High figure-of-merit in the heavy-fermion UN2 system for radioisotope thermoelectric applications

Abstract

Abstract The design of uranium-based thermoelectric (TE) materials presents a novel and intriguing strategy for directly converting nuclear heat into electrical power. Using high-level first-principles approach combined with accurate solution of Boltzmann transport equation, we demonstrate that a giant n-type power factor of 13.8 mW m−1 K−2 and a peak ZT value of 2.2 can be realized in the heavy-fermion UN2 compound at 700 K. Such promising TE performance arises from the large degeneracy (N v = 14) of heavy conduction band coupled with weak electron–phonon interactions, which is in principle governed by the strong Coulomb correlation among the partially filled U-5f electrons in the face-centered cubic structure. Collectively, our theoretical work suggests that the energetic UN2 could serve as both excellent heat source and efficient power convertor, which also uncovers an underexplored area for TE research.