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Engineering of Grain Boundaries in Thermoelectric Materials

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The effect of interfaces in solids on the overall charge transport properties has become a topic of growing importance for energy materials such as thermoelectrics. In some polycrystalline thermoelectric materials, the performance near room temperature is significantly limited due to thermally-activated electrical conductivity near room-temperature, which can be attributed to grain boundaries. In this thesis, a combined experimental and theoretical approach is used to explore the grain-boundary effect on charge transport. A simple two-phase model is developed to explain the charge transport across grain boundaries in heavily-doped thermoelectric materials. The thesis will particularly focus on n-type Mg3Sb2 where the thermoelectric performance is improved by engineering the grain boundaries. The relevance to a broader range of materials is shown via re-examining literature data. The synthetic and measurement techniques for characterizing interfacial resistance is transferred to a study of contact resistance in Li-ion energy storage systems. With carefully design measurements the electrical resistance due to solid-solid contacts is shown to be important, especially under the scale relevant for applications.

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