Enhanced Thermoelectric Properties of Pd and Ni Codoped Electronegative Element-Filled Skutterudites

IF 5.4 3区材料科学 Q2 CHEMISTRY, PHYSICAL ACS Applied Energy Materials Pub Date : 2024-10-18 DOI:10.1021/acsaem.4c0235410.1021/acsaem.4c02354

Shun Wan, Qingfeng Song, Xudong Bai, Pengfei Qiu, Qihao Zhang* and Tian-Ran Wei*,

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Abstract

Electronegative element-filled skutterudites have attracted considerable attention due to their use of environmentally friendly elements and their excellent thermoelectric performance. While single-donor doping at Co or Sb sites has been shown to be thermodynamically favorable, the effects of codoping on electronegative element-filled skutterudites remain underexplored. In this study, we investigate the impact of codoping palladium (Pd) and nickel (Ni) at Co sites on the stability of the electronegative element (S) fillers within the voids of CoSb₃. A series of S_zPd_xNi_yCo_4–x–ySb₁₂ compounds were successfully synthesized, and their electrical and thermal transport properties are systematically analyzed. Our results reveal that the Hall carrier concentration, Seebeck coefficient, and Hall mobility of the S_zPd_xNi_yCo_4–x–ySb₁₂ samples lie between those of S-filled and Pd or Ni single-doped counterparts. Additionally, these compounds exhibit reduced lattice thermal conductivities due to the synergistic interaction between the S filler and Pd/Ni codopants. Notably, a peak figure of merit (zT) of 0.89 is achieved for S_0.05Pd_0.2Ni_0.2Co_3.6Sb₁₂ at 850 K.

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增强掺杂钯和镍的负电元素填充沸石的热电性能

负电性元素填充沸石因其使用环保元素和优异的热电性能而备受关注。虽然在钴或锑位点掺杂单供体已被证明在热力学上是有利的，但掺杂对电负性元素填充沸石的影响仍未得到充分探索。在本研究中，我们研究了在 Co 位点掺杂钯（Pd）和镍（Ni）对 CoSb3 空隙中电负性元素（S）填充物稳定性的影响。我们成功合成了一系列 SzPdxNiyCo4-x-ySb12 化合物，并系统分析了它们的电学和热传输特性。我们的研究结果表明，SzPdxNiyCo4-x-ySb12 样品的霍尔载流子浓度、塞贝克系数和霍尔迁移率介于充满 S 的样品和单一掺杂钯或镍的样品之间。此外，由于 S 填充物和 Pd/Ni 共掺物之间的协同作用，这些化合物的晶格热导率有所降低。值得注意的是，在 850 K 下，S0.05Pd0.2Ni0.2Co3.6Sb12 的峰值优越性（zT）达到了 0.89。

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来源期刊

ACS Applied Energy Materials Materials Science-Materials Chemistry

CiteScore

10.30

自引率

6.20%

发文量

1368

期刊介绍： ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.