固体氧化物电池直孔电极结构的制备技术与性能研究进展

doi:10.15541/jim20250123

无机材料学报 ›› 2025, Vol. 40 ›› Issue (12): 1311-1323.DOI: 10.15541/jim20250123

• 专栏：高温燃料电池关键材料(客座编辑：凌意瀚) • 上一篇下一篇

固体氧化物电池直孔电极结构的制备技术与性能研究进展

凌意瀚(), 郭胜, 曹志强, 田云峰(), 刘方升, 金芳军, 高源

中国矿业大学材料与物理学院, 徐州 221000

收稿日期:2025-03-24 修回日期:2025-07-07 出版日期:2025-12-20 网络出版日期:2025-07-16
通讯作者: 田云峰, 副教授. E-mail: yunfengup@cumt.edu.cn;
凌意瀚, 教授. E-mail: lyhyy@cumt.edu.cn
作者简介:凌意瀚(1986-), 男, 教授. E-mail: lyhyy@cumt.edu.cn
基金资助:
国家自然科学基金(52272257);江苏省杰出青年基金(BK20240109)

Research Progress on Preparation Technologies and Performance of Straight-pore Electrode Structures for Solid Oxide Cells

LING Yihan(), GUO Sheng, CAO Zhiqiang, TIAN Yunfeng(), LIU Fangsheng, JIN Fangjun, GAO Yuan

School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221000, China

Received:2025-03-24 Revised:2025-07-07 Published:2025-12-20 Online:2025-07-16
Contact: TIAN Yunfeng, associate professor. E-mail: yunfengup@cumt.edu.cn;
LING Yihan, professor. E-mail: lyhyy@cumt.edu.cn
About author:LING Yihan (1986-), male, professor. E-mail: lyhyy@cumt.edu.cn
Supported by:
National Natural Science Foundation of China(52272257);Natural Science Foundation of Jiangsu Province(BK20240109)

摘要/Abstract

摘要：

固体氧化物电池(Solid Oxide Cell, SOC)因其燃料电池(SOFC)模式下的高效清洁发电能力和电解池(SOEC)模式下的优异制氢及储能潜力, 近年来受到广泛关注。传统SOC通常采用石墨、碳粉等造孔剂制备多孔电极支撑体, 存在孔隙无序分布、孔结构复杂的问题, 从而产生较高的曲折因子, 尤其在稀薄燃料或高电流密度条件下, 容易引发浓差极化, 这限制了电池性能的进一步提升。为解决这一问题, 近年来直孔结构的应用得到了广泛关注。该结构通过有序的孔道设计, 有效促进了气体扩散与传输, 减轻了浓差极化现象, 并提高了电极材料的浸渍效率及活性位点的利用率, 从而显著提升了SOC的电化学性能。本文系统综述了直孔结构SOC的最新制备技术研究进展, 详细阐述了相转化法、冷冻干燥法及海藻酸盐离子凝胶法等关键技术的成孔机理、工艺特点及其在平板式和管式SOC中的应用; 深入分析了直孔结构在SOFC和SOEC两种模式下对氢气、碳氢燃料适应性和电解性能(包括传统水/CO₂电解及燃料辅助电解)的提升作用与机制。尽管直孔结构在SOC应用中展现出巨大的潜力, 但目前关于这一制备技术的系统性综述仍较为缺乏。本文旨在总结直孔结构SOC的最新制备技术进展, 分析其技术优势与存在的问题, 并提出未来的发展方向, 以期为相关研究提供参考。

关键词: 固体氧化物电池, 直孔结构, 制备技术, 电化学性能, 综述

Abstract:

Solid oxide cell (SOC) has attracted extensive attention in recent years due to its high-efficiency clean power generation capability in fuel cell (SOFC) mode and excellent hydrogen production and energy storage potential in electrolysis cell (SOEC) mode. Conventional SOC typically employs pore-forming agents such as graphite or carbon powder to fabricate porous electrode supports. This approach results in disordered pore distribution and complex pore structure, leading to high tortuosity factor. Particularly under conditions of dilute fuel or high current densities, these factors cause concentration polarization, limiting further performance improvements. To address these challenges, application of straight-pore structures has shown significant progress. The ordered pore channels in this structure enhance gas diffusion and transport, reduce concentration polarization, and improve the impregnation efficiency of electrode materials while increasing the utilization of active sites, thereby significantly boosting the electrochemical performance of SOC. This review systematically summarizes recent advancements in the preparation techniques for straight-pore structured SOC. It details the pore-forming mechanisms, process characteristics, and applications of key technologies (phase inversion, freeze-drying and alginate ion gelation) in both planar and tubular SOC configurations. Furthermore, it provides an in-depth analysis of how the straight-pore structure enhances performance in both SOFC mode (hydrogen and hydrocarbon fuel adaptability) and SOEC mode (conventional H₂O/CO₂ electrolysis and fuel-assisted electrolysis), elucidating the underlying mechanisms. Despite the great potential demonstrated by straight-pore structures in SOC, comprehensive reviews focusing on their fabrication techniques remain scarce. This paper aims to consolidate the latest progress in straight-pore SOC preparation technologies, analyze their technical advantages and existing challenges, and propose future research directions.

Key words: solid oxide cell, straight-pore structure, fabrication technology, electrochemical performance, review

中图分类号:

TQ174

凌意瀚, 郭胜, 曹志强, 田云峰, 刘方升, 金芳军, 高源. 固体氧化物电池直孔电极结构的制备技术与性能研究进展[J]. 无机材料学报, 2025, 40(12): 1311-1323.

LING Yihan, GUO Sheng, CAO Zhiqiang, TIAN Yunfeng, LIU Fangsheng, JIN Fangjun, GAO Yuan. Research Progress on Preparation Technologies and Performance of Straight-pore Electrode Structures for Solid Oxide Cells[J]. Journal of Inorganic Materials, 2025, 40(12): 1311-1323.

图/表 16

图1 (a) SOFC和(b) SOEC工作原理示意图

Fig. 1 Working principles of (a) SOFC and (b) SOEC

图2 不同孔结构的SEM照片[9-12]

Fig. 2 SEM images of different pore structures[9-12] (a) Microchannel pore structure[9]; (b) Dendritic pore structure[10]; (c) Gradient needle-like pore structure[11]; (d) Straight-through pore structure[12]

图3 平板式与管式电池结构[13]

Fig. 3 Structures of planar and tubular cells[13]

表1 各种制备技术的优缺点比较

Table 1 Comparison of advantages and disadvantages of various preparation techniques

Type	Fabrication technique	Technical advantages	Limitations
Planar	Stainless steel mesh-assisted phase inversion	Simple removal of skin/sponge layer	Difficult mass-production; Mechanical weakness
	Phase inversion tape casting method	High consistency; Suitable for mass production; Low cost; High porosity and permeability	Poor consistency; Sponge layer removal difficulty; Mechanical weakness
	Freeze-drying method	Membrane formed without post- processing; High porosity and permeability	High process complexity; High cost; Being only suitable for producing thick films (>3 mm); Mechanical weakness
	Alginate ion gelation method	Simple operation; Low cost	Difficult commercialization; Relatively large functional layer thickness
Tubular	Phase inversion combined with extrusion technology	Suitable for mass production; Simple operation	Small pore size; Difficult current collection
Tubular	Phase inversion combined with dip coating	Simple operation; Low cost	Difficult mass-production; High cost

图4 (a)不锈钢网辅助相转化法制备树枝状燃料电极支撑体的过程示意图以及(b)顶部基底、(c)底部基底和(d)基底表面的SEM照片[10]

Fig. 4 (a) Schematic diagram of stainless steel mesh-assisted phase inversion method for preparing dendritic fuel electrode supports, along with SEM images of (b) top substrate, (c) bottom substrate, and (d) substrate surface[10]

图5 (a)相转化流延法制备流程示意图[25]以及(b)电极横截面的SEM照片[26]

Fig. 5 (a) Schematic illustration of phase inversion tape casting fabrication process[25] and (b) cross-sectional SEM images of electrode[26]

图6 (a)冷冻干燥法制备支撑体的步骤示意图和(b)无规则多孔结构电极与梯度针状结构电极[37]

Fig. 6 (a) Schematic diagram of the steps for preparing support by freeze-drying and (b) random porous structure of electrode and gradient needle-like structure of freeze-dried electrode[37]

图7 冷冻干燥和燃烧法相结合制备的SOFC横截面SEM照片[46]

Fig. 7 Cross-sectional SEM image of SOFC prepared by combining freeze-drying and combustion[46]

图8 (a)直孔燃料电极支撑体的形成过程示意图; (b, c)未还原的直孔NiO-YSZ燃料电极支撑体的(b)横向截面和(c)纵向表面的SEM照片[53]

Fig. 8 (a) Schematic diagram illustrating the formation process of a straight-pore fuel electrode support; (b, c) SEM images of (b) transverse cross-section and (c) longitudinal surface of unreduced straight-pore NiO-YSZ fuel electrode support[53]

图9 相转化法结合挤出技术的(a)制作工艺、(b)实验装置示意图以及(c)管式电池的照片[58]

Fig. 9 Schematic diagrams of phase inversion method combined with extrusion technology for (a) fabrication process, (b) experimental device, and (c) photograph of tubular cells[58]

图10 (a)相转化结合挤出成型技术制备的单SOFC结构图和(b)电池横截面及(c)管壁多孔区域的SEM照片[59]

Fig. 10 (a) Schematic diagram of single SOFC prepared by phase transformation combined extrusion molding technology and SEM images of (b) cell cross-section and (c) porous region of tube wall[59]

图11 (a)通过相转化浸渍工艺制备的管式直孔SOFC的典型制造工艺[62]; (b)管式直孔SOC横截面的SEM照片[66]

Fig. 11 (a) Typical manufacturing process of tubular straight hole structure SOFC prepared by phase transformation impregnation process[62]; (b) SEM image of the cross-section of a tubular straight hole SOC[66]

图12 (a)在550~700 ℃下电流密度对SOFC电势差及功率密度的影响; (b) 550~700 ℃下的EIS谱图[59]

Fig. 12 (a) Effect of current density on cell potential difference and power densities of micro-monolithic SOFC at 550-700 ℃; (b) EIS spectra at 550-700 ℃[59]

图13 SFMNi@YSZ单电池的(a) I-V-P曲线和(b)在750 ℃、0.8 V下的耐久性测试[68]

Fig. 13 (a) I-V-P curves and (b) durability at 750 ℃ and 0.8 V of SFMNi@YSZ single cell[68]

图14 (a)在1.3 V、800 ℃条件下新型SOEC(MC-SOEC)与传统海绵状SOEC(SL-SOEC)的电流密度随时间的变化曲线; (b) MC-SOEC在1.3 V下的高电流密度与以前的工作对比[69]

Fig. 14 (a) Time dependence curves of current density for novel SOEC (MC-SOEC) and conventional sponge-like SOEC (SL-SOEC) under 1.3 V at 800 ℃; (b) High current density of MC-SOEC at 1.3 V compared with previous work[69]

图15 (a) SOEC在800 ℃、2 A·cm-2下CH4辅助CO2电解的长期稳定性[70]; (b) SOEC在800 ℃、3.0 A·cm-2下乙醇辅助电解水的长期稳定性[71]

Fig. 15 Long-term stability of (a) CH4-assisted CO2 electrolysis at 800 ℃ and 2 A·cm-2 for SOEC[70] and (b) ethanol-assisted water electrolysis at 800 ℃ and 3.0 A·cm-2 for SOEC[71]

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固体氧化物电池直孔电极结构的制备技术与性能研究进展

Research Progress on Preparation Technologies and Performance of Straight-pore Electrode Structures for Solid Oxide Cells

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