锰掺杂诱导空气电极相分离实现高性能且耐久的可逆质子陶瓷电池

doi:10.1016/S1872-2067(25)64907-2

催化学报 ›› 2026, Vol. 81: 333-343.DOI: 10.1016/S1872-2067(25)64907-2

锰掺杂诱导空气电极相分离实现高性能且耐久的可逆质子陶瓷电池

陈晓锋, 黄逸轩, 林万斌, 夏娇娇, 张茜瑞, 龚文杰, 简楚倩, 刘豪, 曾嘉成, 刘江, 陈宇^*()

华南理工大学环境与能源学院, 广东广州 510006

收稿日期:2025-07-10 接受日期:2025-09-22 出版日期:2026-02-18 发布日期:2025-12-26
通讯作者: *电子信箱: eschenyu@scut.edu.cn (陈宇).
基金资助:
广东省基础与应用基础研究基金(2024A1515010448);广东省引进创新研发团队(2021ZT09L392);国家自然科学基金(22179039);珠江人才引进计划(2019QN01C693)

Mn-doping induced phase segregation of air electrodes enables high-performance and durable reversible protonic ceramic cells

Xiaofeng Chen, Yixuan Huang, Wanbin Lin, Jiaojiao Xia, Xirui Zhang, Wenjie Gong, Chuqian Jian, Hao Liu, Jiacheng Zeng, Jiang Liu, Yu Chen^*()

School of Environment and Energy, South China University of Technology, Guangzhou 510006, Guangdong, China

Received:2025-07-10 Accepted:2025-09-22 Online:2026-02-18 Published:2025-12-26
Contact: *E-mail: eschenyu@scut.edu.cn (Y. Chen).
Supported by:
Guangdong Basic and Applied Basic Research Foundation(2024A1515010448);Introduced Innovative R&D Team of Guangdong(2021ZT09L392);National Natural Science Foundation of China(22179039);Pearl River Talent Recruitment Program(2019QN01C693)

摘要/Abstract

摘要：

随着能源结构转型加速与不可再生资源日益枯竭, 发展清洁可持续的能源已成为全球性迫切需求. 在此背景下,可逆质子陶瓷电池(R-PCCs)凭借其燃料灵活、效率高及污染少等优势, 展现出广阔的应用前景. 该电池兼具燃料电池(FC)模式下的高效发电与电解(EL)模式下清洁制氢的双重功能. 该技术基于质子传导机制, 具有迁移能垒低、传导速率快等优势, 使得R-PCCs能够在400 - 700 ºC的中低温区间稳定工作, 从而有效缓解材料兼容性与热应力问题. 然而, R-PCCs在中低温下仍面临空气电极氧反应动力学缓慢和耐久性不足的挑战, 这制约了其整体性能与商业化进程. 因此, 开发高活性与高稳定性的空气电极材料, 对推进R-PCCs技术发展具有重要意义.

本文成功开发了一种以低成本的锰元素掺杂的双钙钛矿材料PrBa_0.8Ca_0.2Co_1.5Mn_0.5O₅₊_δ (PBCCM_0.5), 并将其作为空气电极应用于R-PCCs中. 该电极材料由主相Pr_1.25Ba_0.5Ca_0.25Co_1.58Mn_0.42O₅₊_δ (D-PBCCMn, 其化学式按每个单位公式含有2个B位阳离子进行归一化)和六方钙钛矿次相BaCo_0.6Mn_0.4O_3-_δ (BCMO)自组装而成. 实验结果表明, 适量BCMO相的生成有利于提升空气电极的性能及长期运行稳定性. 因此, 采用PBCCM_0.5电极的对称电池在700 ºC表现出0.053 Ω cm²的极化电阻, 低于目前已报道的大部分同类空气电极. 同时, PBCCM_0.5电极在含有3 vol%水蒸气的潮湿环境下仍能保持良好的运行稳定性, 性能衰减率仅为0.0004239 Ω cm² h^-1. 同时, X射线光电子能谱和电导弛豫法等结果证明, 锰掺杂诱导形成的纳米复合结构能有效促进氧空位的形成, 并改善空气电极的氧表面交换和体相扩散能力. 该空气电极材料应用于燃料电极支撑的单电池时, 在FC和EL双模式下表现出令人满意的电化学性能: 在700 ºC, FC模式下运行的峰值功率密度为2.05 W cm^-2, EL模式下运行在1.3 V电压下的电解电流密度为-3.78 A cm^-2. 在600 ºC, 电流密度为-0.5 A cm^-2, 蒸汽浓度为50 vol%条件下, 采用PBCCM_0.5作为空气电极的电池的法拉第效率为97.54 %, 产氢速率为3.40 mL min^-1 cm^-2. 同时, 通过FC模式和EL模式的短期耐久性测试进一步评估PBCCM_0.5空气电极用于R-PCCs的运行稳定性. 在FC模式下, 基于PBCCM_0.5空气电极的R-PCCs在+0.5 A cm^-2恒电流条件下表现出100 h良好的运行稳定性, 在EL模式下同样表现出优异的耐久性. 长期稳定性测试后的电池横截面扫描电镜结果表明, 空气电极与电解质之间没有分层现象, 同时空气电极依旧保持丰富的孔隙率, 没有出现团聚现象, 进一步验证了电极的良好运行稳定性. 由600 ºC下动态双模式循环测试的结果可得, 在电流密度为±0.5 A cm^-2条件下采用PBCCM_0.5作为空气电极的电池能稳定运行120 h (约30个循环), 证明了该空气电极材料在R-PCCs具有出色的可逆操作稳定性.

综上, 通过锰元素掺杂诱导相分离能够有效提升空气电极材料的氧空位浓度、氧表面交换系数和体扩散系数, 该工作为解决锰替代钴导致的性能衰减问题提供了潜在策略, 并为设计高性能的空气电极材料提供了一种新的思路. 未来的研究可集中于稳定制备特定比例的自组装两相空气电极材料, 同时优化锰元素的掺杂浓度, 为提升R-PCCs性能进一步提供了新的研究方向.

关键词: 可逆质子陶瓷电池, 空气电极, 锰掺杂, 氧还原反应, 析氧反应

Abstract:

Reversible protonic ceramic cells (R-PCCs) represent a highly promising energy conversion and storage technology, offering high efficiency at intermediate temperatures (400-700 °C). However, their commercialization is significantly impeded by the sluggish oxygen reaction kinetics on air electrodes. This work reports a Mn-doped PrBa_0.8Ca_0.2Co₂O₅₊_δ air electrode with a nominal composition of PrBa_0.8Ca_0.2Co_1.5Mn_0.5O₅₊_δ, which primarily segregates into a deficient double perovskite Pr_1.25Ba_0.5Ca_0.25Co_1.58Mn_0.42O₅₊_δ phase and a minor BaCo_0.6Mn_0.4O₃_-δ hexagonal perovskite phase, as suggested by the X-ray diffraction refinement. The formation of Mn-doped nanocomposites substantially enhances the activities of oxygen reduction/evolution reactions, attributed to elevated oxygen vacancy concentrations and improved oxygen surface exchange and bulk diffusion capabilities, relative to the undoped PrBa_0.8Ca_0.2Co₂O₅₊_δ. The synergistic effect between the two phases may enhance electrochemical performance. Single cells incorporating these nanocomposite air electrodes achieve exceptional electrochemical performance at 700 °C: peak power density of 2.05 W cm^-2 in fuel cell (FC) mode and current density of -3.78 A cm^-2 at 1.3 V in electrolysis (EL) mode. Furthermore, promising durability is demonstrated during a FC test (100 h), an EL test (100 h), and a FC-EL cycling test (120 h) at 600 °C. This Mn-doping approach establishes an effective strategy for developing advanced air electrode materials.

Key words: Reversible protonic ceramic cells, Air electrodes, Mn-doping, Oxygen reduction reactions, Oxygen evolution reaction

陈晓锋, 黄逸轩, 林万斌, 夏娇娇, 张茜瑞, 龚文杰, 简楚倩, 刘豪, 曾嘉成, 刘江, 陈宇. 锰掺杂诱导空气电极相分离实现高性能且耐久的可逆质子陶瓷电池[J]. 催化学报, 2026, 81: 333-343.

Xiaofeng Chen, Yixuan Huang, Wanbin Lin, Jiaojiao Xia, Xirui Zhang, Wenjie Gong, Chuqian Jian, Hao Liu, Jiacheng Zeng, Jiang Liu, Yu Chen. Mn-doping induced phase segregation of air electrodes enables high-performance and durable reversible protonic ceramic cells[J]. Chinese Journal of Catalysis, 2026, 81: 333-343.

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图/表 4

Fig. 1. Phase and microstructure analyses of the PBCCMx powder. (a) XRD patterns of PBCC and PBCCMx (x = 0.1, 0.3, 0.4, 0.5, 0.6, 1.0, 1.5) powders. (b) Rietveld refinement profile of the PBCCM0.5 sample. (c) High-resolution TEM images showing a D-PBCCMn grain and a BaCo0.6Mn0.4O3-δ grain. (d) STEM-EDS elemental mapping images of PBCCM0.5 powder.

Fig. 2. Electrochemical performance of electrodes. (a) EIS curves of PBCCM0.5 air electrodes measured in wet air (3% H2O) from 500 to 700 °C. (b) ASR comparison of air electrodes with distinct Mn doping levels (0, 0.1, 0.3, 0.4, 0.5, 0.6, 1.0 and 1.5) at 550, 600, and 650 °C in humidified air (3% H2O). (c) ASR comparison between PBCCM0.5 and reference air electrodes in BZCYYb-based symmetrical cells from 500 to 700 °C. (d) EIS data of PBCCM0.5 electrodes at 600 °C under varying pO2 conditions. (e) Corresponding DRT plots for PBCCM0.5 electrodes under different pO2 at 600 °C. (f) Rp dependence of PBCCM0.5 electrodes on pO2 at 600 °C. (g) EIS data of PBCCM0.5 electrodes at 600 °C under varying pH2O conditions. (h) Corresponding DRT plots for PBCCM0.5 electrodes under different pH2O at 600 °C; (i) Rp dependence of PBCCM0.5 electrodes on pH2O at 600 °C.

Fig. 3. Origin of the performance enhancement. (a) Temperature-dependent ASRs for symmetrical cells employing PBCCM0.5 electrodes and physically mixed electrodes (D-PBCCMn and BCMO). (b) Comparative ASR stability of PBCCM0.5, PBCC, BCMO electrodes and physically mixed electrodes (D-PBCCMn and BCMO) in symmetrical cells. (c) DRT analysis of PBCCM0.5, PBCC, BCMO electrodes, and physically mixed electrodes (D-PBCCMn and BCMO) recorded at different measurement times. (d) Derived k*chem and D*chem values for PBCCM0.5 and PBCC materials between 550 and 700 °C. (e) O 1s XPS spectra of PBCCM0.5 and PBCC powder samples. (f) Distribution of oxygen species in PBCCM0.5 and PBCC powders (histogram representation).

Fig. 4. Single cell performance. (a) I-V-P curves of R-PCCs equipped with PBCCM0.5 air electrodes operating in FC mode across 500-700 °C. (b) Performance comparison of PPDs among other electrode materials reported recently (Table S5). (c) Cross-sectional SEM image depicting the PBCCM0.5 air electrode interface within a single-cell assembly. (d) I-V curves of R-PCCs featuring PBCCM0.5 air electrodes in EL mode across 500-700 °C. (e) Evaluation of electrolysis current densities at 1.3 V for various electrode materials (Table S6). (f) Faradaic efficiency measurements under varying current densities and water vapor concentrations. (g) Short-term stability assessment of R-PCCs with PBCCM0.5 in FC mode at 600 °C. (h) EL mode stability analysis of R-PCCs with PBCCM0.5 at 600 °C. (i) Stability evaluation of R-PCCs with PBCCM0.5 during cyclic reversible mode.

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锰掺杂诱导空气电极相分离实现高性能且耐久的可逆质子陶瓷电池

Mn-doping induced phase segregation of air electrodes enables high-performance and durable reversible protonic ceramic cells

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