碳燃料固体氧化物燃料电池结构研究进展

doi:10.11949/0438-1157.20221070

摘要/Abstract

摘要：

直接碳燃料固体氧化物燃料电池（direct carbon-fueled solid oxide fuel cells，DC-SOFC）是一种通过电化学过程将碳燃料的化学能直接转化为电能的发电装置，具有优异的发电效率、高的燃料利用率及低的碳排放。然而，相比气体和液体燃料，固体燃料的流动性较低，因此如何提高固体燃料传输速率并有效促进阳极反应动力学过程，以及在工作状态下高效、便捷地添加燃料是目前DC-SOFC要解决的关键问题。本文综述了近年来直接碳固体氧化物燃料电池结构的研究进展，总结了电池宏观结构与阳极微观形貌方面的发展，讨论了碳燃料固体氧化物燃料电池亟待解决的问题及发展方向。

关键词: 燃料电池, 显微结构, 电化学, 阳极, 碳燃料

Abstract:

Direct carbon-fueled solid oxide fuel cells (DC-SOFC) are power generation device that directly converts the chemical energy of carbon fuel into electrical energy through an electrochemical process. It has excellent power generation efficiency, high fuel efficiency and low carbon emissions. However, solid fuels are less mobile than gas and liquid fuels. So, at present, enhancing the solid fuel transfer rate to promote effectively the anode reaction kinetics process, and how to add fuel efficiently and conveniently are the key problems for DC-SOFC. In this paper, the recent progresses of DC-SOFC structure research are reviewed in terms of fuel cell macrostructure and anode micromorphology, and the key problems and development direction of carbon solid oxide fuel cell are also discussed.

Key words: fuel cells, microstructure, electrochemistry, anode, carbon fuel

中图分类号:

TM 911.4

郭祥, 乔金硕, 王振华, 孙旺, 孙克宁. 碳燃料固体氧化物燃料电池结构研究进展[J]. 化工学报, 2023, 74(1): 290-302.

Xiang GUO, Jinshuo QIAO, Zhenhua WANG, Wang SUN, Kening SUN. Progress of structure for carbon-fueled solid oxide fuel cells[J]. CIESC Journal, 2023, 74(1): 290-302.

图/表 17

图1 平板式四电池串联的SOFC堆[23]

Fig.1 Flat SOFC stack with four cells in series[23]

图2 无密封平板式DC-SOFC结构图[24]

Fig.2 Structure diagram of flat DC-SOFC with non-sealed[24]

图3 管状DCFC原理图[27]

Fig.3 Schematic diagram of tubular DCFC[27]

图4 电气共产示意图[30]

Fig.4 Schematic of the co-production of electricity and gas[30]

图5 三电池管状DC-SOFC电堆示意图[31]：（a）碳燃料在管内；（b）碳燃料在管外

Fig.5 Schematic diagram of the 3-cell-stacks of DC-SOFC system with carbon fuel inside (a) and outside (b) of stack[31]

图6 DC-SOFC原位分离CO/CO2结构示意图[32]

Fig.6 Structure schematic diagram of DC-SOFC in situ separation of CO/CO2[32]

图7 锥形阳极支撑SIS（segmented-in-series）-SOFC电堆示意图[33]

Fig.7 The schematic of the cone-shaped anode-supported SIS-SOFC stack[33]

图8 锥形单SOFC (a)和带有分段串联结构(b)的带有碳燃料的SOFC电堆示意图[34]

Fig.8 Schematic illustrations of cone-shaped single SOFC (a) and SOFC stack with a segmented-in-series configuration (b) with carbon fuel[34]

图9 静电纺丝工艺制备的中空纳米纤维结构形貌[20]

Fig.9 Morphological characterization of CMF hollow nanofibers[20]

图10 棉质纤维制备的阳极结构[39]（a）未装载燃料；（b）装载碳燃料并经过短暂测试

Fig.10 Structure of anode prepared from cotton fiber[39](a) before loading carbon; (b) after short electrochemical testing

图11 蜂窝阳极的碳燃料主反应示意图[21]

Fig.11 Carbon fuel main reaction processes for honeycomb anode[21]

图12 熔融态阳极SOFC工作示意图[42]

Fig.12 Schematic diagram of molten anode SOFC operation[42]

图13 指孔形结构陶瓷扫描电镜图[72]

Fig.13 Scanning electron microscope (SEM) images of ceramics with finger-like hole structure[72]

图14 不使用安全气体的CO2/H2O电解原理图[81]

Fig.14 Schematic diagram of CO2/H2O electrolysis without using the safe gas[81]

图15 （a）U形管状连续供给装置；（b）800℃下电流密度为150 mA/cm2的电池电压与时间函数[84]

Fig.15 (a) U-shaped tubular continuous supply device; (b) Cell voltage as a function of time at 800℃ under a constant polarization current density of 150 mA/cm2 [84]

图16 基于DC-SOFC技术的连续供煤电厂方案[24]

Fig.16 A scheme of power plant based on DC-SOFC technology with continuous supply of coal[24]

表1 直接碳燃料电池燃料及电极

Table 1 Fuels and electrodes of direct carbon fuel cells

燃料	辅助剂	阳极	电解质	阴极	温度/℃	最大功率密度/(mW/cm²)
褐煤^[9]	—	Ag-Gd_0.1Ce_0.9O_2-_δ	YSZ	Ag-Gd_0.1Ce_0.9O_2-_δ	850	221
牙签炭^[36]	—	La_0.3Sr_0.7Fe_0.7Ti_0.3O_3-_δ (LSFT)	YSZ	La_0.3Sr_0.7Fe_0.7Ti_0.3O_3-_δ (LSFT)	850	223
活性炭^[86]	5%（质量分数）BaCO₃	Ag-GDC	YSZ	Ag-GDC	850	328.4
低硫(0.15%)阿拉斯加煤^[87]	CO₂吹扫	Ni-YSZ	YSZ	钙钛矿	930	450
小麦秸秆炭^[88]	—	Ag-Ce_0.8Gd_0.2O_1.9	YSZ	Ag-Ce_0.8Gd_0.2O_1.9	800	187
玉米芯炭^[88]	—	Ag-Ce_0.8Gd_0.2O_1.9	YSZ	Ag-Ce_0.8Gd_0.2O_1.9	800	204
甘蔗渣炭^[88]	—	Ag-Ce_0.8Gd_0.2O_1.9	YSZ	Ag-Ce_0.8Gd_0.2O_1.9	800	260
活性炭^[89]	—	La_0.8Sr_0.2Fe_0.9Nb_0.1O_3-_δ	ScSZ	LSM/ScSZ	850	302.8
玉米秸秆炭^[89]	—	La_0.8Sr_0.2Fe_0.9Nb_0.1O_3-_δ	ScSZ	LSM/ScSZ	850	218.5
石墨^[90]	Ar	Pt	YSZ	Pt	950	16.8
活性炭^[63]	Li₂CO₃+K₂CO₃ Ar	Ni-SDC	SDC	Ba_0.5Sr_0.5Co_0.8Fe_0.2O_3-_δ	750	158.3
废旧纸箱制炭^[91]	—	La_0.3Sr_0.7Fe_0.7Ti_0.3O_3-_δ	SSZ	La_0.3Sr_0.7Fe_0.7Ti_0.3O_3-_δ	850	308.7
海带炭^[92]	—	Ag-GDC	YSZ	Ag-GDC	850	285
核桃壳炭^[93]	Fe	Ag-GDC	YSZ	Ag-GDC	800	205
兰花树叶炭^[94]	—	Ag-GDC	YSZ	Ag-GDC	850	212
活性炭^[35]	—	Ni/Fe-YSZ	YSZ	La_0.6Sr_0.4Co_0.2Fe_0.8O₃-GDC	800	425~529
工业焦炭^[38]	Fe	Ag-GDC	YSZ	Ag-GDC	850	217
小麦秸秆炭^[95]	Ca	Ag-GDC	YSZ	Ag-GDC	800	258
椰壳炭^[96]	Fe	Ag-GDC	YSZ	Ag-GDC	800	274
活性炭^[97]	Li₂CO₃+K₂CO₃ Ar	(PrBa)_0.95Fe_1.4Cu_0.4Nb_0.2O₅₊_δ	LSGM	La_0.6Sr_0.4Co_0.2Fe_0.8O₃	800	431

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