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Ultralow Thermal Conductivity, Enhanced Mechanical Stability, and High Thermoelectric Performance in (GeTe)1–2x(SnSe)x(SnS)x
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-11-20 , DOI: 10.1021/jacs.0c11015 Paribesh Acharyya 1 , Subhajit Roychowdhury 1 , Manisha Samanta 1 , Kanishka Biswas 1, 2
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-11-20 , DOI: 10.1021/jacs.0c11015 Paribesh Acharyya 1 , Subhajit Roychowdhury 1 , Manisha Samanta 1 , Kanishka Biswas 1, 2
Affiliation
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Thermoelectric (TE) energy conversion demands high performance crystalline inorganic solids that exhibit ultralow thermal conductivity, high mechanical stability, and good TE device properties. Pb-free germanium telluride (GeTe)-based material has recently attracted significant attention in TE power generation in mid temperatures, but pristine GeTe possesses significantly higher lattice thermal conductivity (κlatt) compared to that of its theoretical minimum (κmin) of ∼0.3 W/mK. Herein, we have demonstrated the reduction of κlatt of (GeTe)1-2x(SnSe)x(SnS)x very near to its κmin. The (GeTe)1-2x(SnSe)x(SnS)x system behaves as a coexistence of point-defect rich solid solution and phase separation. Initially, the addition of equimolar SnSe and SnS in the GeTe reduces the κlatt by effective phonon scattering because of the excess point defects and rich microstructures. In the second step, introduction of Sb-doping leads to additional phonon scattering centers and optimizes the p-type carrier concentration. Notably, 10 mol % Sb-doped (GeTe)0.95(SnSe)0.025(SnS)0.025 exhibits ultralow κlatt of ∼0.30 W/mK at 300 K. Subsequently, 10 mol % Sb-doped (GeTe)0.95(SnSe)0.025(SnS)0.025 exhibits a high TE figure of merit (zT) of ∼1.9 at 710 K. The high-performance sample exhibits a Vickers microhardness (mechanical stability) value of ∼194 HV that is significantly higher compared to the pristine GeTe and other state-of-the-art thermoelectric materials. Further, we have achieved a high output power, ∼150 mW for the temperature difference of 462 K, in single leg TE device based on 10 mol % Sb-doped (GeTe)0.95(SnSe)0.025(SnS)0.025.
中文翻译：
(GeTe)1–2x(SnSe)x(SnS)x 具有超低导热率、增强的机械稳定性和高热电性能
热电 (TE) 能量转换需要高性能结晶无机固体，这些固体必须具有超低导热率、高机械稳定性和良好的 TE 器件性能。无铅碲化锗 (GeTe) 基材料最近在中温 TE 发电领域引起了广泛关注，但与理论最小值 (κmin) ∼0.3 W 相比，原始 GeTe 具有明显更高的晶格热导率 (κlatt) /mK。在此，我们证明了 (GeTe)1-2x(SnSe)x(SnS)x 的 κlatt 降低非常接近其 κmin。 (GeTe)1-2x(SnSe)x(SnS)x 体系表现为富含点缺陷的固溶体和相分离的共存。最初，由于过量的点缺陷和丰富的微观结构，在GeTe中添加等摩尔的SnSe和SnS通过有效的声子散射降低了κlatt。第二步，引入 Sb 掺杂会产生额外的声子散射中心并优化 p 型载流子浓度。值得注意的是，10 mol % Sb 掺杂 (GeTe)0.95(SnSe)0.025(SnS)0.025 在 300 K 下表现出超低 κlatt，约为 0.30 W/mK。随后，10 mol % Sb 掺杂 (GeTe)0.95(SnSe)0.025( SnS)0.025 在 710 K 时表现出 ∼1.9 的高 TE 品质因数 (zT)。高性能样品的维氏显微硬度（机械稳定性）值为 ∼194 HV，与原始 GeTe 和其他状态相比显着更高最先进的热电材料。此外，我们在基于 10 mol% Sb 掺杂 (GeTe)0.95(SnSe)0.025(SnS)0.025 的单臂 TE 器件中实现了高输出功率，在 462 K 的温差下达到约 150 mW。
更新日期：2020-11-20
中文翻译：
(GeTe)1–2x(SnSe)x(SnS)x 具有超低导热率、增强的机械稳定性和高热电性能
热电 (TE) 能量转换需要高性能结晶无机固体，这些固体必须具有超低导热率、高机械稳定性和良好的 TE 器件性能。无铅碲化锗 (GeTe) 基材料最近在中温 TE 发电领域引起了广泛关注，但与理论最小值 (κmin) ∼0.3 W 相比，原始 GeTe 具有明显更高的晶格热导率 (κlatt) /mK。在此，我们证明了 (GeTe)1-2x(SnSe)x(SnS)x 的 κlatt 降低非常接近其 κmin。 (GeTe)1-2x(SnSe)x(SnS)x 体系表现为富含点缺陷的固溶体和相分离的共存。最初，由于过量的点缺陷和丰富的微观结构，在GeTe中添加等摩尔的SnSe和SnS通过有效的声子散射降低了κlatt。第二步，引入 Sb 掺杂会产生额外的声子散射中心并优化 p 型载流子浓度。值得注意的是，10 mol % Sb 掺杂 (GeTe)0.95(SnSe)0.025(SnS)0.025 在 300 K 下表现出超低 κlatt，约为 0.30 W/mK。随后，10 mol % Sb 掺杂 (GeTe)0.95(SnSe)0.025( SnS)0.025 在 710 K 时表现出 ∼1.9 的高 TE 品质因数 (zT)。高性能样品的维氏显微硬度（机械稳定性）值为 ∼194 HV，与原始 GeTe 和其他状态相比显着更高最先进的热电材料。此外，我们在基于 10 mol% Sb 掺杂 (GeTe)0.95(SnSe)0.025(SnS)0.025 的单臂 TE 器件中实现了高输出功率，在 462 K 的温差下达到约 150 mW。
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