A solid‐state thermoelectric device is attractive for diverse technological areas such as cooling, power generation and waste heat recovery with unique advantages of quiet operation, zero hazardous emissions, and long lifetime. With the rapid growth of flexible electronics and miniature sensors, the low‐cost flexible thermoelectric energy harvester is highly desired as a potential power supply. Herein, a flexible thermoelectric copper selenide (Cu2Se) thin film, consisting of earth‐abundant elements, is reported. The thin film is fabricated by a low‐cost and scalable spin coating process using ink solution with a truly soluble precursor. The Cu2Se thin film exhibits a power factor of 0.62 mW/(m K2) at 684 K on rigid Al2O3substrate and 0.46 mW/(m K2) at 664 K on flexible polyimide substrate, which is much higher than the values obtained from other solution processed Cu2Se thin films (<0.1 mW/(m K2)) and among the highest values reported in all flexible thermoelectric films to date (≈0.5 mW/(m K2)). Additionally, the fabricated thin film shows great promise to be integrated with the flexible electronic devices, with negligible performance change after 1000 bending cycles. Together, the study demonstrates a low‐cost and scalable pathway to high‐performance flexible thin film thermoelectric devices from relatively earth‐abundant elements.
Development of MEMS Process Compatible (Bi,Sb)2(Se,Te)3-Based Thin Films for Scalable Fabrication of Planar Micro-Thermoelectric Generators
Bismuth telluride-based thin films have been investigated as the active material in flexible and micro thermoelectric generators (TEGs) for near room-temperature energy harvesting applications. The latter is a class of compact printed circuit board compatible devices conceptualized for operation at low-temperature gradients to generate power for wireless sensor nodes (WSNs), the fundamental units of the Internet-of-Things (IoT). CMOS and MEMS compatible micro-TEGs require thin films that can be integrated into the fabrication flow without compromising their thermoelectric properties. We present results on the thermoelectric properties of (Bi,Sb)2(Se,Te)3 thin films deposited via thermal evaporation of ternary compound pellets on four-inch SiO2 substrates at room temperature. Thin-film compositions and post-deposition annealing parameters are optimized to achieve power factors of 2.75 mW m−1 K−2 and 0.59 mW m−1 K−2 for p-type and n-type thin films. The measurement setup is optimized to characterize the thin-film properties accurately. Thin-film adhesion is further tested and optimized on several substrates. Successful lift-off of p-type and n-type thin films is completed on the same wafer to create thermocouple patterns as per the target device design proving compatibility with the standard MEMS fabrication process.
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- Award ID(s):
- 2110603
- PAR ID:
- 10374299
- Date Published:
- Journal Name:
- Micromachines
- Volume:
- 13
- Issue:
- 9
- ISSN:
- 2072-666X
- Page Range / eLocation ID:
- 1459
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Thermoelectric generators (TEGs) convert temperature differences into electrical power and are attractive among energy harvesting devices due to their autonomous and silent operation. While thermoelectric materials have undergone substantial improvements in material properties, a reliable and cost-effective fabrication method suitable for microgravity and space applications remains a challenge, particularly as commercial space flight and extended crewed space missions increase in frequency. This paper demonstrates the use of plasma-jet printing (PJP), a gravity-independent, electromagnetic field-assisted printing technology, to deposit colloidal thermoelectric nanoflakes with engineered nanopores onto flexible substrates at room temperature. We observe substantial improvements in material adhesion and flexibility with less than 2% and 11% variation in performance after 10 000 bending cycles over 25 mm and 8 mm radii of curvature, respectively, as compared to previously reported TE films. Our printed films demonstrate electrical conductivity of 2.5 × 10 3 S m −1 and a power factor of 70 μW m −1 K −2 at room temperature. To our knowledge, these are the first reported values of plasma-jet printed thermoelectric nanomaterial films. This advancement in plasma jet printing significantly promotes the development of nanoengineered 2D and layered materials not only for energy harvesting but also for the development of large-scale flexible electronics and sensors for both space and commercial applications.more » « less
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Flexible thermoelectric generators (TEGs) have shown immense potential for serving as a power source for wearable electronics and the Internet of Things. A key challenge preventing large-scale application of TEGs lies in the lack of a high-throughput processing method, which can sinter thermoelectric (TE) materials rapidly while maintaining their high thermoelectric properties. Herein, we integrate high-throughput experimentation and Bayesian optimization (BO) to accelerate the discovery of the optimum sintering conditions of silver–selenide TE films using an ultrafast intense pulsed light (flash) sintering technique. Due to the nature of the high-dimensional optimization problem of flash sintering processes, a Gaussian process regression (GPR) machine learning model is established to rapidly recommend the optimum flash sintering variables based on Bayesian expected improvement. For the first time, an ultrahigh-power factor flexible TE film (a power factor of 2205 μW m −1 K −2 with a zT of 1.1 at 300 K) is demonstrated with a sintering time less than 1.0 second, which is several orders of magnitude shorter than that of conventional thermal sintering techniques. The films also show excellent flexibility with 92% retention of the power factor (PF) after 10 3 bending cycles with a 5 mm bending radius. In addition, a wearable thermoelectric generator based on the flash-sintered films generates a very competitive power density of 0.5 mW cm −2 at a temperature difference of 10 K. This work not only shows the tremendous potential of high-performance and flexible silver–selenide TEGs but also demonstrates a machine learning-assisted flash sintering strategy that could be used for ultrafast, high-throughput and scalable processing of functional materials for a broad range of energy and electronic applications.more » « less
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Abstract Thermoelectric generators are an environmentally friendly and reliable solid‐state energy conversion technology. Flexible and low‐cost thermoelectric generators are especially suited to power flexible electronics and sensors using body heat or other ambient heat sources. Bismuth telluride (Bi2Te3) based thermoelectric materials exhibit their best performance near room temperature making them an ideal candidate to power wearable electronics and sensors using body heat. In this report, Bi2Te3thin films are deposited on a flexible polyimide substrate using low‐cost and scalable manufacturing methods. The synthesized Bi2Te3nanocrystals have a thickness of 35 ± 15 nm and a lateral dimension of 692 ± 186 nm. Thin films fabricated from these nanocrystals exhibit a peak power factor of 0.35 mW m−1·K−2at 433 K, which is among the highest reported values for flexible thermoelectric films. In order to evaluate the flexibility of the thin films, static and dynamic bending tests are performed while monitoring the change in electrical resistivity. After 1000 bending cycles over a 50 mm radius of curvature, the change in electrical resistance of the film is 23%. Using Bi2Te3solutions, the ability to print thermoelectric thin films with an aerosol jet printer is demonstrated, highlighting the potential of additive manufacturing techniques for fabricating flexible thermoelectric generators.
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Over the past decade, Ag 2 Se has attracted increasing attention due to its potentially excellent thermoelectric (TE) performance as an n-type semiconductor. It has been considered a promising alternative to Bi–Te alloys and other commonly used yet toxic and/or expensive TE materials. To optimize the TE performance of Ag 2 Se, recent research has focused on fabricating nanosized Ag 2 Se. However, synthesizing Ag 2 Se nanoparticles involves energy-intensive and time-consuming techniques with poor yield of final product. In this work, we report a low-cost, solution-processed approach that enables the formation of Ag 2 Se thin films from Cu 2−x Se template films via cation exchange at room temperature. Our simple two-step method involves fabricating Cu 2−x Se thin films by the thiol-amine dissolution of bulk Cu 2 Se, followed by soaking Cu 2−x Se films in AgNO 3 solution and annealing to form Ag 2 Se. We report an average power factor (PF) of 617 ± 82 μW m −1 K −2 and a corresponding ZT value of 0.35 at room temperature. We obtained a maximum PF of 825 μW m −1 K −2 and a ZT value of 0.46 at room temperature for our best-performing Ag 2 Se thin-film after soaking for 5 minutes. These high PFs have been achieved via full solution processing without hot-pressing.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.3390/mi13091459
