Preparation and Performances of Tubular Cone-shaped Anode-supported Segmented-in-series Direct Carbon Solid Oxide Fuel Cell

doi:10.15541/jim20230597

Abstract

Abstract:

To solve the problem of large concentration polarization impedance of anode-supported direct carbon solid oxide fuel cell (DC-SOFC), tubular cone-shaped anode-supported segmented-in-series solid oxide fuel cell (SOFC) was prepared by an improved gel-casting method. By appropriately increasing content of the solvent, fluidity of the slurry and quality of the obtained product were improved. By increasing content of the pore-forming agent, the porosity of the anode was increased, reducing the diffusion resistance of gas. As-improved SOFC was fueled by hydrogen and operated at 800 ℃ with an open-circuit voltage of 1.05 V. The polarization impedance of the electrochemical impedance spectrum decreased while the maximum power density was 0.67 W•cm^-2 and the active area of the cathode was 2.2 cm². These SOFC electrochemical performances were significantly higher than that before improvement. Activated carbon loaded on the anode with 5% (in mass) K as catalyst was directedly used as the fuel of SOFCs. Using this anode-supported direct carbon, the DC-SOFC was prepared, showing an open circuit voltage of 1.030 V and a peak power density of 0.74 W•cm^-2 at 800 ℃. This DC-SOFC was discharged at a constant current of 400 mA, and its effective utilization rate of carbon fuel was 31% which was higher than that before improvement (17%). Four improved tubular cone-shaped single cells were connected in series to form a four-cell stack, showing a peak power of 8.0 W and a corresponding power density of 0.91 W•cm^-2 at 800 ℃, which was higher than that before improvement (4.1 W), exceeding the maximum of previous reported DC-SOFC, and displayed an effective utilization rate of 15% for carbon fuel.

Key words: direct carbon solid oxide fuel cell, gel-casting, Boudouard reaction, tubular cone-shaped segmented-in-series, potassium catalyst

CLC Number:

TQ174

YE Zibin, ZOU Gaochang, WU Qiwen, YAN Xiaomin, ZHOU Mingyang, LIU Jiang. Preparation and Performances of Tubular Cone-shaped Anode-supported Segmented-in-series Direct Carbon Solid Oxide Fuel Cell[J]. Journal of Inorganic Materials, 2024, 39(7): 819-827.

Figures/Tables 8

Table S1 Raw materials and chemical reagents

化学试剂	生产公司	纯度
NiO	加拿大Inco公司	98%
YSZ	宜兴市熠辉耐磨材料有限公司	99.9%
丙烯酰胺	上海阿拉丁生化科技有限公司	分析纯
N, N'-亚甲基双丙烯酰胺	上海阿拉丁生化科技有限公司	分析纯
柠檬酸铵	上海麦克林生化科技有限公司	分析纯
聚乙二醇	上海阿拉丁生化科技有限公司	99.0%
邻苯二甲酸二辛酯	上海麦克林生化科技有限公司	99.0%
三乙醇胺	上海麦克林生化科技有限公司	99.0%
聚乙烯醇缩丁醛	上海阿拉丁生化科技有限公司	99.0%
Al₂O₃	淄博信富盟化工有限公司	99.0%
GDC	中国科学院宁波材料技术与工程研究所	99.50%
银导电胶DAD-87	上海合成树脂研究所	99.99%
粒状活性炭	上海阿拉丁试剂有限公司	触媒载体用
碳酸钾	上海麦克林生化科技有限公司	99%

Fig. 1 Preparation of solid oxide fuel cells (a) Illustration of process for preparing anode supports; (b) Photo of a series of tubular cone-shaped SOFCs at different preparation stages (2-6) in contrast to green anode support (1); (c) The segmented-in-series four-cell stack; The tubular cone-shaped SOFCs marked with 2-6 are pre-sintered anode support, anode support with a co-sintered functional layer, anode support coated with electrolyte layer, completed tubular cone-shaped cell with one end closed, and completed tubular cone-shaped cell with both ends open, respectively

Fig. 2 Illustration of testing system of the segmented-in-series four-cell stack

Table 1 Comparison of the composition of gel-casting slurries

Component	Ref.[34]	Ref.[37]	This work
NiO-YSZ	49.7%	57.5%	44.2%
AM	7.9%	11.5%	7.1%
MBAM	0.8%	0.6%	0.9%
Deionized water	20.7%	17.2%	26%
Graphite	10%	11.5%	13.2%
AC	1.7%	-	1.3%
Polyacrylic acid	-	1.7%	-
TEA	1.0%	-	-
PEG-600	8.2%	-	7.3%

Fig. 3 Electrochemical performance and microstructure of hydrogen-fueled SOFC single cell before and after process improvement (a, b) Output performances; (c) Electrochemical impedance spectra; (d) Comparison of the corresponding fitted resistances; (e, f) Microstructures of the SOFC observated by SEM. Colorful figures are available on website

Fig. 4 Electrochemical performance of a single DC-SOFC using 5% (in mass) K activated carbon (a) Output performances; (b) Open circuit voltages; (c) Electrochemical impedance spectra; (d) Comparison of the corresponding fitted resistances; (e) Discharge characteristics. Colorful figures are available on website

Fig. 5 Microstructure of the DC-SOFC anode after testing (a-d) Surface SEM image (a) and EDS mappings of K (b), C (c) and Ag (d); (e-g) Cross-sectional SEM image (e) and EDS mappings of K (f) and C (g)

Fig. 6 (a) Output performance and (b) discharge characteristic of the tubular cone-shaped segmented-in-series stack fueled by 5% (in mass) K-loaded activated carbon

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