中温固体氧化物燃料电池的高熵双钙钛矿阴极材料: 兼容性与活性研究

doi:10.15541/jim20220551

无机材料学报 ›› 2023, Vol. 38 ›› Issue (6): 693-700.DOI: 10.15541/jim20220551

中温固体氧化物燃料电池的高熵双钙钛矿阴极材料: 兼容性与活性研究

郭天民¹(), 董江波², 陈正鹏², 饶睦敏², 李明飞², 李田¹, 凌意瀚¹()

1.中国矿业大学材料科学与物理学院, 徐州 221116
2.广东能源集团科技研究院有限公司, 广州 510000

收稿日期:2022-09-21 修回日期:2022-11-13 出版日期:2022-12-09 网络出版日期:2022-12-09
通讯作者: 凌意瀚, 研究员. E-mail: lyhyy@cumt.edu.cn
作者简介:郭天民(1991-), 男, 硕士. E-mail: 277263262@qq.com

Enhanced Compatibility and Activity of High-entropy Double Perovskite Cathode Material for IT-SOFC

GUO Tianmin¹(), DONG Jiangbo², CHEN Zhengpeng², RAO Mumin², LI Mingfei², LI Tian¹, LING Yihan¹()

1. School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221116, China
2. Guangdong Energy Group Science and Technology Research Institute Co., Ltd., Guangzhou 510000, China

Received:2022-09-21 Revised:2022-11-13 Published:2022-12-09 Online:2022-12-09
Contact: LING Yihan, professor. E-mail: lyhyy@cumt.edu.cn
About author:GUO Tianmin (1991-), male, Master. E-mail: 277263262@qq.com
Supported by:
National Key R&D Program of China(2021YFB4001502);National Natural Science Foundation of China(52272257);National Natural Science Foundation of China(52104229)

摘要/Abstract

摘要：

中温固体氧化物燃料电池(IT-SOFC)有助于国家的碳中和战略, 但其阴极材料难以兼顾热兼容性和催化活性。为此, 基于多元素耦合的高熵策略, 本研究合成了高熵阴极材料GdBa(Fe_0.2Mn_0.2Co_0.2Ni_0.2Cu_0.2)₂O₅₊_δ(HE-GBO), 具有双过氧化物结构, 与Gd_0.1Ce_0.9O_2-_δ(GDC)有良好的化学兼容性, 协调了与催化活性之间的平衡性。采用HE-GBO阴极的对称电池在800 ℃下的极化电阻(R_p)为1.68 Ω·cm², 而HE-GBO-GDC(质量比7 : 3)复合阴极的R_p因引入GDC而显著降低(800 ℃下R_p为0.23 Ω·cm²)。采用HE-GBO和HE-GBO-GDC阴极组装树枝状微通道阳极支撑单电池,在800 ℃的最大功率密度分别达到972.12和1057.06 mW/cm², 使用高熵阴极可以进一步提高电池性能。这些结果表明多尺度优化有助于开发高性能的IT-SOFC阴极材料。

关键词: 高熵阴极, 固体氧化物燃料电池, 热相容性, 树枝状微通道

Abstract:

Intermediate-temperature solid oxide fuel cell (IT-SOFC) is promising for carbon neutrality, but its cathode is limited by the contradiction between thermal compatibility and catalytic activity. Herein, we propose a high-entropy double perovskite cathode material, GdBa(Fe_0.2Mn_0.2Co_0.2Ni_0.2Cu_0.2)₂O₅₊_δ (HE-GBO) with improved compatibility and activity, in view of the high-entropy strategy by multi-elemental coupling, which possesses double perovskite structure and excellent chemical compatibility with state-of-the-art Gd_0.1Ce_0.9O_2-_δ(GDC). The polarization resistance (R_p) of the symmetrical cells with HE-GBO cathode is 1.68 Ω·cm² at 800 ℃, and the corresponding R_p of HE-GBO-GDC (mass ratio 7:3) composite cathode can be greatly reduced (0.23 Ω·cm² at 800 ℃) by introducing GDC. Dendritic microchannels anode-supported single cells with HE-GBO and HE-GBO-GDC cathodes realize maximum power densities of 972.12 and 1057.06 mW/cm² at 800 ℃, respectively, indicating that cell performance can be enhanced by high-entropy cathodes. The results demonstrate that high-entropy double perovskite cathode material HE-GBO has a high potantial to solve the conflict problem of thermal compatibility and catalytic activity in IT-SOFCs.

Key words: high-entropy cathode, solid oxide fuel cells, thermal compatibility, dendritic microchannels

中图分类号:

郭天民, 董江波, 陈正鹏, 饶睦敏, 李明飞, 李田, 凌意瀚. 中温固体氧化物燃料电池的高熵双钙钛矿阴极材料: 兼容性与活性研究[J]. 无机材料学报, 2023, 38(6): 693-700.

GUO Tianmin, DONG Jiangbo, CHEN Zhengpeng, RAO Mumin, LI Mingfei, LI Tian, LING Yihan. Enhanced Compatibility and Activity of High-entropy Double Perovskite Cathode Material for IT-SOFC[J]. Journal of Inorganic Materials, 2023, 38(6): 693-700.

图/表 10

Fig. 1 (a) XRD patterns and (b) corresponding magnified area of 2θ=45°-50° of GBCO and HE-GBO powders calcined at 1150 ℃ for 3 h, and (c) schematic diagram of the HE-GBO double perovskite structure

Fig. 2 XRD patterns of chemical compatibility between cathode (HE-GBO) and electrolytes materials (YSZ and GDC) calcined at 950 ℃ in air

Fig. 3 Temperature dependence of average CTE of GBCO and HE-GBO in air from 25 to 800 ℃ Colorful figure is available on website

Fig. 4 EIS plots of symmetrical single cells with (a) HE-GBO and (b) HE-GBO-GDC cathodes measured from 800 to 600 ℃ in air Colorful figures are available on website

Fig. 5 Cross-section morphologies of single cell with (a) HE-GBO and (b) HE-GBO-GDC after 100 h long-term test, and (c, d) their magnified morphologies, respectively

Fig. 6 EDS surface sweep results for high-entropy cathode material (HE-GBO, in Fig. 5(c)) after 100 h long-term test

Fig. 7 I-V and I-P curves of single cells with (a) HE-GBO and (b) HE-GBO-GDC cathodes measured from 800 ℃ to 600 ℃ in wet H2 (~3% H2O)

Fig. 8 EIS plots of single cells with (a) HE-GBO and (b) HE-GBO-GDC cathodes measured from 800 ℃ to 600 ℃ in wet H2 (~3% H2O), (c) simulated polarization resistance, and (d) Arrhenius plots of single cells with HE-GBO and HE-GBO-GDC cathodes Colorful figures are available on website

Fig. 9 DRT analysis of EIS data for the single cells with (a) HE-GBO and (b) HE-GBO-GDC cathodes from 800-600 ℃

Fig. 10 Long-term stability performance of single cell with HE-GBO cathode in H2 (~3% H2O) atmosphere

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中温固体氧化物燃料电池的高熵双钙钛矿阴极材料: 兼容性与活性研究

Enhanced Compatibility and Activity of High-entropy Double Perovskite Cathode Material for IT-SOFC

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