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The rapid enhancement of the thermoelectric (TE) figure‐of‐merit (zT) in the past decade has opened opportunities for developing and transitioning solid state waste heat recovery systems. Here, a segmented TE device architecture is demonstrated in conjunction with heterogeneous material integration that results in high unicouple‐level conversion efficiency of 12% under a temperature difference of 584 K. This breakthrough is the result of success in fabricating bismuth telluride/half‐Heusler segmented TE unicouple modules using a “hot‐to‐cold” fabrication technique that provides significantly reduced electrical and thermal contact resistance. Extensive analytical and finite element modeling is conducted to provide an understanding of the nature of thermal transport and contributions arising from various thermal and physical parameters. Bismuth telluride/half‐Heusler based segmented thermoelectric generators (TEGs) can provide higher practical temperature difference with optimum average zT across the whole operating range. These results will have immediate impact on the design and development of TEGs and in the general design of devices based upon heterostructures that take advantage of gradients in the figure of merit.

The filling fraction limitation (FFL) in n-type CoSb3 skutterudites is far below that of p-type (Fe,Co)­Sb3-based skutterudites, and it is critical to increase FFL for accomplishing high thermoelectric figure of merit (ZT max). Here, a series of Yb x Co4–y Fe y Sb12 alloys with x = 0.25–0.5 and y = 0.1–0.5 were synthesized, which demonstrate a clear increase of the FFL of Yb from ∼0.3 in CoSb3 to 0.5. Ultralow thermal conductivities of 2.0–2.5 W/m·K at 300 K and 1.75 W/m·K at ∼600 K have been achieved, which are the lowest values reported among skutterudite materials and comparable with p-type skutterudites. These ultralow thermal conductivities result from the combination of secondary phase scattering and phonon scattering from dynamic electron exchange between Fe2+ and Co3+. High ZT max values of 1.28 at 740 K and 1.34 at 780 K are obtained, which are among the best values reported in the temperature range of 740–800 K. The temperature at which maximum ZT max appears is shifted below 850 K. These results are highly exciting toward the development of multistage segmented and cascade thermoelectric power generators for in-air operations.

Thermoelectric generators (TEGs) can convert body heat into electricity, thereby providing a continuous power source for wearable and implantable devices. For wearables, the low fill factor (area occupied by legs over the TEG base area) TEG modules are relevant as they provide large thermal gradient across the legs and require less material, which reduces the cost and weight. However, TEGs with a fill factor below 15% suffer from reduced mechanical robustness; consequently, commercial modules are usually fabricated with a fill factor in the range of 25–50%. In this study, TEG modules with a low and high fill factor are demonstrated and their performance is compared in harvesting body heat. Fabricated modules demonstrate ∼80% output power enhancement as compared to commercially available designs, resulting in high power density of up to 35 μW/cm2 in a steady state. This enhanced power is achieved by using two-third less thermoelectric materials in comparison to commercial modules. These results will advance the ongoing development of wearable devices by providing a consistent high specific power density source.

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Thermoelectric generators (TEGs) exploiting the Seebeck effect provide a promising solution for waste heat recovery. Among the large number of thermoelectric (TE) materials, half-Heusler (hH) alloys are leading candidates for medium- to high-temperature power generation applications. However, the fundamental challenge in this field has been inhomogeneous material properties at large wafer diameters, insufficient power output from the modules, and rigid form factors of TE modules. This has restricted the transition of TEGs in practical applications for over three decades. Here, we successfully demonstrate large diameter wafers with uniform TE properties, high-power conformal hH TE modules for high-temperature application, and their direct integration on flue gas platforms, such as cylindrical tubes, to form large area flexible TEGs. This new conformal architecture design provides a breakthrough toward medium-/high-temperature TEGs over the conventional BiTe- and polymer-based flexible TEG design. A variable fill factor and greater flexibility due to the conformal design result in higher device performance as compared to conventional rigid TEG devices. Modules with 72-couple hH legs exhibit a device high-power-density of 3.13 W cm–2 and a total output power of 56.6 W under a temperature difference of 570 °C. These results provide a promising pathway toward widespread utilization of thermoelectric technology into the waste heat recovery application and will have a significant impact on the development of practical thermal to electrical converters.

High temperature waste heat recovery has gained tremendous interest to generate useful electricity while reducing the harmful impact on the environment. Thermoelectric (TE) solid-state materials enable direct conversion of heat into electricity with high efficiency, thereby offering a practical solution for waste heat recovery. Half-Heusler (hH) alloys are the leading TE materials for medium to high temperature applications, as they exhibit a high figure of merit and mechanical strength at temperatures as high as 973 K. Here we investigate the most promising hH alloys represented as MNiSn, MCoSb, and NbFeSb systems (M = Hf, Zr, and Ti) and provide fundamental understanding of their in-air thermal stability at high temperatures under realistic operating conditions required for energy generation. The understanding of oxidation resistance of TE materials is crucial for their practical deployment in extreme environments without vacuum sealing. The n-type MNiSn and p-type NbFeSb compounds are found to exhibit excellent oxidation resistance at a high temperature of 873 K. The oxidation resistance is enhanced through the presence of an intermetallic Ni–Sn layer for MNiSn and Nb–TiO2 double layer for (Nb,Ti)­FeSb. A unicouple thermoelectric generator (TEG) fabricated from thermally stable materials demonstrated consistent performance for more than 150 h at 873 K in air. These results demonstrate the significance of TE materials in waste heat recovery systems.

Oxide thermoelectric materials are nontoxic, chemically and thermally stable in oxidizing environments, cost-effective, and comparatively simpler to synthesize. However, thermoelectric oxides exhibit comparatively lower figure of merit ( ZT ) than that of metallic alloy counterparts. In this study, nanoscale texturing and interface engineering were utilized for enhancing the thermoelectric performance of oxide polycrystalline Ca 3 Co 4 O 9 materials, which were synthesized using conventional sintering and spark plasma sintering (SPS) techniques. Results demonstrated that nanoscale platelets (having layered structure with nanoscale spacing) and metallic inclusions provide effective scattering of phonons, resulting in lower thermal conductivity and higher ZT . Thermoelectric measurement direction was found to have a significant effect on the magnitude of ZT because of the strong anisotropy in the transport properties induced by the layered nanostructure. The peak ZT value for the Ca 2.85 Lu 0.15 Co 3.95 Ga 0.05 O 9 specimen measured along both perpendicular and parallel directions with respect to the SPS pressure axis is found be 0.16 at 630 °C and 0.04 at 580 °C, respectively. The peak ZT of 0.25 at 670 °C was observed for the spark plasma-sintered Ca 2.95 Ag 0.05 Co 4 O 9 sample. The estimated output power of 2.15 W was obtained for the full size model, showing high-temperature thermoelectric applicability of this nanostructured material without significant oxidation.