Materials with high zT over a wide temperature range are essential for thermoelectric applications. n-Type Mg Sb -based compounds have been shown to achieve high zT at 700 K, but their performance at low temperatures (<500 K) is compromised due to their highly resistive grain boundaries. Syntheses and optimization processes to mitigate this grain-boundary effect has been limited due to loss of Mg, which hinders a sample's n-type dopability. A Mg-vapor anneal processing step that grows a sample's grain size and preserves its n-type carrier concentration during annealing is demonstrated. The electrical conductivity and mobility of the samples with large grain size follows a phonon-scattering-dominated T trend over a large temperature range, further supporting the conclusion that the temperature-activated mobility in Mg Sb -based materials is caused by resistive grain boundaries. The measured Hall mobility of electrons reaches 170 cm V s in annealed 800 °C sintered Mg Sb Bi Te , the highest ever reported for Mg Sb -based thermoelectric materials. In particular, a sample with grain size >30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric materials used at room temperature (n-type Bi Te ) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale.

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http://dx.doi.org/10.1002/adma.201902337DOI Listing

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