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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. 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. 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. 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:
 [1];  [1];  [2];  [1];  [1];  [3];  [2];  [4];  [5];  [3];  [6]
  1. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-ray Science Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  4. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences; Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Materials Science and Engineering
  5. SiEnergy Systems, Cambridge, MA (United States)
  6. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences; Purdue Univ., West Lafayette, IN (United States). School of Materials Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences and Engineering Division; US Army Research Office (ARO); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1261104
Grant/Contract Number:  
AC02-06CH11357; W911NF-14-1-0348; W911NF-14-1-0669; FA9550-12-1-0189
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 534; Journal Issue: 7606; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION

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. https://www.osti.gov/servlets/purl/1261104.
@article{osti_1261104,
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. 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. 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. 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)},
number = 7606,
volume = 534,
place = {United States},
year = {2016},
month = {5}
}

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