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Impurity Removal Leading to High-Performance CoSb3-Based Skutterudites with Synergistic Carrier Concentration Optimization and Thermal Conductivity Reduction
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-11-04 , DOI: 10.1021/acsami.1c16622
Xu-Guang Li 1 , Wei-Di Liu 2 , Shuang-Ming Li 1 , Dou Li 1 , Hong Zhong 1 , Zhi-Gang Chen 2, 3
Affiliation  

Thermoelectric properties of CoSb3-based skutterudites are greatly determined by the removal of detrimental impurities, such as (Fe/Co)Sb2, (Fe/Co)Sb, and Sb. In this study, we use a facile temperature gradient zone melting (TGZM) method to synthesize high-performance CoSb3-based skutterudites by impurity removal. After removing metallic or semimetallic impurities (Fe/Co)Sb, (Fe/Co)Sb2, and Sb, the carrier concentration of TGZM-Ce0.75Fe3CoSb12 can be reduced to 1.21 × 1020 cm–3 and the electronic thermal conductivity dramatically reduced to 0.7 W m–1 K–1 at 693 K. Additionally, removing these impurities also effectively reduces the lattice thermal conductivity from 7.2 W m–1 K–1 of cast-Ce0.75Fe3CoSb12 to 1.02 W m–1 K–1 of TGZM-Ce0.75Fe3CoSb12 at 693 K. As a consequence, TGZM-Ce0.75Fe3CoSb12 approaches a high power factor of 11.7 μW cm–1 K–2 and low thermal conductivity of 1.72 W m–1 K–1 at 693 K, leading to a peak zT of 0.48 at 693 K, which is 10 times higher than that of cast-Ce0.75Fe3CoSb12. This study indicates that our facile TGZM method can effectively synthesize high-performance CoSb3-based skutterudites by impurity removal and set up a solid foundation for further development.

中文翻译:

通过协同优化载流子浓度和降低热导率,去除杂质导致高性能 CoSb3 基方钴矿

CoSb 3基方钴矿的热电特性很大程度上取决于有害杂质的去除,例如(Fe/Co)Sb 2、(Fe/Co)Sb 和Sb。在本研究中,我们使用简便的温度梯度区熔化 (TGZM) 方法通过去除杂质来合成高性能 CoSb 3基方钴矿。去除金属或半金属杂质(Fe/Co)Sb、(Fe/Co)Sb 2和Sb后,TGZM-Ce 0.75 Fe 3 CoSb 12的载流子浓度可降低至1.21 × 10 20 cm –3和电子热导率显着降低至 0.7 W m –1 K –1在 693 K。此外,去除这些杂质还有效地将晶格热导率从 7.2 W m –1 K –1的 Cast-Ce 0.75 Fe 3 CoSb 12 降低到 1.02 W m –1 K –1的 TGZM-Ce 0.75 Fe 3的CoSb 12在693 K.因此,温度梯度区熔铈0.75的Fe 3的CoSb 12接近11.7μWcm的高功率因数-1 ķ -2和1.72女男低热导率-1 ķ -1在693 K,导致达到峰值zT在 693 K 时为 0.48,是铸造 Ce 0.75 Fe 3 CoSb 12 的10 倍。该研究表明,我们简便的 TGZM 方法可以通过去除杂质有效地合成高性能 CoSb 3基方钴矿,为进一步开发奠定了坚实的基础。
更新日期:2021-11-17
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