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Science-driven design of future thermoelectric materials requires a deepunderstanding of the fundamental relationships between microstructure andtransport properties. Grain boundaries in polycrystalline materials influencethe thermoelectric performance through the scattering of phonons or thetrapping of electrons due to space-charge effects. Yet, the current lack ofcareful investigations on grain boundary-associated features hinders furtheroptimization of properties. Here, we study n-type NbCo1-xPtxSn half-Heusleralloys, which were synthesized by ball milling and spark plasma sintering(SPS). Post-SPS annealing was performed on one sample, leading to improvedlow-temperature electrical conductivity. The microstructure of both samples wasexamined by electron microscopy and atom probe tomography. The grain sizeincreases from ~230 nm to ~2.38 {\mu}m upon annealing. Pt is found withingrains and at grain boundaries, where it locally reduces the resistivity, asassessed by in situ four-point-probe electrical conductivity measurement. Ourwork showcases the correlation between microstructure and electricalconductivity, providing opportunities for future microstructural optimizationby tuning the chemical composition at grain boundaries.

Dopant-segregation to grain boundaries controls electrical conductivity of n-type NbCo(Pt)Sn half-Heusler alloy mediating thermoelectric performance