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Abstract The development of new materials and their compositional and microstructural optimization are essential in regard to next-generation technologies such as clean energy and environmental sustainability. However, materials discovery and optimization have been a frustratingly slow process. The Edisonian trial-and-error process is time consuming and resource inefficient, particularly when contrasted with vast materials design spaces¹. Whereas traditional combinatorial deposition methods can generate material libraries^2,3, these suffer from limited material options and inability to leverage major breakthroughs in nanomaterial synthesis. Here we report a high-throughput combinatorial printing method capable of fabricating materials with compositional gradients at microscale spatial resolution. In situ mixing and printing in the aerosol phase allows instantaneous tuning of the mixing ratio of a broad range of materials on the fly, which is an important feature unobtainable in conventional multimaterials printing using feedstocks in liquid–liquid or solid–solid phases^4–6. We demonstrate a variety of high-throughput printing strategies and applications in combinatorial doping, functional grading and chemical reaction, enabling materials exploration of doped chalcogenides and compositionally graded materials with gradient properties. The ability to combine the top-down design freedom of additive manufacturing with bottom-up control over local material compositions promises the development of compositionally complex materials inaccessible via conventional manufacturing approaches. 

Abstract Solution‐processable semiconducting 2D nanoplates and 1D nanorods are attractive building blocks for diverse technologies, including thermoelectrics, optoelectronics, and electronics. However, transforming colloidal nanoparticles into high‐performance and flexible devices remains a challenge. For example, flexible films prepared by solution‐processed semiconducting nanocrystals are typically plagued by poor thermoelectric and electrical transport properties. Here, a highly scalable 3D conformal additive printing approach to directly convert solution‐processed 2D nanoplates and 1D nanorods into high‐performing flexible devices is reported. The flexible films printed using Sb₂Te₃nanoplates and subsequently sintered at 400 °C demonstrate exceptional thermoelectric power factor of 1.5 mW m⁻¹K⁻²over a wide temperature range (350–550 K). By synergistically combining Sb₂Te₃2D nanoplates with Te 1D nanorods, the power factor of the flexible film reaches an unprecedented maximum value of 2.2 mW m⁻¹K⁻²at 500 K, which is significantly higher than the best reported values for p‐type flexible thermoelectric films. A fully printed flexible generator device exhibits a competitive electrical power density of 7.65 mW cm⁻²with a reasonably small temperature difference of 60 K. The versatile printing method for directly transforming nanoscale building blocks into functional devices paves the way for developing not only flexible energy harvesters but also a broad range of flexible/wearable electronics and sensors. 

Abstract Printing is a versatile method to transform semiconducting nanoparticle inks into functional and flexible devices. In particular, thermoelectric nanoparticles are attractive building blocks to fabricate flexible devices for energy harvesting and cooling applications. However, the performance of printed devices are plagued by poor interfacial connections between nanoparticles and resulting low carrier mobility. While many rigid bulk materials have shown a thermoelectric figure of meritZTgreater than unity, it is an exacting challenge to develop flexible materials withZTnear unity. Here, a scalable screen‐printing method to fabricate high‐performance and flexible thermoelectric devices is reported. A tellurium‐based nanosolder approach is employed to bridge the interfaces between the BiSbTe particles during the postprinting sintering process. The printed BiSbTe flexible films demonstrate an ultrahigh room‐temperature power factor of 3 mW m⁻¹K⁻²andZTabout 1, significantly higher than the best reported values for flexible films. A fully printed thermoelectric generator produces a high power density of 18.8 mW cm⁻²achievable with a small temperature gradient of 80 °C. This screen‐printing method, which directly transforms thermoelectric nanoparticles into high‐performance and flexible devices, presents a significant leap to make thermoelectrics a commercially viable technology for a broad range of energy harvesting and cooling applications.