marc T. M.; Reuter, Karsten
    • The Journal of Chemical Physics, Vol. 150, Issue 4
    • DOI: 10.1063/1.5088351

    Activity‐Stability Volcano Plots for Material Optimization in Electrocatalysis
    journal, June 2019

      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: