CN114400332B - 一种可逆固体氧化物电池的电极材料的复合材料、制备方法 - Google Patents
一种可逆固体氧化物电池的电极材料的复合材料、制备方法 Download PDFInfo
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Abstract
一种可逆固体氧化物电池的电极材料的复合材料、制备方法涉及电极材料领域,解决了现有电池成本高和寿命短的问题。所述复合材料为Sr3FeMoO6.5‑BiFe@Sr2‑xBixFe1.5Mo0.5O6‑δ,其中0<δ<0.2,0<x≤0.1。电极材料Sr2‑ xBixFe1.5Mo0.5O6‑δ为钙钛矿结构氧化物,本发明制备的钙钛矿结构的SBFM材料具有成分较简单、均匀,合成工艺较简单等特点。在氢气气氛中高温还原,析出大量且分布均匀的纳米颗粒,同时产生较多的氧空位。纳米颗粒可以显著提升SBFM电极材料的导电性能,并提供大量的活性位点,以SBFM作为阳极,对反应气体具有快速催化的作用。在碳氢燃料气氛中,钙钛矿阳极中析出的纳米颗粒具有良好的催化活性,表现出良好的电化学性能。同时以本发明的SBFM材料用于制备多孔阳极,可以在碳氢燃料气氛中稳定的工作。
Description
技术领域
本发明涉及电极材料领域,具体涉及一种可逆固体氧化物电池的电极材料的复合材料、制备方法。
背景技术
自改革开放以来,我国的能源行业取得了长足的发展,形成了以煤碳、石油、电力为核心,新能源和可再生能源全面发展的能源供应体系,为改善民生和经济发展提供了强有力的保证。然而,化石燃料的过度使用,如石油和煤炭,已经引发了许多问题,如空气污染,温室效应和动物灭绝。可逆对称固体氧化物电池(RSOC)作为一种能量转换装置,可以实现化学能和电能的高效洁净无污染的可逆转换。它既可以在固体氧化物燃料电池(solidoxide fuel cells,SOFCs)模式下运行,以电化学反应的方式将燃料中的化学能转化为电能,相比于受卡诺循环限制的传统发电技术,燃料电池减少了中间过程的能量损失,同时具有高转换效率、低污染和无噪音等优点。又可以在固体氧化物电解池(solid oxideelectrolysis cells,SOECs)模式下高效的将富余的电能快速高效地转换为化学能储存起来。然而,由于运行温度高(>850℃)所带来的一系列问题(成本高和寿命短等),阻碍了SOCs技术的商业化。因此迫切需要将SOCs的运行温度降低至中温区(600~800℃)。然而,温度的降低会使电极的极化电阻急剧增加,从而导致整个电池的性能衰减。因此,在中温区发展高效、稳定且成本低廉的电极材料对于实现SOCs商业化具有重要意义。
发明内容
为了解决现有技术中存在的问题,本发明提供了一种可逆固体氧化物电池的电极材料的复合材料、制备方法,解决了现有电池成本高和寿命短的问题。
本发明解决技术问题所采用的技术方案如下:
一种可逆固体氧化物电池的电极材料,所述电极材料为钙钛矿结构氧化物,结构式为Sr2-xBixFe1.5Mo0.5O6-δ,其中0<δ<0.2,0<x≤0.1。
制备一种可逆固体氧化物电池的电极材料的方法,该方法包括如下步骤:
步骤一:按化学计量比,称取含有Sr、Bi、Fe、Mo元素的粉末,加入无水乙醇进行搅拌处理,获得固液混合物;
步骤二:对步骤一所得的固液混合物球磨,直至充分混合均匀;
步骤三:将步骤二所得物质烘干,所得粉末在1100℃~1200℃烧结,烧结时间为10h~15h,获得钙钛矿结构的Sr2-xBixFe1.5Mo0.5O6-δ粉末,其中0<δ<0.2,0<x≤0.1。
优选的,步骤一所述的粉末为:所述含Sr元素的粉末为碳酸盐,Bi、Fe、Mo元素的粉末均为氧化物。
优选的,步骤二所述的球磨的速度为350-500转/分钟,球磨时间为12-24h。
优选的,所述电极材料作为阳极层在制备固体氧化物燃料电池中的应用。
一种可逆固体氧化物电池的电极材料的应用,该应用包括如下步骤:
步骤一:将电极粉末Sr2-xBixFe1.5Mo0.5O6-δ,其中0<δ<0.2,0<x≤0.1加入松油醇-乙基纤维素混合研磨,制成均匀混合的浆料作为阳极浆料;将阴极粉末NdBaCo2O5+δ加入松油醇-乙基纤维素混合研磨,制成均匀混合的阴极浆料;
步骤二:将步骤一得到的阳极浆料涂覆于电解质层两侧,在空气气氛下烧结获得钙钛矿Sr2-xBixFe1.5Mo0.5O6-δ的多孔电极层的固体氧化物燃料电池半电池;
步骤三:将步骤一得到的阳极浆料涂覆于电解质层一侧,阴极浆料涂覆于电解质另外一侧,在空气气氛下烧结获得钙钛矿Sr2-xBixFe1.5Mo0.5O6-δ的多孔电极层的固体氧化物燃料电池单电池。
一种复合材料,所述复合极材料为Sr3FeMoO6.5-BiFe@Sr2-xBixFe1.5Mo0.5O6-δ,其中0<δ<0.2,0<x≤0.1。
制备一种复合材料的方法,将电极材料Sr2-xBixFe1.5Mo0.5O6-δ,0<δ<0.2,0<x≤0.1至于还原气氛下经过煅烧得到。
一种复合材料的制备方法,所述还原气氛为氢气,还原时间为4h~6h,煅烧温度为800℃~900℃。
本发明的有益效果是:本发明制备的钙钛矿结构的SBFM材料属于一种新的电极材料,具有成分较简单、均匀,合成工艺较简单等特点。可在氢气气氛中进行高温还原,从而析出大量且分布均匀的纳米颗粒,同时产生较多的氧空位。这些纳米颗粒可以显著提升SBFM电极材料的导电性能,并提供大量的活性位点,以SBFM作为阳极,对反应气体具有快速催化的作用。在碳氢燃料气氛中,钙钛矿阳极中析出的纳米颗粒具有良好的催化活性,表现出良好的电化学性能。同时以本发明的SBFM材料用于制备多孔阳极,可以在碳氢燃料气氛中稳定的工作。
附图说明
图1为本发明Sr2Fe1.5Mo0.5O6-δ(SFM)和Sr1.9Bi0.1Fe1.5Mo0.5O6-δ(SBFM0.1)电极材料的XRD图。
图2本发明SBFM0.1电极材料还原后的XRD图。
图3本发明SBFM0.1电极材料还原后的透射电子显微镜图。
图4本发明SBFM0.1|LSGM|NBC的固体氧化物燃料电池以氢气作为燃料时,在不同温度下测得的功率密度图。
图5本发明SBFM0.1|LSGM|NBC的固体氧化物燃料电池以乙醇作为燃料时,在不同温度下测得的功率密度图。
具体实施方式
下面结合附图和实施例对本发明做进一步详细说明,但本发明的保护范围不局限于以下实施例。
实施例1
一种新型的可逆固体氧化物电池电极材料,具体分子式为Sr1.9Bi0.1Fe1.5Mo0.5O6-δ。
可逆固体氧化物电池电极材料的制备方法包括:取5.6098g碳酸锶,0.4659g三氧化二铋,2.3953g三氧化二铁,1.4396g三氧化钼,加入适量乙醇进行搅拌处理,获得固液混合物;将固液混合物置于球磨机中,以350转/分钟的速度球磨24h,将球磨后的粉体放入80℃的干燥箱里干燥。最后在空气氛围下1200℃焙烧12h得到具有钙钛矿相结构的Sr1.9Bi0.1Fe1.5Mo0.5O6-δ电极材料。将制备的电极材料在5%H2/Ar气氛中850℃还原5h后,获得具有钙钛矿支撑体结构的Sr3FeMoO6.5-BiFe@Sr1.9Bi0.1Fe1.5Mo0.5O6-δ的复合材料。
实施例2
一种新型的可逆固体氧化物电池电极材料,具体分子式为Sr1.92Bi0.08Fe1.5Mo0.5O6-δ。
可逆固体氧化物电池电极材料的制备方法包括:取5.6689g碳酸锶,0.3728g三氧化二铋,2.3953g三氧化二铁,1.4396g三氧化钼,加入适量乙醇进行搅拌处理,获得固液混合物;将固液混合物置于球磨机中,以450转/分钟的速度球磨20h,将球磨后的粉体放入80℃的干燥箱里干燥。最后在空气氛围下1150℃焙烧14h得到具有钙钛矿相结构的Sr1.92Bi0.08Fe1.5Mo0.5O6-δ电极材料。将制备的电极材料在5%H2/Ar气氛中900℃还原4h后,获得具有钙钛矿支撑体结构的Sr3FeMoO6.5-BiFe@Sr1.92Bi0.08Fe1.5Mo0.5O6-δ的复合材料。
实施例3
一种新型的可逆固体氧化物电池电极材料,具体分子式为Sr1.95Bi0.05Fe1.5Mo0.5O6-δ。
可逆固体氧化物电池电极材料的制备方法包括:取5.7575g碳酸锶,0.2329g三氧化二铋,2.3953g三氧化二铁,1.4396g三氧化钼,加入适量乙醇进行搅拌处理,获得固液混合物;将固液混合物置于球磨机中,以500转/分钟的速度球磨12h,将球磨后的粉体放入80℃的干燥箱里干燥。最后在空气氛围下1100℃焙烧15h得到具有钙钛矿相结构的Sr1.95Bi0.05Fe1.5Mo0.5O6-δ电极材料。将制备的电极材料在5%H2/Ar气氛中800℃还原6h后,获得具有钙钛矿支撑体结构的Sr3FeMoO6.5-BiFe@Sr1.95Bi0.05Fe1.5Mo0.5O6-δ的复合材料。
对实施例1所得的电极材料进行XRD分析表明所制备的氧化物对应钙钛矿的标准峰,如图1所示,没有杂峰出现,表明样品合成成功;将实施例1制备的电极材料在5%H2/Ar气氛中850℃还原5h后进行XRD分析,如图2所示,表明有金属纳米颗粒的出溶;通过透射电镜电镜观察还原后的材料表面形貌,如图3所示,同样表明有金属纳米颗粒的出溶。
以实施例1合成的材料为阳极材料,以NdBaCo2O5+δ为阴极材料,La0.9Sr0.1Ga0.8Mg0.2O3-δ(LSGM)作为电解质,将阳极粉末和阴极粉末分别与松油醇乙基纤维素混合,在研钵中研磨2h,分别制成均匀混合的浆料;通过丝网印刷的方式将浆料分别刷在电解质两侧组装成单电池,继而在空气氛围下950℃烧结处理4h,最终完成SBFM|LSGM|NBC的固体氧化物燃料单电池的制备。对单电池的阳极层(以SBFM0.1为例),先在H2气氛中进行850℃还原处理2h,随后在不同气氛中进行电化学性能测试,如图4和5所示。以氢气或乙醇为燃料时,电池的功率密度都随温度的增加而增加。相比于氢气,使用乙醇为燃料时开路电压会略有降低,并且相同温度下功率密度也略有降低。
Claims (3)
1.一种可逆固体氧化物电池的电极材料的复合材料,其特征在于,所述复合材料为Sr3FeMoO6.5-BiFe@Sr2-xBixFe1.5Mo0.5O6-δ,其中0<δ<0.2,0<x≤0.1,Sr2-xBixFe1.5Mo0.5O6-δ为钙钛矿结构氧化物。
2.制备权利要求1所述的一种复合材料的制备方法,其特征在于,将电极材料Sr2- xBixFe1.5Mo0.5O6-δ,0<δ<0.2,0<x≤0.1置于还原气氛下经过煅烧得到。
3.根据权利要求2所述的一种复合材料的制备方法,其特征在于,所述还原气氛为氢气,还原时间为4h~6h,煅烧温度为800℃~900℃。
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