Decoupled charge and heat transport for high-performance Fe₂VAl composite thermoelectrics

Decoupling charge and heat transport is essential for optimizing thermoelectric materials. Strategies to inhibit lattice-driven heat transport, however, also compromise carrier mobility, limiting the performance of most thermoelectrics, including Fe$_2$VAl Heusler compounds. Here, we demonstrate an innovative approach, which bypasses this tradeoff: via liquid-phase sintering, we incorporate the archetypal topological insulator Bi$_{1-x}$Sb$_{x}$ between Fe$_2$V$_{0.95}$Ta$_{0.1}$Al$_{0.95}$ grains. Structural investigations alongside extensive thermoelectric and magneto-transport measurements reveal distinct modifications in the microstructure, and a reduced lattice thermal conductivity and enhanced carrier mobility are simultaneously found. This yields a huge performance boost $-$ far beyond the effective-medium limit $-$ and results in one of the highest figure of merits among both half- and full-Heusler compounds, $z\approx 1.6\times 10^{-3}\,$K$^{-1}$ ($zT\approx 0.5$) at 295 K. Our findings highlight the potential of secondary phases to decouple charge and heat transport and call for more advanced theoretical studies of multiphase composites.