Near‐Room‐Temperature Thermoelectric Performance Enhancement Via Phonon Spectra Mismatch in Mg3(Sb, Bi)2‐Based Material by Incorporating Multi‐Walled Carbon Nanotubes

Abstract

AbstractAlthough a high figure of merit (zT) over a wide range of temperatures has been shown in n‐type Zintl Mg3(Sb, Bi)2, further improvement of its near‐room‐temperature performance is still required to promote its application in next‐generation thermoelectric coolers and power generators. Here, a novel strategy of phonon spectra mismatch for enhancing the thermoelectric performance of Mg3(Sb, Bi)2 is reported by incorporating multi‐walled carbon nanotubes (MWCNT). The introduction of very small amounts of MWCNT generates a large interfacial thermal resistance and thus significantly reduces the lattice thermal conductivity of the resulting composites, while maintaining a high power factor. As a result, a zT of ≈1.5 at 573 K and an average zT of 1.14 between 323 and 573 K can be achieved in the 0.5 wt% MWCNT composite. Moreover, a high conversion efficiency of ≈8.1% under a temperature difference of 283 K is realized in a resulting single‐leg device, making it a promising candidate material for low‐grade heat recovery. This study provides not only a material with a high near‐room‐temperature zT but also a unique insight into the design of high‐performance thermoelectric materials via compositing to exploit the large difference in phonon spectra between the components of the composite.