Ba_(1-x)（M）_xCo_(0.9-y)Fe_yNb_(0.1)O_(3-δ)材料性能及电化学应用研究
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摘要
钙钛矿型混合导体是一类同时具有电子和离子导电性能的材料,可以广泛应用于透氧膜(OTM)、固体氧化物燃料电池(SOFC)及固体氧化物电解池(SOEC),从而引起了化学、材料及物理等领域的科研工作者的广泛关注。
本文在材料选择与设计基础上,从合成过程-性能分析-实际应用出发,首先采用固相合成方法制备了Ba1.0Co0.7Fe0.2Nb0.1O3-δ混合电导钙钛矿材料,然后系统评价了Ba缺位及Fe掺杂浓度对Ba1.0Co0.7Fe0.2Nb0.1O3-δ(x=0-0.15, y=0-0.9)材料热膨胀系数、电化学性能的影响。同时评价了Ba1.0Co0.7Fe0.2Nb0.1O3-δ(BCF0.4N)及Ba0.9Co0.7Fe0.2Nb0.1O3.δ(B0.9CFN)与中温电解质材料La0.8Sr0.2Ga0.83Mg0.17O3-δ的化学相容性。在此基础上首次研究了具有p型半导体导电性质的BCF0.4N作为SOEC氧电极的应用可行性及高钴、高活性的B0.9CFN应用于SOFC阴极及OTM的长期稳定性。
最后,通过原位还原混合电导钙钛矿材料Pr0.4Sr0.6CQ0.2Fe0.7Nb0.1O3-δ,开发了新型微纳结构的陶瓷合金复合阳极材料。该复合阳极材料具有很好的抗硫耐积碳性能及氧化还原循环稳定性。综上,通过本文研究为混合电导材料工业化应用奠定了坚实基础。
In recent years, mixed-conducting perovskite-type materials have attracted great attentions to researchers in the fields of chemistry, materials and physics. These materials can be used in many applications such as Oxygen Transport Membranes (OTM), Solid Oxide Fuel Cell (SOFC) and Solid Oxide Electrolysis Cell (SOEC).
In this study, BaCo0.7Fe0.2Nb0.1O3-δhas been synthesized using a solid state reaction method based on the study of synthesis process-performance analysis-practical application. The effects of A-site cation deficiency and B-site iron doping concentration on the thermal expansion coefficient (TEC) and electrochemical performance of Ba1-xCo0.9-yFeyNb0.1O3_δ(x=0-0.15,y=0-0.9) have been systematically evaluated. X-ray diffraction results showed that Bao.9Coo.sFeo.4Nb0.1O3.5(BCF0.4N) and Ba0.9Co0.7Fe0.2Nb0.1O3-δ(B0.9CFN) were chemically compatible with the La0.8Sr0.2Ga0.83Mg0.17O3-δLSGM) electrolyte. A novel BCF0.4N was prepared and characterized as oxygen electrode for SOEC. The performance and stability of B0.9CFN for OTM application and as cathode for LSGM-electrolyte supported SOFCs were reporetd for the first time.
Furthermore, a novel ceramic-alloy composite anode obtained by reduction of Pr0.4Sr0.6Co0.2Fe0.7Nbo0.1O3-δ has been reported. The novel ceramic-alloy composite anode has demonstrated excellent sulfur tolerance and coking resistance as well as redox cyclability. In conclusion, this dissertation has established a solid foundation for the practical application of mix-conducting materials.
本文在材料选择与设计基础上,从合成过程-性能分析-实际应用出发,首先采用固相合成方法制备了Ba1.0Co0.7Fe0.2Nb0.1O3-δ混合电导钙钛矿材料,然后系统评价了Ba缺位及Fe掺杂浓度对Ba1.0Co0.7Fe0.2Nb0.1O3-δ(x=0-0.15, y=0-0.9)材料热膨胀系数、电化学性能的影响。同时评价了Ba1.0Co0.7Fe0.2Nb0.1O3-δ(BCF0.4N)及Ba0.9Co0.7Fe0.2Nb0.1O3.δ(B0.9CFN)与中温电解质材料La0.8Sr0.2Ga0.83Mg0.17O3-δ的化学相容性。在此基础上首次研究了具有p型半导体导电性质的BCF0.4N作为SOEC氧电极的应用可行性及高钴、高活性的B0.9CFN应用于SOFC阴极及OTM的长期稳定性。
最后,通过原位还原混合电导钙钛矿材料Pr0.4Sr0.6CQ0.2Fe0.7Nb0.1O3-δ,开发了新型微纳结构的陶瓷合金复合阳极材料。该复合阳极材料具有很好的抗硫耐积碳性能及氧化还原循环稳定性。综上,通过本文研究为混合电导材料工业化应用奠定了坚实基础。
In recent years, mixed-conducting perovskite-type materials have attracted great attentions to researchers in the fields of chemistry, materials and physics. These materials can be used in many applications such as Oxygen Transport Membranes (OTM), Solid Oxide Fuel Cell (SOFC) and Solid Oxide Electrolysis Cell (SOEC).
In this study, BaCo0.7Fe0.2Nb0.1O3-δhas been synthesized using a solid state reaction method based on the study of synthesis process-performance analysis-practical application. The effects of A-site cation deficiency and B-site iron doping concentration on the thermal expansion coefficient (TEC) and electrochemical performance of Ba1-xCo0.9-yFeyNb0.1O3_δ(x=0-0.15,y=0-0.9) have been systematically evaluated. X-ray diffraction results showed that Bao.9Coo.sFeo.4Nb0.1O3.5(BCF0.4N) and Ba0.9Co0.7Fe0.2Nb0.1O3-δ(B0.9CFN) were chemically compatible with the La0.8Sr0.2Ga0.83Mg0.17O3-δLSGM) electrolyte. A novel BCF0.4N was prepared and characterized as oxygen electrode for SOEC. The performance and stability of B0.9CFN for OTM application and as cathode for LSGM-electrolyte supported SOFCs were reporetd for the first time.
Furthermore, a novel ceramic-alloy composite anode obtained by reduction of Pr0.4Sr0.6Co0.2Fe0.7Nbo0.1O3-δ has been reported. The novel ceramic-alloy composite anode has demonstrated excellent sulfur tolerance and coking resistance as well as redox cyclability. In conclusion, this dissertation has established a solid foundation for the practical application of mix-conducting materials.
引文
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