硅酸盐学报

火焰法与喷雾干燥法共合成固体氧化物燃料电池阴极La_0.6Sr_0.4CoO_3-_δ-Ce_0.8Gd_0.2O_2-_δ的微观结构与性能分析

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王天齐 ¹ , 相龙凯 ² , 高展 ² , 张毅然 ¹ , 倪娜 ² , 屠恒勇 ² , 朱磊 ² , 黄震 ¹^,²

硅酸盐学报 | 氢能储能专题—研究论文 2024,52(6): 1810-1819

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硅酸盐学报 |氢能储能专题—研究论文 2024 , 52 (6) : 1810 -1819

火焰法与喷雾干燥法共合成固体氧化物燃料电池阴极La_0.6Sr_0.4CoO_3-_δ-Ce_0.8Gd_0.2O_2-_δ的微观结构与性能分析

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王天齐¹, 相龙凯², 高展², 张毅然¹, 倪娜², 屠恒勇², 朱磊², 黄震¹^,²

作者信息

^1．上海交通大学国家电投智慧能源创新学院，上海 200240

^2．上海交通大学机械与动力工程学院，上海 200240

通讯作者:

朱磊（1983—），男，博士，教授。

作者简介:

王天齐（1996—），男，硕士研究生。

Microstructure and Performance Analysis of Solid Oxide Fuel Cell La_0.6Sr_0.4CoO_3-_δ-Ce_0.8Gd_0.2O_2-_δ Cathode Synthesized by Flame Spray Pyrolysis and Spray Drying

Tianqi WANG¹, Longkai XIANG², Zhan GAO², Yiran ZHANG¹, Na NI², Hengyong TU², Lei ZHU², Zhen HUANG¹^,²

Affiliations

^1.College of Smart Energy, Shanghai Jiao Tong University, Shanghai 200240, China

^2.School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

Corresponding Author:

ZHU Lei (1983-), male, Ph.D., Professor. E-mail: tonyzhulei@sjtu.edu.cn

WANG Tianqi (1996-), male, Master candidate. E-mail: wtq_archie@sjtu.edu.cn

出版时间: 2024-06-20 doi: 10.14062/j.issn.0454-5648.20240112

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摘要

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实现阴极结构的纳米化以提升电极三相界面长度，是提升固体氧化物燃料电池（SOFC）性能的有效途径。基于火焰喷雾热解法和喷雾干燥法，分别一步法合成纳米级和亚微米级的La_0.6Sr_0.4CoO_3-δ-Ce_0.8Gd_0.2O_2-_δ复相材料。将2种粒径范围材料按照不同质量比混合，制成氧化钇部分稳定氧化锆电解质支撑的固体氧化物燃料电池的阴极，并系统分析电池性能与结构特征。结果表明，喷雾干燥合成材料与火焰喷雾热解合成材料的质量比为70∶30时，SOFC电化学性能最优，850 ℃时最大功率密度为0.47 W/cm²，面电阻为0.62 Ω·cm²，相应的欧姆阻抗和极化阻抗为0.36 Ω·cm²和0.26 Ω·cm²。实验证明，混合不同粒径颗粒制成的SOFC阴极，可有效构建电子-离子导通网络，并形成更多的三相界面和反应活性位点，从而获得较好的电化学性能。本研究为固体氧化物燃料电池阴极材料微观结构和性能优化提供了新的思路。

关键词

固体氧化物燃料电池 / 火焰喷雾热解法 / 喷雾干燥法 / 阴极 / 弛豫时间分布法

Abstract

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Introduction

Optimizing the nanostructure of the cathode is an effective approach to enhance the performance of solid oxide fuel cells at a triple-phase boundary (TPB). The most commonly used method is an impregnation method, which can produce nano-sized particles on the cathode framework structure. However, it is not able to achieve the related large-scale application due to its laborious preparation process and unstable performance. In this paper, nano-sized and submicron-sized composite powders of La_0.6Sr_0.4CoO_3-_δ-Ce_0.8Gd_0.2O_2-_δ (LSC-GDC) were synthesized by flame spray pyrolysis (FSP) and spray drying (SD) methods for the preparation of cathode, respectively.

Methods

A uniform submicron-sized LSC-GDC composite powder was prepared by SD with a solution of metal nitrates as a precursor solution. Also, a uniform nano-sized LSC-GDC composite powder was directly synthesized by FSP with a solution of metal acetates as a precursor solution. The submicron-sized and nano-sized powders were blended in different mass ratios (i.e., 100∶0, 90∶10, 80∶20, 70∶30, 60∶40, 50∶50, and 40∶60) to produce cathode slurries. These slurries were then screen-printed onto the button cells of NiO-GDC|GDC|3YSZ|GDC|LSC-GDC|LSC structure with an effective electrode area of approximately 0.5 cm². The voltammetric characteristics of the cells were tested by an electrochemical workstation. The electrochemical characterization was performed by electrochemical impedance spectroscopy (EIS) at open circuit voltage (OCV), and the impedance spectra were analyzed via distribution of relaxation time (DRT) analysis.

Results and discussion

Nano-sized particles synthesized by FSP and submicron-sized particles synthesized by SD can be distinguished via microscopic analysis. In addition, the fine particles are evenly distributed around the coarse particles, having a porous structure that meets an expected cathode microstructure. Under the experimental conditions, the overall ohmic impedance and polarization impedance both increase and then decrease as the proportion of nano-sized particles increases. The cathode performance is optimal when a mass ratio of SD powder: flame FSP powder is 70∶30. Under SOFC mode at 850 ℃, the maximum power density of the button cell is 0.47 W/cm², with an area specific resistance of 0.62 Ω·cm². The corresponding ohmic impedance and polarization impedance values are 0.36 Ω·cm² and 0.26 Ω·cm², respectively. Combined with the results by DRT analysis, the doping of an appropriate amount of nano-sized powder significantly enhances the cathode O₂ reduction reaction (ORR) process and cathode oxygen diffusion process.

Conclusions

Nano-sized and submicron-sized LSC-GDC composite materials were prepared by FSP and SD as one-pot methods, respectively. The feasibility of these two approaches for the large-scale preparation of SOFC cathode powders was investigated. The results showed that incorporating an appropriate amount of nano-sized powder into the submicron-sized powder for the preparation of the cathode could effectively enhance the cell performance.

Key words

solid oxide fuel cell / flame spray pyrolysis / spray drying / cathode / distribution of relaxation time

引用本文

王天齐, 相龙凯, 高展, 张毅然, 倪娜, 屠恒勇, 朱磊, 黄震. 火焰法与喷雾干燥法共合成固体氧化物燃料电池阴极La_0.6Sr_0.4CoO_3-_δ-Ce_0.8Gd_0.2O_2-_δ的微观结构与性能分析. 硅酸盐学报, 2024 , 52 (6) : 1810 -1819 . DOI: 10.14062/j.issn.0454-5648.20240112

Tianqi WANG, Longkai XIANG, Zhan GAO, Yiran ZHANG, Na NI, Hengyong TU, Lei ZHU, Zhen HUANG. Microstructure and Performance Analysis of Solid Oxide Fuel Cell La_0.6Sr_0.4CoO_3-_δ-Ce_0.8Gd_0.2O_2-_δ Cathode Synthesized by Flame Spray Pyrolysis and Spray Drying[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (6) : 1810 -1819 . DOI: 10.14062/j.issn.0454-5648.20240112

基金

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上海市市级科技重大专项
上海市基础研究试点项目(21ZQ1400207)
上海市科技创新行动计划(21DZ1206400)

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2024年第52卷第6期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240112

接收时间：2024-02-04
首发时间：2026-10-22
出版时间：2024-06-20

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收稿日期：2024-02-04
修回日期：2024-03-06

基金

上海市市级科技重大专项

上海市基础研究试点项目(21ZQ1400207)

上海市科技创新行动计划(21DZ1206400)

作者信息

^1．上海交通大学国家电投智慧能源创新学院，上海 200240

^2．上海交通大学机械与动力工程学院，上海 200240

通讯作者:

朱磊（1983—），男，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240112

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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