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P-type Fe3CoSb12-based skutterudite thin films are successfully fabricated, exhibiting high thermoelectric performance, stability, and flexibility at medium-to-high temperatures, based on preparing custom target materials and employing advanced pulsed laser deposition techniques to address the bonding challenge between the thin films and high-temperature flexible polyimide substrates. Through the optimization of fabrication processing and nominal doping concentration of Ce, the thin films show a power factor of >100 μW m−1 K−2 and a ZT close to 0.6 at 653 K. After >2000 bending cycle tests at a radius of 4 mm, only a 6 % change in resistivity can be observed. Additionally, the assembled p-type Fe3CoSb12-based flexible device exhibits a power density of 135.7 µW cm−2 under a temperature difference of 100 K with the hot side at 623 K. This work fills a gap in the realization of flexible thermoelectric devices in the medium-to-high-temperature range and holds significant practical application value. The authors fabricate p-type Fe3CoSb12-based skutterudite films exhibiting high thermoelectric performance, stability, and flexibility at medium-to-high temperatures, based on preparing custom target materials and pulsed laser deposition techniques. [ABSTRACT FROM AUTHOR]

As a most promising mid‐temperature thermoelectric material, CoSb3‐based bulk material exhibits an applicable figure‐of‐merit (ZT) of more than one. However, their fabrication is historically time‐consuming due to the long‐time solid‐state phase transitions from CoSb2 to CoSb3. To overcome this challenge, here, a fast one‐step process is developed to fabricate n‐type Yb‐doped CoSb3 with stable ZT of 1.12 at 765 K in <5 h. Experiments confirm Yb promotes peritectic reactions of CoSb + Liquid → CoSb2 and CoSb2 + Liquid → CoSb3, optimizes power factor, and suppresses thermal conductivity. Moreover, the dense grains, induced by the one‐step crystallization, result in outstanding mechanical properties with a Young's modulus of 171.4 GPa and a hardness of 8.8 GPa in the Yb‐doped CoSb3. This study indicates that the fast one‐step fabrication route can effectively promote the practical applications of CoSb3‐based thermoelectrics and provide guidance for thermoelectric fabrication via rational phase design. [ABSTRACT FROM AUTHOR]

Realizing high thermoelectric performance in CoSb3 skutterudite‐based thin films and their devices is historically challenging, especially due to the lack of high‐performing thin‐film‐based device working at medium‐to‐high temperatures. Here, a record‐high ZT of 1.1 is achieved at 683 K in an n‐type Ce0.3Ni1.5Co2.5Sb12 thin film, fabricated from a self‐designed target via advanced pulsed laser deposition. Both experimental and computational results confirm that the Ce‐filling and metal‐featured nanoinclusions such as CeSb contribute to high electrical conductivity, while the Ni‐doping and significantly strengthen the energy filtering effect that occurs at the dense interfaces between the Ce0.3Ni1.5Co2.5Sb12 matrix and the nanoinclusions which leads to a large Seebeck coefficient, giving rise to such a high ZT. In addition, a new‐type CoSb3 thin‐film‐based device is successfully fabricated, which exhibits a high output power density of 8.25 mW cm−2 at a temperature difference of 140 K and a cold‐side temperature of 573 K, indicating the potential for application to medium‐to‐high‐temperature power generation scenarios. [ABSTRACT FROM AUTHOR]