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Nb‐Mediated Grain Growth and Grain‐Boundary Engineering in Mg 3 Sb 2 ‐Based Thermoelectric Materials
Author(s) -
Luo Ting,
Kuo Jimmy J.,
Griffith Kent J.,
Imasato Kazuki,
CojocaruMirédin Oana,
Wuttig Matthias,
Gault Baptiste,
Yu Yuan,
Snyder G. Jeffrey
Publication year - 2021
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.202100258
Subject(s) - materials science , grain boundary , thermoelectric effect , scattering , electrical resistivity and conductivity , crystallite , impurity , carrier scattering , analytical chemistry (journal) , ionized impurity scattering , condensed matter physics , grain growth , alloy , grain size , metallurgy , microstructure , optoelectronics , doping , optics , thermodynamics , physics , electrical engineering , chemistry , organic chemistry , chromatography , engineering
The poor carrier mobility of polycrystalline Mg 3 Sb 2 at low temperatures strongly degrades the thermoelectric performance. Ionized impurities are initially thought to dominate charge carrier scattering at low temperatures. Accordingly, the increased electrical conductivity by replacing Mg with metals such as Nb is also attributed to reduced ionized impurity scattering. Recent experimental and theoretical studies challenge this view and favor the grain boundary (GB) scattering mechanism. A reduction of GB scattering improves the low‐temperature performance of Mg 3 (Sb, Bi) 2 alloys. However, it is still elusive how these metal additions reduce the GB resistivity. In this study, Nb‐free and Nb‐added Mg 3 Sb 2 are studied through diffraction, X‐ray absorption spectroscopy, solid‐state nuclear magnetic resonance spectroscopy, and atom probe tomography. It is shown that Nb does not enter the Mg 3 Sb 2 matrix and remains in the metallic state. Besides, Nb diffuses along the GB forming a wetting layer, which modifies the interfacial energy and accelerates grain growth. The GB resistivity appears to be reduced by Nb‐enrichment, as evidenced by modeling the electrical transport properties. This study not only confirms the GB scattering in Mg 3 Sb 2 but also reveals the hitherto hidden role of metallic additives on enhancing grain growth and reducing the GB resistivity.