Excellent thermomagnetic power generation for harvesting waste heat viaa second-order ferromagnetic transitionElectronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d3mh02225k

Thermomagnetic generation (TMG), a promising technology to convert low-grade waste heat to electricity, utilizes high performance TMG materials. However, the drawbacks of large hysteresis, poor mechanical properties and inadequate service life hinder the practical applications. For the first time, we evaluated the effect of different phase transitions on the TMG performance by systematically comparing the TMG performance of three typical Heusler alloys with similar composition but different phase transitions. Ni2Mn1.4In0.6exhibits second-order magnetic transition (SOMT) from the ferromagnetic (FM) to paramagnetic (PM) state around TC= 316 K without thermal hysteresis. It presents highly comprehensive TMG performance, which is not only better than those of other two Heusler alloys with different phase transitions, but also better than those of most typical TMG materials. The maximum power density (1752.3 mW m−3), cost index (2.78 μW per €), and power generation index PGI (8.91 × 10−4) of Ni2Mn1.4In0.6are 1–5, 1–4, and 1–7 orders of magnitude higher than those of most typical reported materials, respectively. In addition, Ni2Mn1.4In0.6with SOMT also shows some advantages that first-order magnetic transition (FOMT) materials do not have, such as zero hysteresis and a long-term service life. In contrast to the short lifetime of a few minutes for the materials with FOMT, Ni2Mn1.4In0.6with SOMT can serve for one month or even longer with excellent cycling stability. Consequently, we conclude that the SOMT Ni2Mn1.4In0.6Heusler alloy with good TMG performance as well as zero hysteresis and long service life can be a better candidate than FOMT materials for practical applications of TMG.