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通过特洛伊木马掺杂提高GeSbTe的热电性能以实现高输出功率

Boosting the Thermoelectric Properties of GeSbTe via Trojan Doping for High Output Power.

作者信息

Jiang Yuanxin, Zhang Yu, Wang Xiaoqiang, Chen LeLe, Zhang Jiye, Du Yusong, Xing Weiwei, Zhao Jing-Tai, Li Shuankui, Guo Kai

机构信息

School of Physics and Materials Science, Guangzhou University, Guangzhou 510006, China.

School of Materials Science and Engineering, Shanghai University, Shanghai 200444, China.

出版信息

ACS Appl Mater Interfaces. 2024 Oct 23;16(42):57218-57227. doi: 10.1021/acsami.4c13775. Epub 2024 Oct 13.

Abstract

GeTe stands as a promising lead-free medium-temperature thermoelectric material that has garnered considerable attention in recent years. Suppressing carrier concentration by aliovalent doping in GeTe-based thermoelectrics is the most common optimization strategy due to the intrinsically high Ge vacancy concentration. However, it inevitably results in a significant deterioration of carrier mobility, which limits further improvement of the value. Thus, an effective Trojan doping strategy via CuScTe alloying is utilized to optimize carrier concentration without intensifying charge carrier scattering by increasing the solubility of Sc in the GeTe system. Because of the high doping efficiency of the Trojan doping strategy, optimized hole concentration and high mobility are obtained. Furthermore, CuScTe alloying leads to band convergence in GeTe, increasing the effective mass * in (GeSbTe)(CuScTe) and thus significantly improving the Seebeck coefficient throughout the measured temperature range. Meanwhile, the achievement of the ultralow lattice thermal conductivity ( ∼ 0.34 W m K) at 623 K is attributed to dense point defects with mass/strain-field fluctuations. Ultimately, the (GeSbTe)(CuScTe) sample exhibits a desirable thermoelectric performance of ∼ 1.81 at 623 K and ∼ 1.01 between 300 and 723 K. This study showcases an effective doping strategy for enhancing the thermoelectric properties of GeTe-based materials by decoupling phonon and carrier scattering.

摘要

锗碲是一种很有前景的无铅中温热电材料,近年来受到了广泛关注。由于锗碲基热电材料中本征锗空位浓度较高,通过异价掺杂来抑制载流子浓度是最常见的优化策略。然而,这不可避免地导致载流子迁移率显著下降,限制了优值的进一步提高。因此,采用一种通过铜钪碲合金化的有效特洛伊掺杂策略,在不加剧载流子散射的情况下优化载流子浓度,方法是提高钪在锗碲体系中的溶解度。由于特洛伊掺杂策略的高掺杂效率,获得了优化的空穴浓度和高迁移率。此外,铜钪碲合金化导致锗碲中的能带收敛,增加了(锗锑碲)(铜钪碲)中的有效质量,从而在整个测量温度范围内显著提高了塞贝克系数。同时,在623 K时实现超低晶格热导率(约0.34 W m K)归因于具有质量/应变场波动的密集点缺陷。最终,(锗锑碲)(铜钪碲)样品在623 K时表现出约1.81的理想热电性能,在300至723 K之间约为1.01。本研究展示了一种通过解耦声子和载流子散射来提高锗碲基材料热电性能的有效掺杂策略。

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