CN110707205A - 一种提升Te基热电接头性能的方法 - Google Patents
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Abstract
本发明一种提升Te基热电接头性能的方法,属热电器件制备和连接件技术领域,其特征在于在热电材料和电极材料之间引入合适的化合物作为阻隔层,构建热电接头浓度梯度结构,解决二者连接过程中元素的严重扩散导致的热电接头性能削弱的问题,实现热电接头性能提升和服役寿命提高的目的。通过在Fe和Te之间引入FexTey(0<x/y<1.5)化合物作为阻隔层,采用放电等离子烧结方法(SPS)制备了Te\FexTey\Fe梯度连接结构,在外加电场和压力场的耦合作用下,在实现材料致密化的同时,同步实现阻隔层与二者之间的扩散反应而形成连接。通过引入阻隔层控制热电材料和电极材料中的元素平衡,解决热电接头界面两侧原子的过度扩散问题,提升接头性能,提高界面稳定性。
Description
技术领域
本发明一种提升Te基热电接头性能的方法属于热电器件制备和连接件技术领域,具体涉及一种提升Te基热电接头性能的方法。通过在Te基热电材料和电极之间引入合适的化合物作为阻隔层,构成梯度连接结构,这种方法有效抑制了热电材料和电极材料之间过度的元素扩散,从而实现Te基热电接头的性能大大提升。
背景技术
Te基热电材料以其优异的热电性能得到科研工作者的广泛关注,但该领域关于器件制备和连接界面的研究尚属空白。在Te基热电材料和电极的连接过程中,温度和化学势梯度的共同作用促使原子沿垂直于界面方向进行定向输运,严重影响了热电材料和电极材料的热电输运性能,导致接头热电转换效率降低。
发明内容
本发明一种提升Te基热电接头性能的方法,目的在于通过引入符合性能要求的化合物作为阻隔层,减小热电材料和电极材料两侧元素的浓度梯度,进而抑制在材料合成和同步扩散连接过程中元素的过度扩散对热电材料以及电极材料性能的影响,从而达到提升热电接头的性能的目的。
本发明由如下技术方案实现的:一种提升Te基热电接头性能的方法,其特征在于是一种以本征Te作为热电材料,Fe和FexTey(0<x/y<1.5)化合物分别为电极和阻隔层,采用放电等离子烧结方法(SPS)制备了Te\FexTey\Fe梯度连接结构,在外加电场和压力场的耦合作用下,在实现材料致密化的同时,同步实现三者之间的扩散反应而形成连接的方法;具体步骤如下:
(1)原料准备:将纯度≥99.99%的块体Te手工研磨作为粉体1;将颗粒度小于50μm,纯度≥99.9%的Fe粉作为粉体2;将粉体1和粉体2按照化学计量比称量并充分混合后得到成分为FexTey(0<x/y<1.5)的粉体3;
(2)粉体装入模具:将粉体1装入石墨模具中,冷压至50-60%致密度;再将粉体3置于粉体1上方,同样冷压至50-60%致密度;最后将粉体2置于粉体3上方,再次冷压至50-60%致密度备用;
(3)烧结连接:将装有粉体的石墨模具放入热压炉中进行烧结连接,首先预压2.5-5MPa,待炉中真空度抽到高于20Pa后,充入99.999%的氩气至0.05MPa,再通入脉冲电流以50-100℃/min的加热速率匀速升温,粉体升温至350℃保温2-5min,同时将压力提升至40-60MPa;保温结束后,将烧结温度升至400-420℃,保温15-20min;然后以10-15℃/min的速率均匀降温至300℃,随后卸压冷却,形成热电接头。
本发明一种提升Te基热电接头性能的方法,其优点在于:在Te基热电材料和电极材料Fe之间引入FexTey(0<x/y<1.5)作为阻隔层,制备了Te\FexTey\Fe梯度连接结构,解决了热电材料和电极材料在扩散连接过程中元素的过度扩散,大幅度提升了热电接头的性能和服役寿命。
附图说明
图1为热电接头Te\FexTey\Fe连接界面处微观形貌
①区域表示Te;②区域表示化合物相β;③区域表示Fe。
具体实施方式
实施方式1:一种提升Te基热电接头性能的方法。将纯度≥99.99%的块体Te手工研磨作为粉体1;将颗粒度小于50μm,纯度≥99.9%的Fe粉作为粉体2;将粉体1和粉体2按照化学计量比称量并充分混合后得到成分为Fe53Te47的粉体3。将粉体1装入石墨模具中,冷压至50-60%致密度;再将粉体3置于粉体1上方,同样冷压至50-60%致密度;最后将粉体2置于粉体3上方,再次冷压至50-60%致密度备用。将上述模具放入热压炉中进行烧结连接,首先预压2.5MPa,待炉中真空度抽到高于20Pa后,充入高纯氩气(99.999%)至0.05MPa,再通入脉冲电流以100℃/min的加热速率匀速升温,将粉体升温至350℃保温2min,同时将压力提升至40MPa,保温结束后,将烧结温度升至420℃,保温15min后,以12℃/min的速率均匀降温至300℃,随后卸压冷却,形成梯度结构热电接头Te\Fe53Te47\Fe。对实验得到的梯度结构热电接头截面进行了X射线能谱扫描(EDS),结果如图1所示,其中①区域表示Te,②区域表示化合物相β,③区域表示Fe。可以发现②在①和③之间能够起到很好的阻隔作用,引入②有效解决了①和③连接过程中存在的严重的元素扩散问题,扩散反应层厚度由500+μm减小到10μm左右。且在扫描电子显微镜(SEM)下可以观察到其与二者的连接质量较Te\Fe好,②与①和③的接触电阻分别为50.75μΩ·cm2和14.43μΩ·cm2,与Te\Fe接头中近100μΩ·cm2的接触电阻相比有了明显改善,所以引入β相是一种提升Te基热电接头性能的有效方法。
实施方式2:一种提升Te基热电接头性能的方法。将纯度≥99.99%的块体Te手工研磨作为粉体1;将颗粒度小于50μm,纯度≥99.9%的Fe粉作为粉体2;将粉体1和粉体2按照化学计量比称量并充分混合后得到成分为Fe53Te47的粉体3。将粉体1装入石墨模具中,冷压至50-60%致密度;再将粉体3置于粉体1上方,同样冷压至50-60%致密度;最后将粉体2置于粉体3上方,再次冷压至50-60%致密度备用。将上述模具放入热压炉中进行烧结连接,首先预压2.5MPa,待炉中真空度抽到高于20Pa后,充入高纯氩气(99.999%)至0.05MPa,再通入脉冲电流以100℃/min的加热速率匀速升温,将粉体升温至350℃保温2min,同时将压力提升至50MPa,保温结束后,将烧结温度升至415℃,保温20min后,以12℃/min的速率均匀降温至300℃,随后卸压冷却,形成梯度结构热电接头Te\Fe53Te47\Fe。对实验得到的梯度结构热电接头截面进行了X射线能谱扫描(EDS),结果与实施例1相似,可以发现②在改变温度和保温时间等实验条件后仍够起到很好的阻隔作用,有效解决①和③连接过程中存在的严重的元素扩散问题。②与①和③的接触电阻分别为41.38μΩ·cm2和9.22μΩ·cm2。与Te\Fe接头中近100μΩ·cm2的接触电阻相比有了更明显改善,所以引入β相是一种提升Te基热电接头性能的有效方法。
实施方式3:一种提升Te基热电接头性能的方法。将纯度≥99.99%的块体Te手工研磨作为粉体1;将颗粒度小于50μm,纯度≥99.9%的Fe粉作为粉体2;将粉体1和粉体2按照化学计量比称量并充分混合后得到成分为Fe33Te67的粉体3。将粉体1装入石墨模具中,冷压至50-60%致密度;再将粉体3置于粉体1上方,同样冷压至50-60%致密度;最后将粉体2置于粉体3上方,再次冷压至50-60%致密度备用。将上述模具放入热压炉中进行烧结连接,首先预压2.5MPa,待炉中真空度抽到高于20Pa后,充入高纯氩气(99.999%)至0.05MPa,再通入脉冲电流以100℃/min的加热速率匀速升温,将粉体升温至350℃保温2min,同时将压力提升至40MPa,保温结束后,将烧结温度升至420℃,保温15min后,以12℃/min的速率均匀降温至300℃,随后卸压冷却,形成梯度结构热电接头Te\Fe33Te67\Fe。对实验得到的梯度结构热电接头截面进行了X射线能谱扫描(EDS),结果与实施例1相似,扩散反应层厚度也仅有10μm左右,可以发现改变化学计量比后的②仍够起到很好的阻隔作用,有效解决①和③连接过程中存在的严重的元素扩散问题。且在扫描电子显微镜(SEM)下可以观察到其与二者的连接质量较Te\Fe好,②与①和③的接触电阻分别为43.23μΩ·cm2和17.52μΩ·cm2,与Te\Fe接头中近100μΩ·cm2的接触电阻相比有了更明显改善,引入β相也是一种提升Te基热电接头性能的有效方法。
Claims (1)
1.一种提升Te基热电接头性能的方法,其特征在于是一种采用FexTey(0<x/y<1.5)作为Te基热电材料和Fe电极的阻隔层,采用放电等离子烧结方法制备了Te\FexTey\Fe梯度连接结构,在外加电场和压力场的耦合作用下,在实现材料致密化的同时,同步实现三者之间的扩散反应而形成连接的方法;具体步骤如下:
1)原料准备:将纯度≥99.99%的块体Te手工研磨作为粉体1;将颗粒度小于50μm,纯度≥99.9%的Fe粉作为粉体2;将粉体1和粉体2按照化学计量比称量并充分混合后得到成分为FexTey的粉体3;
2)粉体装入模具:将粉体1装入石墨模具中,冷压至50-60%致密度;再将粉体3置于粉体1上方,同样冷压至50-60%致密度;最后将粉体2置于粉体3上方,再次冷压至50-60%致密度备用;
3)烧结连接:将装有粉体的石墨模具放入热压炉中进行烧结连接,首先预压2.5-5MPa,待炉中真空度抽到高于20Pa后,充入99.999%的氩气至0.05MPa,再通入脉冲电流以50-100℃/min的加热速率匀速升温,粉体升温至350℃保温2-5min,同时将压力提升至40-60MPa;保温结束后,将烧结温度升至400-420℃,保温15-20min;然后以10-15℃/min的速率均匀降温至300℃,随后卸压冷却,形成热电接头。
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US3208835A (en) * | 1961-04-27 | 1965-09-28 | Westinghouse Electric Corp | Thermoelectric members |
CN1173742A (zh) * | 1996-07-26 | 1998-02-18 | 株式会社泰库诺瓦 | 热电半导体及其制造工艺 |
CN109219893A (zh) * | 2016-06-01 | 2019-01-15 | Lg伊诺特有限公司 | 热电臂及包括该热电臂的热电元件 |
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US3208835A (en) * | 1961-04-27 | 1965-09-28 | Westinghouse Electric Corp | Thermoelectric members |
CN1173742A (zh) * | 1996-07-26 | 1998-02-18 | 株式会社泰库诺瓦 | 热电半导体及其制造工艺 |
CN109219893A (zh) * | 2016-06-01 | 2019-01-15 | Lg伊诺特有限公司 | 热电臂及包括该热电臂的热电元件 |
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