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Adv Mater. 2019 Aug;31(35):e1902337. doi: 10.1002/adma.201902337. Epub 2019 Jul 5.

Improvement of Low-Temperature zT in a Mg3 Sb2 -Mg3 Bi2 Solid Solution via Mg-Vapor Annealing.

Author information

1
Materials Science & Engineering (MSE), Northwestern University, Evanston, IL, 60208, USA.

Abstract

Materials with high zT over a wide temperature range are essential for thermoelectric applications. n-Type Mg3 Sb2 -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-3/2 trend over a large temperature range, further supporting the conclusion that the temperature-activated mobility in Mg3 Sb2 -based materials is caused by resistive grain boundaries. The measured Hall mobility of electrons reaches 170 cm2 V-1 s-1 in annealed 800 °C sintered Mg3 + δ Sb1.49 Bi0.5 Te0.01 , the highest ever reported for Mg3 Sb2 -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 Bi2 Te3 ) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale.

KEYWORDS:

Mg3Sb2; grain boundaries; ionized impurities; thermoelectrics; vapor annealing

PMID:
31273874
DOI:
10.1002/adma.201902337

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