DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media

Abstract

Development of acid-stable electrocatalysts with low overpotential for oxygen evolution reaction (OER) is a major challenge to produce hydrogen directly from water. We report in this paper a pyrochlore yttrium ruthenate (Y2Ru2O7-δ) electrocatalyst that has significantly enhanced performance toward OER in acid media over the best-known catalysts, with an onset overpotential of 190 mV and high stability in 0.1 M perchloric acid solution. X-ray absorption near-edge structure (XANES) indicates Y2Ru2O7-δ electrocatalyst had a low valence state that favors the high OER activity. Density functional theory (DFT) calculation shows this pyrochlore has lower band center energy for the overlap between Ru 4d and O 2p orbitals and is therefore more stable Ru–O bond than RuO2, highlighting the effect of yttrium on the enhancement in stability. Finally, the Y2Ru2O7-δ pyrochlore is also free of expensive iridium metal and thus is a cost-effective candidate for practical applications.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [1]
  1. Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana−Champaign, 600 South Mathews Avenue, Urbana, Illinois 61801, United States
  2. X-ray Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, United States
Publication Date:
Research Org.:
Univ. of Illinois at Urbana-Champaign, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1375508
Alternate Identifier(s):
OSTI ID: 1421364
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Name: Journal of the American Chemical Society; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kim, Jaemin, Shih, Pei-Chieh, Tsao, Kai-Chieh, Pan, Yung-Tin, Yin, Xi, Sun, Cheng-Jun, and Yang, Hong. High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media. United States: N. p., 2017. Web. doi:10.1021/jacs.7b06808.
Kim, Jaemin, Shih, Pei-Chieh, Tsao, Kai-Chieh, Pan, Yung-Tin, Yin, Xi, Sun, Cheng-Jun, & Yang, Hong. High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media. United States. https://doi.org/10.1021/jacs.7b06808
Kim, Jaemin, Shih, Pei-Chieh, Tsao, Kai-Chieh, Pan, Yung-Tin, Yin, Xi, Sun, Cheng-Jun, and Yang, Hong. Thu . "High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media". United States. https://doi.org/10.1021/jacs.7b06808.
@article{osti_1375508,
title = {High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media},
author = {Kim, Jaemin and Shih, Pei-Chieh and Tsao, Kai-Chieh and Pan, Yung-Tin and Yin, Xi and Sun, Cheng-Jun and Yang, Hong},
abstractNote = {Development of acid-stable electrocatalysts with low overpotential for oxygen evolution reaction (OER) is a major challenge to produce hydrogen directly from water. We report in this paper a pyrochlore yttrium ruthenate (Y2Ru2O7-δ) electrocatalyst that has significantly enhanced performance toward OER in acid media over the best-known catalysts, with an onset overpotential of 190 mV and high stability in 0.1 M perchloric acid solution. X-ray absorption near-edge structure (XANES) indicates Y2Ru2O7-δ electrocatalyst had a low valence state that favors the high OER activity. Density functional theory (DFT) calculation shows this pyrochlore has lower band center energy for the overlap between Ru 4d and O 2p orbitals and is therefore more stable Ru–O bond than RuO2, highlighting the effect of yttrium on the enhancement in stability. Finally, the Y2Ru2O7-δ pyrochlore is also free of expensive iridium metal and thus is a cost-effective candidate for practical applications.},
doi = {10.1021/jacs.7b06808},
journal = {Journal of the American Chemical Society},
number = ,
volume = ,
place = {United States},
year = {Thu Jul 27 00:00:00 EDT 2017},
month = {Thu Jul 27 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/jacs.7b06808

Citation Metrics:
Cited by: 237 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Benchmarking Hydrogen Evolving Reaction and Oxygen Evolving Reaction Electrocatalysts for Solar Water Splitting Devices
journal, March 2015

  • McCrory, Charles C. L.; Jung, Suho; Ferrer, Ivonne M.
  • Journal of the American Chemical Society, Vol. 137, Issue 13
  • DOI: 10.1021/ja510442p

The evolution of ‘sol–gel’ chemistry as a technique for materials synthesis
journal, January 2016

  • Danks, A. E.; Hall, S. R.; Schnepp, Z.
  • Materials Horizons, Vol. 3, Issue 2
  • DOI: 10.1039/C5MH00260E

Ca 2 Mn 2 O 5 as Oxygen-Deficient Perovskite Electrocatalyst for Oxygen Evolution Reaction
journal, October 2014

  • Kim, Jaemin; Yin, Xi; Tsao, Kai-Chieh
  • Journal of the American Chemical Society, Vol. 136, Issue 42
  • DOI: 10.1021/ja506254g

The Role of TiO 2 Doping on RuO 2 -Coated Electrodes for the Water Oxidation Reaction
journal, February 2013

  • Näslund, Lars-Åke; Sánchez-Sánchez, Carlos M.; Ingason, Árni S.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 12
  • DOI: 10.1021/jp308941g

Highly Active and Stable Iridium Pyrochlores for Oxygen Evolution Reaction
journal, May 2017


Using Surface Segregation To Design Stable Ru-Ir Oxides for the Oxygen Evolution Reaction in Acidic Environments
journal, October 2014

  • Danilovic, Nemanja; Subbaraman, Ramachandran; Chang, Kee Chul
  • Angewandte Chemie International Edition, Vol. 53, Issue 51
  • DOI: 10.1002/anie.201406455

Heterojunction confinement on the atomic structure evolution of near monolayer core–shell nanocatalysts in redox reactions of a direct methanol fuel cell
journal, January 2015

  • Chen, Tsan-Yao; Lee, Guo-Wei; Liu, Yu-Ting
  • Journal of Materials Chemistry A, Vol. 3, Issue 4
  • DOI: 10.1039/C4TA04640D

Computational predictions of energy materials using density functional theory
journal, January 2016


A metal–organic framework-derived bifunctional oxygen electrocatalyst
journal, January 2016


Mechanism of oxygen evolution on perovskites
journal, July 1983

  • Bockris, John O'M.; Otagawa, Takaaki
  • The Journal of Physical Chemistry, Vol. 87, Issue 15
  • DOI: 10.1021/j100238a048

Ultrathin two-dimensional layered metal hydroxides: an emerging platform for advanced catalysis, energy conversion and storage
journal, January 2016

  • Yin, Huajie; Tang, Zhiyong
  • Chemical Society Reviews, Vol. 45, Issue 18
  • DOI: 10.1039/C6CS00343E

Double perovskites as a family of highly active catalysts for oxygen evolution in alkaline solution
journal, September 2013

  • Grimaud, Alexis; May, Kevin J.; Carlton, Christopher E.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3439

Nature of the electronic states in the layered perovskite noncuprate superconductor Sr 2 Ru O 4
journal, June 1996


The metal-to-semiconductor transition in ternary ruthenium (IV) oxides: a study by electron spectroscopy
journal, November 1983

  • Cox, P. A.; Egdell, R. G.; Goodenough, J. B.
  • Journal of Physics C: Solid State Physics, Vol. 16, Issue 32
  • DOI: 10.1088/0022-3719/16/32/014

Improvement in the efficiency of an OrganoMetallic Fuel Cell by tuning the molecular architecture of the anode electrocatalyst and the nature of the carbon support
journal, January 2012

  • Bevilacqua, M.; Bianchini, C.; Marchionni, A.
  • Energy & Environmental Science, Vol. 5, Issue 9
  • DOI: 10.1039/c2ee22055e

Valence properties of Cu and Ru in titanium-substituted LnCu 3 Ru 4 O 12+δ (Ln = La, Pr, Nd) investigated by XANES and TGA
journal, January 2015

  • Riegg, Stefan; Reller, Armin; Loidl, Alois
  • Dalton Transactions, Vol. 44, Issue 23
  • DOI: 10.1039/C4DT03876B

The Mechanism of Water Oxidation: From Electrolysis via Homogeneous to Biological Catalysis
journal, June 2010


Pyrochlore electrocatalysts for efficient alkaline water electrolysis
journal, January 2015

  • Parrondo, Javier; George, Morgan; Capuano, Christopher
  • Journal of Materials Chemistry A, Vol. 3, Issue 20
  • DOI: 10.1039/C5TA01771H

Carbon-Incorporated Nickel-Cobalt Mixed Metal Phosphide Nanoboxes with Enhanced Electrocatalytic Activity for Oxygen Evolution
journal, February 2017

  • He, Peilei; Yu, Xin-Yao; Lou, Xiong Wen David
  • Angewandte Chemie International Edition, Vol. 56, Issue 14
  • DOI: 10.1002/anie.201612635

First-Principles Studies on Cation Dopants and Electrolyte|Cathode Interphases for Lithium Garnets
journal, May 2015


A highly active and stable IrO x /SrIrO 3 catalyst for the oxygen evolution reaction
journal, September 2016


Solar Water Splitting Cells
journal, November 2010

  • Walter, Michael G.; Warren, Emily L.; McKone, James R.
  • Chemical Reviews, Vol. 110, Issue 11, p. 6446-6473
  • DOI: 10.1021/cr1002326

Water-Splitting Electrocatalysis in Acid Conditions Using Ruthenate-Iridate Pyrochlores
journal, September 2014

  • Sardar, Kripasindhu; Petrucco, Enrico; Hiley, Craig I.
  • Angewandte Chemie International Edition, Vol. 53, Issue 41
  • DOI: 10.1002/anie.201406668

Water-oxidation catalysis by manganese in a geochemical-like cycle
journal, May 2011

  • Hocking, Rosalie K.; Brimblecombe, Robin; Chang, Lan-Yun
  • Nature Chemistry, Vol. 3, Issue 6
  • DOI: 10.1038/nchem.1049

A pentanuclear iron catalyst designed for water oxidation
journal, February 2016

  • Okamura, Masaya; Kondo, Mio; Kuga, Reiko
  • Nature, Vol. 530, Issue 7591
  • DOI: 10.1038/nature16529

Electrolysis of water on (oxidized) metal surfaces
journal, December 2005


Schizophrenic electrons in ruthenium-based oxides
journal, January 2004


Designed Formation of Co 3 O 4 /NiCo 2 O 4 Double-Shelled Nanocages with Enhanced Pseudocapacitive and Electrocatalytic Properties
journal, April 2015

  • Hu, Han; Guan, Buyuan; Xia, Baoyu
  • Journal of the American Chemical Society, Vol. 137, Issue 16
  • DOI: 10.1021/jacs.5b02465

Photodeposited ruthenium dioxide films for oxygen evolution reaction electrocatalysis
journal, January 2017

  • Salvatore, D. A.; Peña, B.; Dettelbach, K. E.
  • Journal of Materials Chemistry A, Vol. 5, Issue 4
  • DOI: 10.1039/C6TA09094J

Oxygen electrocatalysts for water electrolyzers and reversible fuel cells: status and perspective
journal, January 2012

  • Park, Sehkyu; Shao, Yuyan; Liu, Jun
  • Energy & Environmental Science, Vol. 5, Issue 11
  • DOI: 10.1039/c2ee22554a

Water Oxidation Electrocatalyzed by an Efficient Mn 3 O 4 /CoSe 2 Nanocomposite
journal, January 2012

  • Gao, Min-Rui; Xu, Yun-Fei; Jiang, Jun
  • Journal of the American Chemical Society, Vol. 134, Issue 6
  • DOI: 10.1021/ja211526y

Synthesis and Activities of Rutile IrO 2 and RuO 2 Nanoparticles for Oxygen Evolution in Acid and Alkaline Solutions
journal, January 2012

  • Lee, Youngmin; Suntivich, Jin; May, Kevin J.
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 3
  • DOI: 10.1021/jz2016507

Degradation Mechanisms of Pt/C Fuel Cell Catalysts under Simulated Start–Stop Conditions
journal, April 2012

  • Meier, Josef C.; Galeano, Carolina; Katsounaros, Ioannis
  • ACS Catalysis, Vol. 2, Issue 5
  • DOI: 10.1021/cs300024h

Solvothermal synthesis of perovskites and pyrochlores: crystallisation of functional oxides under mild conditions
journal, January 2010

  • Modeshia, Deena R.; Walton, Richard I.
  • Chemical Society Reviews, Vol. 39, Issue 11
  • DOI: 10.1039/b904702f

Electrolysis of water on oxide surfaces
journal, September 2007


Ultrathin metal–organic framework nanosheets for electrocatalytic oxygen evolution
journal, November 2016


Synthesis of a metallic mesoporous pyrochlore as a catalyst for lithium–O2 batteries
journal, November 2012

  • Oh, Si Hyoung; Black, Robert; Pomerantseva, Ekaterina
  • Nature Chemistry, Vol. 4, Issue 12, p. 1004-1010
  • DOI: 10.1038/nchem.1499

Toward an Active and Stable Catalyst for Oxygen Evolution in Acidic Media: Ti-Stabilized MnO 2
journal, August 2015

  • Frydendal, Rasmus; Paoli, Elisa A.; Chorkendorff, Ib
  • Advanced Energy Materials, Vol. 5, Issue 22
  • DOI: 10.1002/aenm.201500991

Electrochemical Catalyst–Support Effects and Their Stabilizing Role for IrO x Nanoparticle Catalysts during the Oxygen Evolution Reaction
journal, September 2016

  • Oh, Hyung-Suk; Nong, Hong Nhan; Reier, Tobias
  • Journal of the American Chemical Society, Vol. 138, Issue 38
  • DOI: 10.1021/jacs.6b07199

Robust Photogeneration of H2 in Water Using Semiconductor Nanocrystals and a Nickel Catalyst
journal, November 2012


IrO 2 Coated on RuO 2 as Efficient and Stable Electroactive Nanocatalysts for Electrochemical Water Splitting
journal, February 2016

  • Audichon, Thomas; Napporn, Teko W.; Canaff, Christine
  • The Journal of Physical Chemistry C, Vol. 120, Issue 5
  • DOI: 10.1021/acs.jpcc.5b11868

Coordination tuning of cobalt phosphates towards efficient water oxidation catalyst
journal, September 2015

  • Kim, Hyunah; Park, Jimin; Park, Inchul
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9253

General Synthesis of Multishell Mixed-Metal Oxyphosphide Particles with Enhanced Electrocatalytic Activity in the Oxygen Evolution Reaction
journal, January 2017

  • Guan, Bu Yuan; Yu, Le; Lou, Xiong Wen David
  • Angewandte Chemie International Edition, Vol. 56, Issue 9
  • DOI: 10.1002/anie.201611804

Homogeneously dispersed multimetal oxygen-evolving catalysts
journal, March 2016


Origin of additional capacities in metal oxide lithium-ion battery electrodes
journal, November 2013

  • Hu, Yan-Yan; Liu, Zigeng; Nam, Kyung-Wan
  • Nature Materials, Vol. 12, Issue 12
  • DOI: 10.1038/nmat3784

Oxide pyrochlores — A review
journal, January 1983

  • Subramanian, M. A.; Aravamudan, G.; Subba Rao, G. V.
  • Progress in Solid State Chemistry, Vol. 15, Issue 2
  • DOI: 10.1016/0079-6786(83)90001-8

Design and Tailoring of the Nanotubular Arrayed Architecture of Hydrous RuO 2 for Next Generation Supercapacitors
journal, December 2006

  • Hu, Chi-Chang; Chang, Kuo-Hsin; Lin, Ming-Champ
  • Nano Letters, Vol. 6, Issue 12
  • DOI: 10.1021/nl061576a

Gold-supported cerium-doped NiOx catalysts for water oxidation
journal, April 2016

  • Ng, Jia Wei Desmond; García-Melchor, Max; Bajdich, Michal
  • Nature Energy, Vol. 1, Issue 5
  • DOI: 10.1038/nenergy.2016.53

Oxide-Supported IrNiO x Core-Shell Particles as Efficient, Cost-Effective, and Stable Catalysts for Electrochemical Water Splitting
journal, January 2015

  • Nong, Hong Nhan; Oh, Hyung-Suk; Reier, Tobias
  • Angewandte Chemie International Edition, Vol. 54, Issue 10
  • DOI: 10.1002/anie.201411072

Iridium-based double perovskites for efficient water oxidation in acid media
journal, August 2016

  • Diaz-Morales, Oscar; Raaijman, Stefan; Kortlever, Ruud
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12363

Combining theory and experiment in electrocatalysis: Insights into materials design
journal, January 2017


A metal-free bifunctional electrocatalyst for oxygen reduction and oxygen evolution reactions
journal, April 2015

  • Zhang, Jintao; Zhao, Zhenghang; Xia, Zhenhai
  • Nature Nanotechnology, Vol. 10, Issue 5
  • DOI: 10.1038/nnano.2015.48