Jarwal Bhawna, Abbas Suman, Chou Ta-Lei, Vailyaveettil Suneesh M, Kumar Ashutosh, Quadir Shaham, Ho Thi-Thong, Wong Deniz P, Chen Li-Chyong, Chen Kuei-Hsien
Molecular Science and Technology Program, Taiwan International Graduate Program, Academia Sinica, Taipei 10617, Taiwan.
International Graduate Program of Molecular Science and Technology, National Taiwan University, Taipei 10617, Taiwan.
ACS Appl Mater Interfaces. 2024 Mar 27;16(12):14770-14780. doi: 10.1021/acsami.3c17695. Epub 2024 Mar 15.
Metal-semiconductor nanocomposites have emerged as a viable strategy for concurrently tailoring both thermal and electronic transport properties of established thermoelectric materials, ultimately achieving synergistic performance. In this investigation, a series of nanocomposite thin films were synthesized, embedding metallic cobalt telluride (CoTe) nanophase within the nanocrystalline ternary skutterudite (Co(GeSb)Te or CGST) matrix. Our approach harnessed composition fluctuation-induced phase separation and in situ growth during thermal annealing to seamlessly integrate the metallic phase. The distinctive band structures of both materials have developed an ohmic-type contact characteristic at the interface, which raised carrier density considerably yet negligibly affected the mobility counterpart, leading to a substantial improvement in electrical conductivity. The intricate balance in transport properties is further influenced by the metallic CoTe phase's role in diminishing lattice thermal conductivity. The presence of the metallic phase instigates enhanced phonon scattering at the interface boundaries. Consequently, a 2-fold enhancement in the thermoelectric figure of merit (zT ∼ 1.30) is attained with CGST-7 wt. % CoTe nanocomposite film at 655 K compared to that of pristine CGST.
金属-半导体纳米复合材料已成为一种可行的策略,可同时调整既定热电材料的热传输和电子传输特性,最终实现协同性能。在本研究中,合成了一系列纳米复合薄膜,将金属碲化钴(CoTe)纳米相嵌入纳米晶三元方钴矿(Co(GeSb)Te或CGST)基体中。我们的方法利用了热退火过程中成分波动诱导的相分离和原位生长,以无缝集成金属相。两种材料独特的能带结构在界面处形成了欧姆型接触特性,这大大提高了载流子密度,但对迁移率的影响可忽略不计,从而导致电导率大幅提高。传输特性的复杂平衡还受到金属CoTe相在降低晶格热导率方面作用的进一步影响。金属相的存在促使界面边界处的声子散射增强。因此,与原始CGST相比,在655 K时,含7 wt.% CoTe的CGST纳米复合薄膜的热电优值(zT ∼ 1.30)提高了两倍。