N型Mg3Sb2基热电材料和发电器件的制备及研究

热电技术能够回收利用低品位余热将其转换成清洁无污染的电能，从而提高能源利用效率、实现节能减排。在诸多热电材料体系中，Mg₃Sb₂基热电材料凭借其无毒无污染、价廉、含量丰富的优势，在中低温热电发电领域有着巨大的应用前景。尽管Mg₃Sb₂基材料的热电性能提升策略被广泛研究，但其相关的阻挡层界面和发电器件制备的研究报道很少。因此制备高热电性能的n型Mg₃Sb₂基材料以及优化其热电发电器件的界面设计和制备方法有着重要意义。本课题利用行星球磨和放电等离子烧结方法制备n型Mg₃Sb₂基材料，对材料性能提升、阻挡层制备以及发电器件制备进行了研究，获得了高热电性能的n型Mg₃Sb₂基材料，并制备了具有高能量转换效率的热电发电器件。主要的研究成果如下：

本课题通过多壁碳纳米管（MWCNTs）和Cu的掺杂策略提升了n型Mg₃Sb₂基材料的热电性能。少量的MWCNTs掺杂使得功率因子显著提高，并且降低了热导率，从而提高样品的ZT值。而微量Cu元素掺杂能够有效提高样品的低温ZT值。微量Cu和MWCNTs共同掺杂可以结合两者对样品热电性能的有利影响。Mg_3.5Sb_1.5Bi_0.45Te_0.05Cu_0.01/ 0.1_wt% CNT共掺样品在整个工作温度范围内的ZT值得到提高，749K时样品的ZT峰值为1.7，室温ZT值也有约20%的提高，而且样品的热电性能可重复性好。

本课题对n型Mg₃Sb₂基热电材料的两种阻挡层界面进行了研究。在600℃、20min的放电等离子烧结条件下，相比于Fe-Co合金，316L不锈钢作为阻挡层时样品与原热电材料有着更相近的功率因子。Fe-Co合金阻挡层的厚度和致密度不均匀，在烧结制备时阻挡层中就已经存在较为明显的元素扩散。316L不锈钢阻挡层结构致密且均匀，可以在阻挡层制备的过程中有效地阻止元素扩散，经过退火后各种元素的分布情况与退火前相比没有显著变化。故316L不锈钢作为阻挡层时，界面有良好的热稳定性。

本课题制备了具有高能量转换效率的发电器件。利用n型Mg₃Sb₂材料和p型PbTe材料制备包含两对热电臂的发电器件。当热端温度为766K，电流为2.32A时，器件的最大输出功率约为0.5W，最大能量转换效率为10.3%。

Thermoelectric technology can recycle low-grade waste heat and convert it into clean electrical energy, thereby improving energy efficiency and achieving energy conservation and emission reduction. Among many thermoelectric material systems, Mg₃Sb₂-based thermoelectric materials have great application prospects in the field of medium and low temperature thermoelectric power generation by virtue of their advantages of non-toxicity, non-polluting, low price and abundant content. Although the thermoelectric performance enhancement strategies of Mg₃Sb₂-based materials have been widely studied, there are few reports on their contact layer preparation and power generation device fabrication. Therefore, it is of great significance to prepare n-type Mg₃Sb₂-based materials with high thermoelectric performance and to optimize the interfaces design and fabrication method of the devices. The n-type Mg₃Sb₂-based materials were prepared by planetary ball milling and spark plasma sintering, and the improvement of material performance, the preparation of contact layers and the fabrication of devices were studied. N-type Mg₃Sb₂-based materials with high ZT value were obtained, and a device with high conversion efficiency was fabricated. The main research results are as follows:

The thermoelectric performance of n-type Mg₃Sb₂-based materials was enhanced by the doping strategy of MWCNTs and Cu. A small amount of MWCNTs doping significantly improves the power factor and reduces the thermal conductivity, thereby increasing the ZT value of the samples. The doping of trace Cu elements can effectively improve the low temperature ZT value of the material. Co-doping of Cu and MWCNTs can combine the favorable effects of both on the thermoelectric performance of the samples. The ZT value of the Mg_3.5Sb_1.5Bi_0.45Te_0.05Cu_0.01/ 0.1_wt% CNT co-doped sample is improved in the whole operation temperature range, the ZT peak value of the sample is 1.7 at 749K, and the room temperature ZT value also has about 20% improvement. In addition, the thermoelectric performance of the sample is highly repeatable.

The interfaces of two contact layers of n-type Mg₃Sb₂-based materials were investigated. Under the condition of SPS at 600℃ and 20min, compared with Fe-Co alloy, when 316L stainless steel is used as the contact layer, the sample has a power factor more similar to that of the TE material. The thickness and density of the Fe-Co alloy contact layer are not uniform, and there is obvious element diffusion in the contact layer during sintering. The structure of the 316L stainless steel contact layer is dense and uniform, which can effectively prevent the diffusion of elements during the preparation of the contact layer, and the distribution of elements after annealing has no significant change compared with before annealing. Therefore, when 316L stainless steel is used as the contact layer, the interfaces have good thermal stability.

A power generation device with high conversion efficiency was fabricated. Using n-type Mg₃Sb₂ material and p-type PbTe material, the device containing two pairs of thermoelectric arms was fabricated. When the hot side temperature is 766K and the current is 2.32A, the maximum output power of the device is about 0.5W, and the maximum conversion efficiency is 10.3%.

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