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A high-entropy ceramic oxide is used as the cathode for the first time for proton-conducting solid oxide fuel cells (H-SOFCs). The Fe0.6Mn0.6Co0.6Ni0.6Cr0.6O4 (FMCNC) high-entropy spinel oxide has been successfully prepared, and the in situ chemical stability test demonstrates that the FMCNC material has good stability against CO2. The first-principles calculation indicates that the high-entropy structure enhances the properties of the FMCNC material that surpasses their individual components, leading to lower O2 adsorption energy for FMCNC than that for the individual components. The H-SOFC using the FMCNC cathode reaches an encouraging peak power density (PPD) of 1052 mW·cm−2 at 700 ℃, which is higher than those of the H-SOFCs reported recently. Additional comparison was made between the high-entropy FMCNC cathode and the traditional Mn1.6Cu1.4O4 (MCO) spinel cathode without the high-entropy structure, revealing that the formation of the high-entropy material allows the enhanced protonation ability as well as the movement of the O p-band center closer to the Fermi level, thus improving the cathode catalytic activity. As a result, the high-entropy FMCNC has a much-decreased polarization resistance of 0.057 Ω·cm2 at 700 ℃, which is half of that for the traditional MCO spinel cathode without the high-entropy design. The excellent performance of the FMCNC cell indicates that the high-entropy design makes a new life for the spinel oxide as the cathode for H-SOFCs, offering a novel and promising route for the development of high-performance materials for H-SOFCs.


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A high-entropy spinel ceramic oxide as the cathode for proton-conducting solid oxide fuel cells

Show Author's information Yangsen XUa,Xi XUb,Lei BIa( )
School of Resource Environment and Safety Engineering, University of South China, Hengyang 421001, China
Department of Materials, Imperial College London, London SW72BP, UK

† Yangsen Xu and Xi Xu contributed equally to this work.

Abstract

A high-entropy ceramic oxide is used as the cathode for the first time for proton-conducting solid oxide fuel cells (H-SOFCs). The Fe0.6Mn0.6Co0.6Ni0.6Cr0.6O4 (FMCNC) high-entropy spinel oxide has been successfully prepared, and the in situ chemical stability test demonstrates that the FMCNC material has good stability against CO2. The first-principles calculation indicates that the high-entropy structure enhances the properties of the FMCNC material that surpasses their individual components, leading to lower O2 adsorption energy for FMCNC than that for the individual components. The H-SOFC using the FMCNC cathode reaches an encouraging peak power density (PPD) of 1052 mW·cm−2 at 700 ℃, which is higher than those of the H-SOFCs reported recently. Additional comparison was made between the high-entropy FMCNC cathode and the traditional Mn1.6Cu1.4O4 (MCO) spinel cathode without the high-entropy structure, revealing that the formation of the high-entropy material allows the enhanced protonation ability as well as the movement of the O p-band center closer to the Fermi level, thus improving the cathode catalytic activity. As a result, the high-entropy FMCNC has a much-decreased polarization resistance of 0.057 Ω·cm2 at 700 ℃, which is half of that for the traditional MCO spinel cathode without the high-entropy design. The excellent performance of the FMCNC cell indicates that the high-entropy design makes a new life for the spinel oxide as the cathode for H-SOFCs, offering a novel and promising route for the development of high-performance materials for H-SOFCs.

Keywords: cathode, high-entropy oxides, proton-conducting oxides, solid oxide fuel cells (SOFCs)

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Publication history

Received: 15 July 2021
Revised: 14 January 2022
Accepted: 16 January 2022
Published: 20 April 2022
Issue date: May 2022

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© The Author(s) 2022.

Acknowledgements

This work is supported by the National Natural Science Foundation of China (Grant No. 51972183) and Hundred Youth Talents Program of Hunan and the Startup Funding for Talents at University of South China.

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