A reversible perovskite air electrode for active and durable oxygen reduction and evolution reactions via the A-site entropy engineering

He, Fan; Zhu, Feng; Liu, Dongliang; Zhou, Yucun; Sasaki, Kotaro; Choi, YongMan; Liu, Meilin; Chen, Yu

doi:10.1016/j.mattod.2023.02.006

A reversible perovskite air electrode for active and durable oxygen reduction and evolution reactions via the A-site entropy engineering

Journal Article · Fri Feb 24 00:00:00 EST 2023 · Materials Today

DOI:https://doi.org/10.1016/j.mattod.2023.02.006· OSTI ID:1995479

He, Fan ^[1]; Zhu, Feng ^[1]; Liu, Dongliang ^[2]; Zhou, Yucun ^[3]; ^[4]; Choi, YongMan ^[5]; Liu, Meilin ^[3]; Chen, Yu ^[1]

South China Univ. of Technology (SCUT), Guangzhou (China)
Nanjing Tech University (China)
Georgia Institute of Technology, Atlanta, GA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
National Yang Ming Chiao Tung University, Tainan (Taiwan)

The performance of reversible solid oxide electrochemical cells (R-SOECs) is largely hindered by the insufficient electroactivity and poor durability of the bifunctional air electrodes, where the oxygen reduction and evolution reactions (ORR and OER) occur. Here, we report our findings in boosting the electrochemical activity and durability of an air electrode with Pr_0.2Ba_0.2Sr_0.2La_0.2Ca_0.2CoO_3-δ (PBSLCC) via an A-site entropy engineering. The PBSLCC electrode shows enhanced oxygen reaction activity and excellent durability compared to binary and ternary double perovskites (PrBaCo₂O_5+δ and Pr_0.8Ba_0.8Ca_0.4Co₂O_5+δ, respectively). A low and nearly unchanged area-specific resistance of 0.042Ωcm² is achieved at 750 °C during the 225-h stability test. La_0.9Sr_0.1Ga_0.8Mg_0.2O_3-δ electrolyte-supported cells with the PBSLCC air electrode show remarkable performance at 800 °C, demonstrating a peak power density of 1.2Wcm^-2 in the fuel cell mode, and a current density of -1.1 Acm^-2 at 1.3 V in the electrolysis mode while maintaining the excellent cycling durability of 228 h at ±0.5 Acm^-2 under humidified H₂ (10% H₂O). A bulk oxygen p-band center model is applied to verify that tailoring of the A-site entropy strongly influences the surface exchange coefficients (k*_chem), leading to higher oxygen reaction activity of PBSLCC than the binary and ternary perovskites. Finally, this study opens a new class of high-entropy perovskites for the rational design of air electrodes for R-SOECs with high activity and durability.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Sponsoring Organization:: Fundamental Research Funds for the Central Universities; Introduced Innovative Research and Development Team of Guangdong; National Natural Science Foundation of China (NSFC); National Science and Technology Council (NSTC); Natural Science Foundation of Guangdong Province; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: SC0012704

OSTI ID:: 1995479

Report Number(s):: BNL-224662-2023-JAAM

Journal Information:: Materials Today, Journal Name: Materials Today Vol. 63; ISSN 1369-7021

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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