Enhanced Thermoelectric Performance in Vacancy‐Filling Heuslers due to Kondo‐Like Effect

To improve thermoelectric efficiency, various tactics have been employed with considerable success to decouple intertwined material attributes. However, the integration of magnetism, derived from the unique spin characteristic that other methods cannot replicate, has been comparatively underexplored and presents an ongoing intellectual challenge. A previous research has shown that vacancy‐filling Heuslers offer a highly adaptable framework for modulating thermoelectric properties. Here, it is demonstrated how intrinsic magnetic‐electrical‐thermal coupling can enhance the thermoelectric performance of vacancy‐filling Heusler alloys. The materials, Nb0.75Ti0.25FeCrxSb with 0 ≤ x ≤ 0.1, feature a fraction of magnetic Cr ions that randomly occupy the vacancy sites of the Nb0.75Ti0.25FeSb half‐Heusler matrix. These alloys achieve a remarkable thermoelectric figure of merit (zT) of 1.21 at 973 K, owing to increased Seebeck coefficient and decreased thermal conductivity. The mechanism is primarily due to the introduction of magnetism, which increases the density‐of‐states effective mass (reaching levels up to 15 times that of a free electron's mass) and simultaneously reduces the electronic thermal conductivity. Mass and strain‐field fluctuations further reduce the lattice thermal conductivity. Even higher zT values can potentially be achieved by carefully balancing electron mobility and effective mass. This work underscores the substantial prospects for exploiting magnetic‐electrical‐thermal synergies in cutting‐edge thermoelectric materials. This work demonstrate that intrinsic magnetic‐electrical‐thermal coupling can enhance the thermoelectric performance. The vacancy‐filling Heusler alloy Nb0.75Ti0.25FeCrxSb shows a Kondo‐like effect, which not only increases the effective mass but also reduces the thermal conductivity. As a result, a remarkable thermoelectric figure of merit (zT) of 1.21 is achieved at 973 K in Nb0.75Ti0.25FeCr0.1Sb.