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。本文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了对比分析，并且对提高SOC空气电极抗铬性能的研究进行了总结和展望。

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 such as high energy efficiency, low pollution emissions, and high fuel flexibility, making them crucial 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 modes are reviewed. Additionally, it summarizes and prospects the research on improving the resistance of SOC air electrodes to chromium poisoning.

Key words: solid oxide cells, air electrode, chromium poisoning, chromium resistivity

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, DOI: 10.11949/0438-1157.20240130.

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, DOI: 10.11949/0438-1157.20240130.

图/表 17

图1 SOC在发电和电解模式下的工作原理示意图[3]

Fig. 1 SOC working principle schematics when working as fuel cell and electrolysis cell[3]

图2 阴极材料晶体结构[7]注:(a)立方钙钛矿结构 (b)双钙钛矿结构

Fig. 2 Crystal structure of cathode materials [7]

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变化图[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图[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·cm^-2）	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	SUS430，20h	1.10	34.80	0.75	1.20	^[33]
750	200	SUS430，20h	1.12	32.25	0.22	0.30	^[33]
750	800	SUS430，20h	2.00	33.00	0.12	1.20	^[33]
800	200	FCM，20h	1.80	1.02	0.40	0.97	^[34]
800	200	FCMM，20h	-0.05	-1.57	-0.18	0.14	^[34]
900	200	RA446，20h	0.21	0.79	0.12	0.73	^[35]

图6 LSM阴极铬物种沉积注:(a)开路电压 (b)恒定电流密度

Fig. 6 LSM cathode chromium species deposition map

图7 LSM（A，B）与LSCF（C,D）铬中毒前后扫描电镜图[36]

Fig. 7 Scanning electron microscopy of LSM (A, B) and LSCF (C,D) 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	Reference
700	OCV	LSCF	SUS430，40h	-	0.36	^[42]
700	OCV	LSCF-Ag	SUS430，40h	-	0.02	^[47]
700	OCV	LSCF	Crofer22H，200h	0.60	0.48	^[73]
700	OCV	LSCF-GDC0.24	Crofer22H，200h	0.20	0.28	^[47]
700	OCV	LSCF-GDC0.32	Crofer22H，200h	0.08	0.12	^[47]
700	100	LSCF	Crofer22H，200h	0.76	0.77	^[47]
700	100	LSCF-GDC0.24	Crofer22H，200h	0.24	0.34	^[47]
700	100	LSCF-GDC0.32	Crofer22H，200h	0.11	0.20	^[47]
800	OCV	LSCF	RA446，20h	0.76	1.22	^[39]
800	200	LSCF	RA446，20h	0.74	1.49	^[39]
900	OCV	LSCF	RA446，20h	0.76	0.18	^[39]
900	200	LSCF	RA446，20h	0.69	0.18	^[39]

图8 LSCF阴极OCV与恒定电流密度下铬中毒对比图[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（a）与阳极极化（b）铬中毒机制注:(a) (b)

Fig. 9 Cathode polarization (a) and anode polarization (b) 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（a）与阳极极化（b）铬中毒机理

Fig. 11 Cathode polarization (a) and anode polarization (b) 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16 n-LNF-GDC阴极制备过程[84]

Fig. 16 n-LNF-GDC cathode preparation process[84]

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