Rb掺杂的可逆质子陶瓷电化学电池双钙钛矿空气电极的氧还原和制氢电催化性能提升研究

doi:10.1016/S1872-2067(25)64786-3

催化学报 ›› 2025, Vol. 78: 313-323.DOI: 10.1016/S1872-2067(25)64786-3

Rb掺杂的可逆质子陶瓷电化学电池双钙钛矿空气电极的氧还原和制氢电催化性能提升研究

简楚倩^a, 黄逸轩^a, 高辉^a, 夏娇娇^a, 龚文杰^a, 张茜瑞^a, 陈晓锋^a, 刘江^a, 刘瑛^b^,^*(), 陈宇^a^,^*()

^a华南理工大学环境与能源学院, 广东广州 510006
^b紫金矿业集团股份有限公司可再生能源与先进材料研究院, 福建厦门 361101

收稿日期:2025-05-15 接受日期:2025-06-19 出版日期:2025-11-18 发布日期:2025-10-14
通讯作者: *电子信箱: liu_ying@zijinmining.com (刘瑛), 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);广东省引进创新创业团队项目(2021ZT09L392);国家自然科学基金(22179039);广州市科技计划(2024A04J3079);珠江人才计划(2019QN01C693);紫金矿业集团股份有限公司科研项目(5405-ZC-2023-00008)

Boosting the electrocatalytic performance of double perovskite air electrodes via Rb-doping for oxygen reduction and hydrogen production in reversible protonic ceramic electrochemical cells

Chuqian Jian^a, Yixuan Huang^a, Hui Gao^a, Jiaojiao Xia^a, Wenjie Gong^a, Xirui Zhang^a, Xiaofeng Chen^a, Jiang Liu^a, Ying Liu^b^,^*(), Yu Chen^a^,^*()

^aSchool of Environment and Energy, South China University of Technology, Guangzhou 510006, Guangdong, China
^bResearch Institute of Renewable Energy and Advanced Materials, Zijin Mining Group Co., Ltd., Xiamen 361101, Fujian, China

Received:2025-05-15 Accepted:2025-06-19 Online:2025-11-18 Published:2025-10-14
Contact: *E-mail: liu_ying@zijinmining.com (Y. Liu), 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);Guangzhou Science and Technology Project(2024A04J3079);Pearl River Talent Recruitment Program(2019QN01C693);Zijin Mining Group Co., Ltd(5405-ZC-2023-00008)

摘要/Abstract

摘要：

在全球能源需求持续增长与生产规模快速扩张的背景下, 发展低碳、高效、可持续的能源转换与存储技术已成为解决能源与环境问题的关键. 其中, 可逆质子陶瓷电化学电池(R-PCECs)因其兼具燃料电池(FC)模式下的高效化学能-电能转换能力与电解电池(EL)模式下的清洁能源存储特性, 近年来受到学术界与工业界的广泛关注. 该技术通过质子传导机制实现零碳排放的能量转换, 展现出显著的环保优势与技术潜力. 然而, R-PCECs的实际性能仍受限于空气电极缓慢的氧还原反应(ORR)与析氧反应(OER)动力学. 因此, 开发兼具高催化活性与长期稳定性的新型空气电极材料已成为该领域亟待解决的关键挑战.

本文成功开发了一种新型铷掺杂双钙钛矿材料PrBa_0.8Ca_0.1Rb_0.1Co₂O₅₊_δ (PBCR_0.1C), 并将其作为空气电极应用于R-PCECs中. 采用PBCR_0.1C电极的对称电池在700 ^oC下表现出0.044 Ω cm²的极化电阻, 低于目前已报道的大多数同类电极材料. 值得注意的是, 即使在含有3 vol%水蒸气的潮湿空气环境中, 该电极仍能保持优异的稳定性. 通过X射线光电子能谱、热重分析和电导率测试等表征手段证实, 该电极的优异性能源于其高电导率、高氧空位浓度和快速表面氧交换的特性. 该材料在FC和EL两种工作模式下均展现出卓越的电化学性能: FC模式峰值功率密度达2.32 W cm^-2; EL模式在1.3 V电压下电解电流密度达-3.55 A cm^-2. 在650 ^oC, 当蒸汽浓度为30 vol%、电流密度为-0.5 A cm^-2时, 电池的法拉第效率达到87.80%, 相应的产氢速率为3.05 mL min^-1 cm^-2. 此外, 对采用PBCR_0.1C空气电极的R-PCECs, 在650 ^oC下进行了短期耐久性测试. 在FC模式下, 基于PBCR_0.1C空气电极的R-PCECs在+0.5 A cm^-2的恒电流条件下展现出优异的稳定性, 可连续运行120 h以上. 在EL模式下, 单电池同样表现出优异的耐久性. 长期稳定性测试后的截面电镜照片显示, 电池结构和微观形貌均保持良好. 通过在650 ^oC下进行动态循环切换测试发现, 采用PBCR_0.1C空气电极的电池在±0.5 A cm^-2电流密度下连续运行100 h后, 电压未出现明显衰减, 充分证明了该电极材料在R-PCECs中的优异可逆操作稳定性. 这些实验结果不仅证实了PBCR_0.1C作为高性能空气电极的巨大潜力, 也为开发下一代高效且稳定的R-PCECs提供了重要的设计思路.

综上所述, A位Rb掺杂策略有效提升了氧空位浓度和电导率, 显著增强了ORR/OER催化活性和耐久性. 该工作为开发高性能R-PCECs电极材料提供了新思路. 未来研究可进一步优化材料的掺杂策略, 以提升电极在中低温工作条件下的电化学性能, 这为R-PCECs技术的性能提升提供了新的研究方向.

关键词: 空气电极, 稳定性, 铷掺杂, 可逆质子陶瓷电化学电池, 氧还原/析出反应

Abstract:

The slow oxygen reaction kinetics of air electrodes impair the performance of reversible protonic ceramic electrochemical cells (R-PCECs); hence, it is imperative to design novel air electrodes featuring excellent catalytic activity and endurance. Here, we report an Rb-doped double perovskite PrBa_0.8Ca_0.1Rb_0.1Co₂O₅₊_δ (denoted as PBCR_0.1C) as an air electrode for R-PCECs, displaying a low polarization resistance of 0.044 Ω cm² at 700 °C and excellent stability during exposure to humid air (3 vol% H₂O). The high performance is attributed to the high electrical conductivity, high concentration of oxygen vacancies, and fast surface exchange, as verified by the analyses of X-ray photoelectron spectroscopy, thermogravimetric testing, and conductivity tests. The R-PCECs with the PBCR_0.1C air electrode demonstrate an encouraging performance at 700 °C: a peak power density of 2.32 W cm^-2 in a fuel cell (FC) mode and an electrolysis current density of -3.55 A cm^-2 at 1.3 V in an electrolysis (EL) mode. At 30 vol% steam concentration, a Faraday efficiency of 87.80% and a corresponding H₂ production rate of 3.05 mL min^-1 cm^-2 at a current density of -0.5 A cm^-2 at 650 °C. Additionally, the durability of the cell in the FC mode (120 h), EL mode (120 h), and cycling FC/EL mode (100 h) at 650 °C suggests the great potential of PBCR_0.1C as the highly reactive and robust air electrodes of R-PCECs.

Key words: Air electrode, Stability, Rubidium-doping, Reversible protonic ceramic, electrochemical cells, Oxygen reduction/evolution reaction

简楚倩, 黄逸轩, 高辉, 夏娇娇, 龚文杰, 张茜瑞, 陈晓锋, 刘江, 刘瑛, 陈宇. Rb掺杂的可逆质子陶瓷电化学电池双钙钛矿空气电极的氧还原和制氢电催化性能提升研究[J]. 催化学报, 2025, 78: 313-323.

Chuqian Jian, Yixuan Huang, Hui Gao, Jiaojiao Xia, Wenjie Gong, Xirui Zhang, Xiaofeng Chen, Jiang Liu, Ying Liu, Yu Chen. Boosting the electrocatalytic performance of double perovskite air electrodes via Rb-doping for oxygen reduction and hydrogen production in reversible protonic ceramic electrochemical cells[J]. Chinese Journal of Catalysis, 2025, 78: 313-323.

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图/表 5

Fig. 1. Phase structure of PBCR0.1C powder. (a) Refined XRD profiles of PBCR0.1C sample after being fired in air at 950 °C for 2 h. (b) XRD profiles of PBCC and PBCR0.1C powders. (c) Detailed XRD patterns of PBCR0.1C and PBCC in 2θ of 32°-34°, corresponding to the dashed box in (b). TEM (d) and HR-TEM (e) images of the PBCR0.1C sample and corresponding FFT pattern. (f) A linear scanning pattern within the red frame in (e). (g) STEM image and corresponding EDS mapping results of Pr, Ba, Ca, Rb, Co, and O on PBCR0.1C.

Fig. 2. Symmetrical cell performance of the PBCR0.1C air electrode. (a) The EIS curves PBCR0.1C symmetrical cells from 500 to 700 °C. (b) Polarization resistance of PBCR0.1C and PBCC air electrodes compared with other high-performance electrodes at different temperatures. (c) DRT analyses for symmetrical cells featuring PBCR0.1C air electrodes at 650 °C under various partial pressures of oxygen (pO2). (d) pO2 dependence of Rp of the PBCR0.1C air electrode at LF, IF, and HF regions. (e) DRT profiles for symmetrical cells featuring PBCR0.1C air electrodes tested at 650 °C for EIS at different pH2O. (f) pH2O dependence of Rp of the PBCR0.1C air electrode at different frequency ranges. (g) Rp stability of PBCR0.1C and PBCC air electrode in humid air (3 vol% H2O) at 650 °C under OCV conditions; insets correspond to EIS of PBCR0.1C and PBCC. (h) DRT of the EIS of PBCR0.1C air electrode at different testing times during stability test.

Fig. 3. Electrical conductivity and surface properties of the PBCR0.1C. (a) The electrical conductivity of dense PBCR0.1C and PBCC bars in dry air. (b) The XPS profiles of Co 2p3/2 and Ba 3d5/2 for PBCR0.1C. (c) The XPS profile of O 1s for the PBCR0.1C sample. (d) FTIR spectra of PBCR0.1C powders that have been steam-treated.

Fig. 4. Electrochemical performance and Microstructure evaluation of single cells. (a) I-V-P curves of PBCR0.1C single cell (FC mode). (b) The EIS curves of the PBCR0.1C single cell under OCV conditions. (c) I-V curves of PBCR0.1C single cell (EL mode). (d) Comparison of PPD with other high-performance electrodes. (e) Comparison of the current density with various electrode materials in EL mode (1.3 V). (f) A cross-sectional scanning electron micrograph of a PBCR0.1C single cell.

Fig. 5. Durability test and Faradaic efficiency of single cells. (a) Durability test of the PBCR0.1C single cells in FC/EL mode at 650 °C. (b) Cycling durability test of R-PCEC equipped PBCR0.1C air electrode at 650 °C. FE (c) and corresponding H2 generation rates (d) at different steam concentrations (10 and 30 vol% H2O) and 600 °C with various current densities (-0.5, -0.75, and -1 A cm?2). FE (e) and corresponding H2 generation rates (f) at different steam concentrations (10 and 30 vol% H2O) at 650 °C with various current densities (-0.5, -0.75, and -1 A cm?2).

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Rb掺杂的可逆质子陶瓷电化学电池双钙钛矿空气电极的氧还原和制氢电催化性能提升研究

Boosting the electrocatalytic performance of double perovskite air electrodes via Rb-doping for oxygen reduction and hydrogen production in reversible protonic ceramic electrochemical cells

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