Precursor-Led Grain Boundary Engineering for Superior Thermoelectric Performance in Niobium Strontium Titanate

前驱体引导的晶界工程实现钛酸铌锶的卓越热电性能

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作者:Yibing Zhu, Feridoon Azough, Xiaodong Liu, Xiangli Zhong, Minghao Zhao, Kalliope Margaronis, Sohini Kar-Narayan, Ian Kinloch, David J Lewis, Robert Freer

Abstract

We present a novel method to significantly enhance the thermoelectric performance of ceramics in the model system SrTi0.85Nb0.15O3 through the use of the precursor ammonium tetrathiomolybdate (0.5-2% w/w additions). After sintering the precursor-infused green body at 1700 K for 24 h in 5% H2/Ar, single-crystal-like electron transport behavior developed with electrical conductivity reaching ∼3000 S/cm at ∼300 K, almost a magnitude higher than that in the control sample. During processing, the precursor transformed into MoS2, then into MoOx, and finally into Mo particles. This limited grain growth promoted secondary phase generation but importantly helped to reduce the grain boundary barriers. Samples prepared with additions of the precursor exhibited vastly increased electrical conductivity, without significant impact on Seebeck coefficients giving rise to high power factor values of 1760 μW/mK2 at ∼300 K and a maximum thermoelectric figure-of-merit zT of 0.24 at 823 K. This processing strategy provides a simple method to achieve high charge mobility in polycrystalline titanate and related materials and with the potential to create "phonon-glass-electron-crystal" oxide thermoelectric materials.

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