Thermoelectric generators (TEGs) are an excellent candidate for powering wearable electronics and the “Internet of Things,” due to their capability of directly converting heat to electrical energy. Here, we report a high-performance wearable TEG with superior stretchability, self-healability, recyclability, and Lego-like reconfigurability, by combining modular thermoelectric chips, dynamic covalent polyimine, and flowable liquid-metal electrical wiring in a mechanical architecture design of “soft motherboard-rigid plugin modules.” A record-high open-circuit voltage among flexible TEGs is achieved, reaching 1 V/cm² at a temperature difference of 95 K. Furthermore, this TEG is integrated with a wavelength-selective metamaterial film on the cold side, leading to greatly improved device performance under solar irradiation, which is critically important for wearable energy harvesting during outdoor activities. The optimal properties and design concepts of TEGs reported here can pave the way for delivering the next-generation high-performance, adaptable, customizable, durable, economical, and eco-friendly energy-harvesting devices with wide applications.

Two-dimensional (2D) semiconductor is a potential candidate for thermoelectric materials due to its high Seebeck coefficient. However, its high lattice thermal conductivity limits its applications in the field of thermoelectric materials. Here, we constructed an unsymmetrical 2D Janus semiconductor XMoSiN₂(X = S, Se, Te) based on to significantly reduce the lattice thermal conductivity to only one-sixth that of at 300 K. We found that XMoSiN₂ had an ultra-high carrier mobility up to 4640 cm²V⁻¹s⁻¹ leading to a metal-like electrical conductivity. Meanwhile, XMoSiN₂ reserved the high Seebeck coefficient of . The lower lattice thermal conductivity and metal-like electrical conductivity resulted in excellent thermoelectric performance. possessed a record-high ZT value of 3.57 at 900 K. We believed that other materials with a similar structure to XMoSiN₂ can also be potential candidates for high-performance thermoelectric materials. Our work provides valuable insights into designing novel high-performance thermoelectric materials.

Two-dimensional (2D) group IV metal chalcogenides are potential candidates for thermoelectric (TE) applications due to their unique structural properties. In this paper, we predicted a 2D monolayer group IV metal chalcogenide semiconductor $\gamma$-PbSn₂ (X = S, Se, Te), and first-principles calculations and Boltzmann transport theory were used to study the thermoelectric performance. We found that $\gamma$-PbSnX₂ had an ultra-high carrier mobility of up to 4.04 × 10³ cm² V⁻¹ s⁻¹, which produced metal-like electrical conductivity. Moreover, $\gamma$-PbSn₂ not only has a very high Seebeck coefficient, which leads to a high power factor, but also shows an intrinsically low lattice thermal conductivity of 6–8 W/mK at room temperature. The lower lattice thermal conductivity and high power factors resulted in excellent thermoelectric performance. The $ZT$ values of $\gamma$-PbSnS₂ and $\gamma$-PbSnSe₂ were as high as 2.65 and 2.96 at 900 K, respectively. The result suggests that the $\gamma$-PbSnX₂ monolayer is a better candidates for excellent thermoelectric performance.

Flexible thermoelectric materials have drawn significant attention from researchers due to their potential applications in wearable electronics and the Internet of Things. Despite many reports on these materials, it remains a significant challenge to develop cost-effective methods for large-scale, patterned fabrication of materials that exhibit both excellent thermoelectric performance and remarkable flexibility. In this study, we have developed an Ag₂Se-based ink with excellent printability that can be used to fabricate flexible thermoelectric films by screen printing and low-temperature sintering. The printed films exhibit a Seebeck coefficient of −161 μV/K and a power factor of 3250.9 μW/m·K² at 400 K. Moreover, the films demonstrate remarkable flexibility, showing minimal changes in resistance after being bent 5000 times at a radius of 5 mm. Overall, this research offers a new opportunity for the large-scale patterned production of flexible thermoelectric films.

The interface between high-performance thermoelectric materials and electrodes critically governs the conversion efficiency and long-term reliability of thermoelectric generators under high-temperature operation. Here, we propose Al_xCoCrFeNi high-entropy alloys (HEA) as barrier layers to bond Cu-W electrodes with p-type skutterudite (p-SKD) thermoelectric materials. The HEA/p-SKD interface exhibited excellent chemical bonding with a stable and controllable reaction layer, forming a dense, defect-free (Fe,Ni,Co,Cr)Sb phase (thickness of ~2.5 μm) at the skutterudites side. The interfacial resistivity achieved a low value of 0.26 μΩ·cm² and remained at 7.15 μΩ·cm² after aging at 773 K for 16 days. Moreover, the interface demonstrated remarkable mechanical stability, with an initial shear strength of 88 MPa. After long-term aging for 16 days at 773 K, the shear strength retained 74 MPa (only 16% degradation), ranking among the highest reported for thermoelectric materials/metal joints. Remarkably, the joint maintained a shear strength of 29 MPa even after 100 continuous thermal cycles (623–773 K), highlighting its outstanding thermo-mechanical stability. These results validate the Al_xCoCrFeNi high-entropy alloys as an ideal interfacial material for thermoelectric generators, enabling simultaneous optimization of electrical and mechanical performance in harsh environments.

Two-dimensional (2D) of transition metal dichalcogenides (TMDCs) are potential candidates for thermoelectric (TE) applications due to their unique structural properties. In this paper, we constructed an 2D monolayer TMDCs semiconductor γ-PbSn2(X=S, Se, Te) and first-principles calculations and Boltzmann transport theory are used to study the thermoelectric performance. We found that γ-PbSnX2 had an ultra-high carrier mobility up to 4.04×103 cm2V−1s−1 leading to a metal-like electrical conductivity. Meanwhile, γ-PbSnX2 both have high Seebeck coefficients, resulting in high power-factors, and also shows intrinsic low lattice thermal conductivity of 6-8 W/mK at room temperature. The lower lattice thermal conductivity and high power-factors resulted in excellent thermoelectric performance. The high ZT values of γ-PbSnS2 and γ-PbSnSe2 were as high as 2.65 and 2.96 at 900 K, respectively. The result suggests that the monolayer γ-PbSnX2 are better candidates for excellent thermoelectric performance.