固体氧化物电池空气电极铬中毒机理及抗铬性能研究进展

doi:10.11949/0438-1157.20240130

摘要/Abstract

摘要：

固体氧化物电池（SOC）具有能源利用率高、污染排放量低、燃料灵活性高等优势，将在未来的能源供应和储存中发挥关键作用。当前，其长期稳定性尚不能满足大规模商业化的需求，电池堆中用于串联电池的金属连接体所导致的空气电极“铬中毒”是电堆性能衰减的重要因素之一。传统空气电极在发电模式（SOFC）下的铬中毒机理已较为明晰。然而，随着电解模式（SOEC）下应用的不断攀升，基于传统电极材料的毒化机理不适用于该运行模式下的电极体系。对典型空气电极材料在SOFC模式和SOEC模式下铬中毒机理进行对比分析，并且对提高SOC空气电极抗铬性能的研究进行总结和展望。

关键词: 燃料电池, 电化学, 电解, 催化剂, 固体氧化物电池, 空气电极, 铬中毒, 抗铬性能

Abstract:

Solid oxide cells (SOCs) have advantages of high energy utilization, low pollution emissions, and high fuel flexibility, and will play a key role in future energy supply and storage. At present, the main bottleneck restricting the large-scale commercial application of SOC is the long-term stability that needs to be improved. The chromium poisoning of SOC air electrode caused by the metallic interconnect used for serial connection of cells is one of the key issues. The chromium poisoning mechanism in traditional air electrodes operating in power generation mode (SOFC) is relatively well understood. However, with the increasing application demand of SOC in electrolytic mode (SOEC), the mechanism of chromium poisoning in SOEC mode needs to be explored urgently. In this paper, the mechanisms of chromium poisoning for typical SOC air electrodes in both SOFC and SOEC mode are reviewed. Additionally, it summarizes and prospects the research on improving the resistance of SOC air electrodes to chromium poisoning.

Key words: fuel cell, electrochemistry, electrolysis, catalyst, solid oxide cells, air electrode, chromium poisoning, chromium-resistivity

中图分类号:

TM 911.4

王天闻, 闫肃, 赵梦园, 杨天让, 刘建国. 固体氧化物电池空气电极铬中毒机理及抗铬性能研究进展[J]. 化工学报, 2024, 75(6): 2091-2108.

Tianwen WANG, Su YAN, Mengyuan ZHAO, Tianrang YANG, Jianguo LIU. Mechanisms of chromium poisoning in solid oxide cell air electrodes and research advances in enhancing chromium-resistivity[J]. CIESC Journal, 2024, 75(6): 2091-2108.

图/表 17

图1 SOC在发电和电解模式下的工作原理示意图[4]

Fig.1 SOC working principle schematics when working as fuel cell and electrolysis cell[4]

图2 阴极材料晶体结构

Fig.2 Crystal structure of cathode materials

图3 固体氧化物电池空气电极铬中毒过程

Fig.3 Chromium poisoning processes of SOFC air electrode

图4 不同铬物种的分压随温度的变化[17]

Fig.4 Temperature variation of partial pressure of different chromium species[17]

图5 Cr蒸气的传质速率与流速的关系[18]

Fig.5 Relationship between mass transfer rate and velocity of Cr steam[18]

表1 LSM阴极不同条件下加速铬中毒实验后的性能变化

Table 1 Performance changes of LSM cathode after accelerated chromium poisoning test under different conditions

T/℃	Cathode polarization current density/ (mA/cm²)	Experimental conditions for accelerated chromium poisoning	Change in R_Ω/Ω	Change in R_P/Ω	Change in η/mV	Change in E/mV	Ref.
750	400	SUS430，20 h	1.10	34.80	0.75	1.20	[33]
750	200	SUS430，20 h	1.12	32.25	0.22	0.30	[33]
750	800	SUS430，20 h	2.00	33.00	0.12	1.20	[33]
800	200	FCM，20 h	1.80	1.02	0.40	0.97	[34]
800	200	FCMM，20 h	-0.05	-1.57	-0.18	0.14	[34]
900	200	RA446，20 h	0.21	0.79	0.12	0.73	[35]

图6 LSM阴极铬物种沉积图

Fig.6 LSM cathode chromium species deposition map

图7 LSM与LSCF铬中毒前后扫描电镜图[36]

Fig.7 Scanning electron microscopy images of LSM and LSCF before and after chromium poisoning[36]

表2 LSCF阴极不同条件下加速铬中毒实验后的电阻变化

Table 2 Resistance changes of LSCF cathode after accelerated chromium poisoning test under different conditions

Temperature/℃	Whether polarization occurs	Materials	Experimental conditions for accelerated chromium poisoning	Change in R_Ω/Ω	Change in R_P/Ω	Ref.
700	OCV	LSCF	SUS430，40 h	—	0.36	[42]
700	OCV	LSCF-Ag	SUS430，40 h	—	0.02	[47]
700	OCV	LSCF	Crofer22H，200 h	0.60	0.48	[73]
700	OCV	LSCF-GDC0.24	Crofer22H，200 h	0.20	0.28	[47]
700	OCV	LSCF-GDC0.32	Crofer22H，200 h	0.08	0.12	[47]
700	100	LSCF	Crofer22H，200 h	0.76	0.77	[47]
700	100	LSCF-GDC0.24	Crofer22H，200 h	0.24	0.34	[47]
700	100	LSCF-GDC0.32	Crofer22H，200 h	0.11	0.20	[47]
800	OCV	LSCF	RA446，20 h	0.76	1.22	[39]
800	200	LSCF	RA446，20 h	0.74	1.49	[39]
900	OCV	LSCF	RA446，20 h	0.76	0.18	[39]
900	200	LSCF	RA446，20 h	0.69	0.18	[39]

图8 LSCF阴极OCV与恒定电流密度下铬中毒对比[38]

Fig.8 LSCF cathode OCV and constant current density chromium poisoning comparison[38]

图9 LSM空气电极阴极极化与阳极极化铬中毒机制

Fig.9 Cathode polarization and anode polarization of LSM air electrode mechanism of chromium poisoning

图10 LSM空气电极阳极极化下的铬中毒过程[51]

Fig.10 Chromium poisoning process under anode polarization of LSM air electrode[51]

图11 LSCF空气电极阴极极化与阳极极化铬中毒机理

Fig.11 Cathode polarization and anode polarization of LSCF air electrode mechanism of chromium poisoning

图12 Ni-Mo-Cr合金对LSM阴极铬中毒的抑制机理[53]

Fig.12 Inhibition mechanism of Ni-Mo-Cr alloy on chromium poisoning of LSM cathode[53]

图13 铬吸收剂作用机理[66]

Fig.13 Mechanism of chromium absorbent[66]

图14 SCT@LSCF-GDC空气电极合成及抑制Cr中毒机理图[79]

Fig.14 Electrode synthesis and Cr poisoning inhibition mechanism diagram of SCT@LSCF-GDC[79]

图15 n-LNF-GDC阴极制备过程[84]

Fig.15 n-LNF-GDC cathode preparation process[84]

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次数	150	705
比例	18%	82%

[1]	江洋, 彭长宏, 陈伟, 周豪, 马忠彬, 李洪博, 邱在容, 张国鹏, 周康根. 废旧磷酸铁锂粉料综合回收中试研究[J]. 化工学报, 2024, 75(6): 2353-2361.
[2]	赵亭亭, 鄢立祥, 唐福利, 肖敏之, 谭烨, 宋刘斌, 肖忠良, 李灵均. 光辅助锂-二氧化碳电池催化剂的设计策略与反应机理研究进展[J]. 化工学报, 2024, 75(5): 1750-1764.
[3]	王金山, 王世学, 朱禹. 冷却表面温差对高温质子交换膜燃料电池性能的影响[J]. 化工学报, 2024, 75(5): 2026-2035.
[4]	莫锦洪, 韩雪, 朱毅翔, 李菁, 王旭裕, 纪红兵. Pt-Ga/CeO₂-ZrO₂-Al₂O₃脱氢裂解双功能催化剂用于正丁烷催化制烯烃研究[J]. 化工学报, 2024, 75(5): 1855-1869.
[5]	丁禹, 杨昌泽, 李军, 孙会东, 商辉. 原子尺度钼系加氢脱硫催化剂的研究进展与展望[J]. 化工学报, 2024, 75(5): 1735-1749.
[6]	裴欣哲, 孙朱行, 林钰翔, 张朝阳, 钱勇, 吕兴才. 电催化分解液氨阳极材料的研究[J]. 化工学报, 2024, 75(5): 1843-1854.
[7]	程骁恺, 历伟, 王靖岱, 阳永荣. 镍催化可控/活性自由基聚合反应研究进展[J]. 化工学报, 2024, 75(4): 1105-1117.
[8]	吴希, 孙博, 刘银东, 齐传磊, 陈凯毅, 王路海, 许崇, 李永峰. 钠离子电池沥青基碳负极材料制备技术研究进展[J]. 化工学报, 2024, 75(4): 1270-1283.
[9]	韩宇, 周乐, 张鑫, 罗勇, 孙宝昌, 邹海魁, 陈建峰. 高黏附性Pd/SiO₂/NF整体式催化剂的制备及加氢性能研究[J]. 化工学报, 2024, 75(4): 1533-1542.
[10]	张劲, 郭志斌, 罗来明, 卢善富, 相艳. 5 kW重整甲醇高温质子交换膜燃料电池系统设计与性能[J]. 化工学报, 2024, 75(4): 1697-1704.
[11]	李添翼, 武玉泰, 王永胜, 顾佳锐, 宋沂恒, 杨丰铖, 郝广平. 轻同位素分离纯化与催化标记研究进展[J]. 化工学报, 2024, 75(4): 1284-1301.
[12]	孙铭泽, 黄鹤来, 牛志强. 铂基氧还原催化剂：从单晶电极到拓展表面纳米材料[J]. 化工学报, 2024, 75(4): 1256-1269.
[13]	李云璇, 刘新悦, 陈熙, 刘文, 周明月, 蓝兴英. 基于固液氧化还原靶向反应的能量存储技术：材料、器件及动力学[J]. 化工学报, 2024, 75(4): 1222-1240.
[14]	范以薇, 刘威, 李盈盈, 王培霞, 张吉松. 有机液体储氢中全氢化乙基咔唑催化脱氢研究进展[J]. 化工学报, 2024, 75(4): 1198-1208.
[15]	冯彬彬, 卢明佳, 黄志宏, 常译文, 崔志明. 碳载体在质子交换膜燃料电池中的应用及优化[J]. 化工学报, 2024, 75(4): 1469-1484.