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

Title: Strongly correlated perovskite fuel cells

Abstract

Fuel cells convert chemical energy directly into electrical energy with high efficiencies and environmental benefits, as compared with traditional heat engines(1-4). Yttria-stabilized zirconia is perhaps the material with the most potential as an electrolyte in solid oxide fuel cells (SOFCs), owing to its stability and near-unity ionic transference number(5). Although there exist materials with superior ionic conductivity, they are often limited by their ability to suppress electronic leakage when exposed to the reducing environment at the fuel interface. Such electronic leakage reduces fuel cell power output and the associated chemo-mechanical stresses can also lead to catastrophic fracture of electrolyte membranes(6). Here we depart from traditional electrolyte design that relies on cation substitution to sustain ionic conduction. Instead, we use a perovskite nickelate as an electrolyte with high initial ionic and electronic conductivity. Since many such oxides are also correlated electron systems, we can suppress the electronic conduction through a filling-controlled Mott transition induced by spontaneous hydrogen incorporation. Using such a nickelate as the electrolyte in free-standing membrane geometry, we demonstrate a low-temperature micro-fabricated SOFC with high performance. The ionic conductivity of the nickelate perovskite is comparable to the best-performing solid electrolytes in the same temperature range, with a very lowmore » activation energy. The results present a design strategy for high-performance materials exhibiting emergent properties arising from strong electron correlations.« less

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division; U.S. Army Research Laboratory - U.S. Army Research Office (ARO)
OSTI Identifier:
1413749
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Nature (London)
Additional Journal Information:
Journal Volume: 534; Journal Issue: 7606; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

Citation Formats

Zhou, You, Guan, Xiaofei, Zhou, Hua, Ramadoss, Koushik, Adam, Suhare, Liu, Huajun, Lee, Sungsik, Shi, Jian, Tsuchiya, Masaru, Fong, Dillon D., and Ramanathan, Shriram. Strongly correlated perovskite fuel cells. United States: N. p., 2016. Web. doi:10.1038/nature17653.
Zhou, You, Guan, Xiaofei, Zhou, Hua, Ramadoss, Koushik, Adam, Suhare, Liu, Huajun, Lee, Sungsik, Shi, Jian, Tsuchiya, Masaru, Fong, Dillon D., & Ramanathan, Shriram. Strongly correlated perovskite fuel cells. United States. doi:10.1038/nature17653.
Zhou, You, Guan, Xiaofei, Zhou, Hua, Ramadoss, Koushik, Adam, Suhare, Liu, Huajun, Lee, Sungsik, Shi, Jian, Tsuchiya, Masaru, Fong, Dillon D., and Ramanathan, Shriram. Mon . "Strongly correlated perovskite fuel cells". United States. doi:10.1038/nature17653.
@article{osti_1413749,
title = {Strongly correlated perovskite fuel cells},
author = {Zhou, You and Guan, Xiaofei and Zhou, Hua and Ramadoss, Koushik and Adam, Suhare and Liu, Huajun and Lee, Sungsik and Shi, Jian and Tsuchiya, Masaru and Fong, Dillon D. and Ramanathan, Shriram},
abstractNote = {Fuel cells convert chemical energy directly into electrical energy with high efficiencies and environmental benefits, as compared with traditional heat engines(1-4). Yttria-stabilized zirconia is perhaps the material with the most potential as an electrolyte in solid oxide fuel cells (SOFCs), owing to its stability and near-unity ionic transference number(5). Although there exist materials with superior ionic conductivity, they are often limited by their ability to suppress electronic leakage when exposed to the reducing environment at the fuel interface. Such electronic leakage reduces fuel cell power output and the associated chemo-mechanical stresses can also lead to catastrophic fracture of electrolyte membranes(6). Here we depart from traditional electrolyte design that relies on cation substitution to sustain ionic conduction. Instead, we use a perovskite nickelate as an electrolyte with high initial ionic and electronic conductivity. Since many such oxides are also correlated electron systems, we can suppress the electronic conduction through a filling-controlled Mott transition induced by spontaneous hydrogen incorporation. Using such a nickelate as the electrolyte in free-standing membrane geometry, we demonstrate a low-temperature micro-fabricated SOFC with high performance. The ionic conductivity of the nickelate perovskite is comparable to the best-performing solid electrolytes in the same temperature range, with a very low activation energy. The results present a design strategy for high-performance materials exhibiting emergent properties arising from strong electron correlations.},
doi = {10.1038/nature17653},
journal = {Nature (London)},
issn = {0028-0836},
number = 7606,
volume = 534,
place = {United States},
year = {2016},
month = {5}
}

Works referenced in this record:

In Situ X-Ray Absorption Near-Edge Structure Evidence for Quadrivalent Nickel in Nickel Battery Electrodes
journal, January 1996

  • O'Grady, W. E.
  • Journal of The Electrochemical Society, Vol. 143, Issue 5
  • DOI: 10.1149/1.1836687

Lowering the Temperature of Solid Oxide Fuel Cells
journal, November 2011


Design of Electroceramics for Solid Oxides Fuel Cell Applications: Playing with Ceria
journal, April 2008


Materials for fuel-cell technologies
journal, November 2001

  • Steele, Brian C. H.; Heinzel, Angelika
  • Nature, Vol. 414, Issue 6861, p. 345-352
  • DOI: 10.1038/35104620

Proton conduction in thin film yttrium-doped barium zirconate
journal, June 2008

  • Shim, Joon Hyung; Gür, Turgut M.; Prinz, Fritz B.
  • Applied Physics Letters, Vol. 92, Issue 25
  • DOI: 10.1063/1.2947584

Tailoring the chemical stability of Ba(Ce0.8−xZrx)Y0.2O3−δ protonic conductors for Intermediate Temperature Solid Oxide Fuel Cells (IT-SOFCs)
journal, June 2008


Oxygen ion transference number of doped lanthanum gallate
journal, December 2008


Structural, magnetic and electronic properties of perovskites (R = rare earth)
journal, February 1997


Advances in solid oxide fuel cell technology
journal, November 2000


A quantum molecular dynamics study of proton conduction phenomena in BaCeO3
journal, July 1996


Readily processed protonic ceramic fuel cells with high performance at low temperatures
journal, July 2015


Progress in perovskite nickelate research
journal, July 2008


A quantum molecular dynamics study of proton diffusion in SrTiO3 and CaTiO3
journal, October 1999


A thermally self-sustained micro solid-oxide fuel-cell stack with high power density
journal, June 2005

  • Shao, Zongping; Haile, Sossina M.; Ahn, Jeongmin
  • Nature, Vol. 435, Issue 7043
  • DOI: 10.1038/nature03673

Free standing oxide alloy electrolytes for low temperature thin film solid oxide fuel cells
journal, March 2012


Effect of Interfacial Resistance on Determination of Transport Properties of Mixed-Conducting Electrolytes
journal, January 1996

  • Liu, Meilin
  • Journal of The Electrochemical Society, Vol. 143, Issue 6
  • DOI: 10.1149/1.1836892

Origins of bad-metal conductivity and the insulator–metal transition in the rare-earth nickelates
journal, March 2014

  • Jaramillo, R.; Ha, Sieu D.; Silevitch, D. M.
  • Nature Physics, Vol. 10, Issue 4
  • DOI: 10.1038/nphys2907

Defect engineering: design tools for solid state electrochemical devices
journal, September 2003


Electronic and ionic transport properties and other physical aspects of perovskites
journal, September 2004


High proton conduction in grain-boundary-free yttrium-doped barium zirconate films grown by pulsed laser deposition
journal, September 2010

  • Pergolesi, Daniele; Fabbri, Emiliana; D’Epifanio, Alessandra
  • Nature Materials, Vol. 9, Issue 10
  • DOI: 10.1038/nmat2837

Solid acids as fuel cell electrolytes
journal, April 2001

  • Haile, Sossina M.; Boysen, Dane A.; Chisholm, Calum R. I.
  • Nature, Vol. 410, Issue 6831
  • DOI: 10.1038/35073536

Proton Conductivity:  Materials and Applications
journal, January 1996

  • Kreuer, Klaus-Dieter
  • Chemistry of Materials, Vol. 8, Issue 3
  • DOI: 10.1021/cm950192a

Nature of hole doping in Nd 2 NiO 4 and La 2 NiO 4 : Comparison with La 2 CuO 4
journal, May 1993


Intermediate Temperature Solid Oxide Fuel Cells Using LaGaO[sub 3] Electrolyte II. Improvement of Oxide Ion Conductivity and Power Density by Doping Fe for Ga Site of LaGaO[sub 3]
journal, January 2000

  • Ishihara, Tatsumi; Shibayama, Takaaki; Honda, Miho
  • Journal of The Electrochemical Society, Vol. 147, Issue 4
  • DOI: 10.1149/1.1393358

Colossal resistance switching and band gap modulation in a perovskite nickelate by electron doping
journal, September 2014

  • Shi, Jian; Zhou, You; Ramanathan, Shriram
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5860

Charge disproportionation in R NiO 3 perovskites ( R = rare earth) from high-resolution x-ray absorption spectroscopy
journal, December 2009


On the complexity of proton conduction phenomena
journal, November 2000


    Works referencing / citing this record:

    Ni( ii )-based coordination polymers for efficient electrocatalytic oxygen evolution reaction
    journal, January 2018

    • Jiang, Zhi-Qiang; Li, Yu-Feng; Zhu, Xue-Jun
    • RSC Advances, Vol. 8, Issue 67
    • DOI: 10.1039/c8ra07492e

    Delta-temperatural electronic transportation achieved in metastable perovskite rare-earth nickelate thin films
    journal, January 2019

    • Chen, Jikun; Hu, Haiyang; Yajima, Takeaki
    • Journal of Materials Chemistry C, Vol. 7, Issue 26
    • DOI: 10.1039/c9tc02327e

    Semiconductor TiO 2 thin film as an electrolyte for fuel cells
    journal, January 2019

    • Dong, Wenjing; Tong, Yuzhu; Zhu, Bin
    • Journal of Materials Chemistry A, Vol. 7, Issue 28
    • DOI: 10.1039/c9ta01941c

    Interfacial Octahedral Manipulation Imparts Hysteresis‐Free Metal to Insulator Transition in Ultrathin Nickelate Heterostructure
    journal, July 2019

    • Dong, Yongqi; Ma, Zhiyuan; Luo, Zhenlin
    • Advanced Materials Interfaces, Vol. 6, Issue 17
    • DOI: 10.1002/admi.201900644

    Nanoscale Trimetallic Metal-Organic Frameworks Enable Efficient Oxygen Evolution Electrocatalysis
    journal, December 2017

    • Li, Fei-Long; Shao, Qi; Huang, Xiaoqing
    • Angewandte Chemie International Edition, Vol. 57, Issue 7
    • DOI: 10.1002/anie.201711376

    Exploring the Influence of Halogen Coordination Effect of Stable Bimetallic MOFs on Oxygen Evolution Reaction
    journal, October 2019

    • Lu, Jia‐Ni; Liu, Jiang; Dong, Long‐Zhang
    • Chemistry – A European Journal, Vol. 25, Issue 69
    • DOI: 10.1002/chem.201903482

    Arabinogalactan protein–rare earth element complexes activate plant endocytosis
    journal, June 2019

    • Wang, Lihong; Cheng, Mengzhu; Yang, Qing
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 28
    • DOI: 10.1073/pnas.1902532116

    Interfacial Octahedral Manipulation Imparts Hysteresis‐Free Metal to Insulator Transition in Ultrathin Nickelate Heterostructure
    journal, July 2019

    • Dong, Yongqi; Ma, Zhiyuan; Luo, Zhenlin
    • Advanced Materials Interfaces, Vol. 6, Issue 17
    • DOI: 10.1002/admi.201900644

    Nanoscale Trimetallic Metal-Organic Frameworks Enable Efficient Oxygen Evolution Electrocatalysis
    journal, December 2017


    Exploring the Influence of Halogen Coordination Effect of Stable Bimetallic MOFs on Oxygen Evolution Reaction
    journal, October 2019

    • Lu, Jia‐Ni; Liu, Jiang; Dong, Long‐Zhang
    • Chemistry – A European Journal, Vol. 25, Issue 69
    • DOI: 10.1002/chem.201903482

    Ni( ii )-based coordination polymers for efficient electrocatalytic oxygen evolution reaction
    journal, January 2018

    • Jiang, Zhi-Qiang; Li, Yu-Feng; Zhu, Xue-Jun
    • RSC Advances, Vol. 8, Issue 67
    • DOI: 10.1039/c8ra07492e

    Semiconductor TiO 2 thin film as an electrolyte for fuel cells
    journal, January 2019

    • Dong, Wenjing; Tong, Yuzhu; Zhu, Bin
    • Journal of Materials Chemistry A, Vol. 7, Issue 28
    • DOI: 10.1039/c9ta01941c

    Delta-temperatural electronic transportation achieved in metastable perovskite rare-earth nickelate thin films
    journal, January 2019

    • Chen, Jikun; Hu, Haiyang; Yajima, Takeaki
    • Journal of Materials Chemistry C, Vol. 7, Issue 26
    • DOI: 10.1039/c9tc02327e

    Arabinogalactan protein–rare earth element complexes activate plant endocytosis
    journal, June 2019

    • Wang, Lihong; Cheng, Mengzhu; Yang, Qing
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 28
    • DOI: 10.1073/pnas.1902532116

    Fuel cells: Hydrogen induced insulation
    journal, June 2016