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Abstract Highly resistive grain boundaries significantly reduce the electrical conductivity that compromises the thermoelectric figure‐of‐meritzTin n‐type polycrystalline Mg3Sb2. In this work, discovered is a Mg deficiency near grain boundaries using atom‐probe tomography. Approximately 5 at% of Mg deficiency is observed uniformly in a 10 nm region along the grain boundary without any evidence of a stable secondary or impurity phase. The off‐stoichiometry can prevent n‐type dopants from providing electrons, lowering the local carrier concentration near the grain boundary and thus the local conductivity. This observation explains how nanometer scale compositional variations can dramatically determine thermoelectriczT, and provides concrete strategies to reduce grain‐boundary resistance and increasezTin Mg3Sb2‐based materials.
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Grain Boundary Engineering Nanostructured SrTiO 3 for Thermoelectric Applications
Abstract Nanostructuring to reduce thermal conductivity is among the most promising strategies for designing next‐generation, high‐performance thermoelectric materials. In practice, electrical grain boundary resistance can overwhelm the thermal conductivity reduction induced by nanostructuring, which results in worse overall performance. Since a large body of work has characterized the transport of both polycrystalline ceramics and single crystals of SrTiO3, it is an ideal material system for conducting a case study of electrical grain boundary resistance. An effective mass model is used to characterize the transport signatures of electrical grain boundary resistance and evaluate thermodynamic design principles for controlling that resistance. Treating the grain boundary as a secondary phase to the bulk crystallites explains the transport phenomena. Considering that the interface can be engineered by controlling oxygen partial pressure, temperature, and the addition of extrinsic elements into the grain boundary phase, the outlook for SrTiO3as a nanostructured thermoelectric is promising, and thezTcould be greater than 0.5 at room temperature.
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- PAR ID:
- 10460166
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials Interfaces
- Volume:
- 6
- Issue:
- 15
- ISSN:
- 2196-7350
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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