Grain Boundary Complexions Enable a Simultaneous Optimization of Electron and Phonon Transport Leading to High-Performance GeTe Thermoelectric Devices

Chaohua Zhang; Gan Yan; Yibo WangXuelian WuLipeng HuFusheng LiuWeiqin AoOana Cojocaru-MiredinMatthias WuttigG. Jeffrey SnyderYuan Yu

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Grain Boundary Complexions Enable a Simultaneous Optimization of Electron and Phonon Transport Leading to High-Performance GeTe Thermoelectric Devices

机译：Grain Boundary Complexions Enable a Simultaneous Optimization of Electron and Phonon Transport Leading to High-Performance GeTe Thermoelectric Devices

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Grain boundaries (GBs) form ubiquitous microstructures in polycrystalline materials which play a significant role in tuning the thermoelectric figure of merit (ZT). However, it is still unknown which types of GB features are beneficial for thermoelectrics due to the challenge of correlating complex GB microstructures with transport properties. Here, it is demonstrated that GB complexions formed by Ga segregation in GeTe-based alloys can optimize electron and phonon transport simultaneously. The Ga-rich complexions increase the power factor by reducing the GB resistivity with slightly improved Seebeck coefficients. Simultaneously, they lower the lattice thermal conductivity by strengthening the phonon scattering. In contrast, Ga_2Te_3 precipitates at GBs act as barriers to scatter both phonons and electrons and are thus unable to improve ZT. Tailoring GBs combined with the beneficial alloying effects of Sb and Pb enables a peak ZT of ≈2.1 at 773 K and an average ZT of 1.3 within 300–723 K for Ge_(0.78)Ga_(0.01)Pb_(0.1)Sb_(0.07)Te. The corresponding thermoelectric device fabricated using 18-pair p-n legs shows a power density of 1.29 W cm~(?2) at a temperature difference of 476 K. This work indicates that GB complexions can be a facile way to optimize electron and phonon transport, further advancing thermoelectric materials.

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《Advanced energy materials》 |2023年第3期|2203361.1-2203361.12|共12页
作者
Chaohua Zhang; Gan Yan; Yibo WangXuelian WuLipeng HuFusheng LiuWeiqin AoOana Cojocaru-MiredinMatthias WuttigG. Jeffrey SnyderYuan Yu;
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Institute of Physics (IA) RWTH Aachen University Sommerfeldstrasse 14 52074, Aachen, Germany;

Institute of Physics (IA) RWTH Aachen University Sommerfeldstrasse 14 52074, Aachen, Germany,Peter Gruenberg Institute—JARA-Institute Energy-Efficient Information Technology (PGI-10) Forschungszentrum Juelich GmbH 52428, Juelich, Germany;

Department of Materials Science and Engineering Northwestern University Evanston, IL 60208, USACollege of Materials Science and Engineering Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advanced Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials Institut;

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atom probe tomography; density functional theory; grain boundary complexion; metavalent bonding; thermoelectric devices;

Grain Boundary Complexions Enable a Simultaneous Optimization of Electron and Phonon Transport Leading to High-Performance GeTe Thermoelectric Devices

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