Decoupled charge and heat transport in Fe2VAl composite thermoelectrics with topological-insulating grain boundary networks

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 Fe2VAl Heusler compounds. Here, we demonstrate an innovative approach, which bypasses this tradeoff: via liquid-phase sintering, we incorporate the archetypal topological insulator Bi1−xSbx between Fe2V0.95Ta0.1Al0.95 grains. Structural investigations alongside extensive thermoelectric and magneto-transport measurements reveal distinct modifications in the microstructure, a reduced lattice thermal conductivity and a simultaneously enhanced carrier mobility arising from topologically protected charge transport along the grain boundaries. This yields a huge performance boost, resulting in one of the highest figure of merits among both half- and full-Heusler compounds, z ≈ 1.6 × 10−3 K−1 (zT ≈ 0.5) at 295 K. Our findings highlight the potential of topological-insulating secondary phases to decouple charge and heat transport and call for more advanced theoretical studies of multiphase composites.