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Thermoelectric generators held great promise through energy harvesting from waste heat. Their practical application, however, is greatly constrained by poor raw material utilization and tedious processing in fabricating desired shapes. Herein, a state‐of‐the‐art process is reported for 3D printing the half‐Heusler (Nb0.88Hf0.12FeSb) thermoelectric material using laser powder bed fusion (LPBF). The multi‐dimensional intra‐ and inter‐granular defects created by this process greatly suppress thermal conductivity by providing numerous phonon scattering centers. The resulting LPBF‐fabricated half‐Heusler exhibits a high figure of merit ≈1.2 at 923 K and a single‐leg maximum efficiency of ≈3.3% at a temperature difference (ΔT) of 371 K. Hafnium oxide nanoparticles generated during LPBF effectively prevent crack propagation, ensuring competent mechanical performance and reliable thermoelectric output. The findings highlight the significant potential of LPBF in driving the next industrial revolution of highly efficient and customizable thermoelectric materials. [ABSTRACT FROM AUTHOR]

Thermoelectric generators held great promise through energy harvesting from waste heat. Their practical application, however, is greatly constrained by poor raw material utilization and tedious processing in fabricating desired shapes. Herein, a state-of-the-art process is reported for 3D printing the half-Heusler (Nb 0.88 Hf 0.12 FeSb) thermoelectric material using laser powder bed fusion (LPBF). The multi-dimensional intra- and inter-granular defects created by this process greatly suppress thermal conductivity by providing numerous phonon scattering centers. The resulting LPBF-fabricated half-Heusler exhibits a high figure of merit ≈1.2 at 923 K and a single-leg maximum efficiency of ≈3.3% at a temperature difference (ΔT) of 371 K. Hafnium oxide nanoparticles generated during LPBF effectively prevent crack propagation, ensuring competent mechanical performance and reliable thermoelectric output. The findings highlight the significant potential of LPBF in driving the next industrial revolution of highly efficient and customizable thermoelectric materials., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Thermoelectric (TE) energy conversion technology provides a promising way to improve the efficiency of fossil energy by generating electricity from low-grade waste heat. With regard to these applications, thermoelectric generators (TEGs) should be designed from system integration perspectives to simultaneously improve heat transfer efficiency and system simplification as well as the robust mechanical properties. However, typical TEGs fabricated by conventional methods barely accomplish such requirements. Herein, high-quality TEGs were assembled by combining the well-flowable spherical bismuth telluride (BT) powdered precursors and selective laser melting (SLM) technology. By optimizing the electronic and phonon transport properties through defect engineering driven by 3D printing, a high figure of merit was accomplished for 1.27 (p-type) and 1.13 (n-type) in BT. This achievement is primarily attributed to the nonequilibrium solidification mechanism, which leads to the formation of multiscale defects during the 3D printing process. The introduction of these multiscale defects enables the effective scattering of wide frequency phonons, leading to a substantial reduction in lattice thermal conductivity. Meanwhile, robust mechanical properties were obtained in the printed p-type/n-type BT TE materials parallel to the building direction (BD) with a compressive strength reaching 257/250 MPa by employing the fine grain structure and the high density of nanotwins introduced during the SLM process. A well shape-controllable and high-performance TEG was designed using 3D-printed BT half-rings, and an output power of 134 mW was achieved at a temperature gradient of 38.9 °C. Our study opens a new route for the great potential of TE materials based on standard commercial SLM 3D printing technology for low-grade waste heat emitted from structures with heterogeneous shapes.

High-energy-conversion Bi 2 Te 3 -based thermoelectric generators (TEGs) are needed to ensure that the assembled material has a high value of average figure of merit ( ZT ave ). However, the inferior ZT ave of the n-type leg severely restricts the large-scale applications of Bi 2 Te 3 -based TEGs. In this study, we achieved and reported a high peak ZT (1.33) of three-dimensional (3D)-printing n-type Bi 2 Te 2.7 Se 0.3 . In addition, a superior ZT ave of 1.23 at a temperature ranging from 300 to 500 K was achieved. The high value of ZT ave was obtained by synergistically optimizing the electronic- and phonon-transport properties using the 3D-printing-driven defect engineering. The nonequilibrium solidification mechanism facilitated the multiscale defects formed during the 3D-printed process. Among the defects formed, the nanotwins triggered the energy-filtering effect, thus enhancing the Seebeck coefficient at a temperature range of 300-500 K. The effective scattering of wide-frequency phonons by multiscale defects reduced the lattice thermal conductivity close to the theoretical minimum of ∼0.35 W m -1 k -1 . Given the advantages of 3D printing in freeform device shapes, we assembled and measured bionic honeycomb-shaped single-leg TEGs, exhibiting a record-high energy conversion efficiency (10.2%). This work demonstrates the great potential of defect engineering driven by selective laser melting 3D-printing technology for the rational design of advanced n-type Bi 2 Te 2.7 Se 0.3 thermoelectric material.