Highly Distorted Grain Boundary with an Enhanced Carrier/Phonon Segregation Effect Facilitates High-Performance...

Grain boundary plays an important role in determining the phonon/carrier transport behaviors of thermoelectric (TE) materials, especially for the polycrystalline materials with the average grain size in nanoscale dimensions. Adjusting the grain size and boundaries of TE materials is considered as an effective approach to decouple TE parameters and thereby synergistically optimize the TE performance. Here, the highly distorted grain boundary with an enhanced carrier/phonon segregation effect is introduced to the commercial n-type Bi₂Te_2.7Se_0.3 matrix. The existence of highly distorted grain boundaries can not only enhance the interfacial Seebeck coefficient without significant detriment to the electrical conductivity but also increase the interfacial thermal resistance of grain boundaries, leading to the synergistic reduction of the thermal conductivity. As a result, a peak figure of merit zT_max ≈ 1.22@425 K and an average zT_avg ≈ 1.1(300-500 K) are obtained, which are about 55 and 57% higher than the corresponding values of the commercial Bi₂Te_2.7Se_0.3 matrix, respectively. This work represents a new avenue for improving the commercial Bi₂Te_2.7Se_0.3 TE material, which could further promote the development of the TE technology.