Thermoelectric materials have the ability to convert heat energy to electrical power and vice versa. While the thermodynamic upper limit is defined by the Carnot efficiency, the material figure of merit, ZT is far from this theoretical limit, typically limited by a complex interplay of non-equilibrium charge and phonon scattering. Materials innovation is a slow, arduous process due to the complex correlations between crystal structure, microstructure engineering and thermoelectric properties. Many physical concepts and materials have been unearthed in this path to discovery, supported ably by innovations in technology over many decades, revealing important material and transport descriptors. In this review, we look back at some case studies of inorganic thermoelectric materials employing a birds-eye view of complementary advancements in scientific concepts and technological advancements and conclude that most high values of zT have emerged from new scientific ideas fueled by moderately mature technologies. Based on this conclusion, we then propose that the recent emergence of datadriven approaches and high throughput experiments, encompassing synthesis as well as characterization, with machine learning guided inverse design is perfectly suited to provide an accelerated pathway towards the discovery of next-generation thermoelectric materials, potentially providing a feasible alternative source of energy for a sustainable future.
Direct patterning of thermoelectric metal chalcogenides can be challenging and is normally constrained to certain geometries and sizes. Here we report the synthesis, characterization, and direct writing of sub-10 nm wide bismuth sulfide (Bi2S3) using a single source, spin coatable, and electron beam sensitive bismuth(III) ethylxanthate precursor. In order to increase the intrinsically low carrier concentration of pristine Bi2S3, we developed a self-doping methodology in which 23 sulfur vacancies are manipulated by tuning the temperature during vacuum annealing, to produce 24 an electron-rich thermoelectric material. We report a room temperature electrical conductivity of 25 6 S m -1 and a Seebeck coefficient of -21.41 µV K -1 for a directly patterned, sub-stoichiometric 26 Bi2S3 thin film. We expect that our demonstration of directly-writable thermoelectric films, with further optimization of structure and morphology can be useful for on-chip applications.
The discovery of novel materials for thermoelectric energy conversion has potential to be accelerated by data-driven screening combined with high-throughput calculations. One way to increase the efficacy of successfully choosing...
The best known thermoelectric material for near room temperature heat-to-electricity conversion is bismuth telluride. Amongst the possible fabrication techniques, electrodeposition has attracted attention due to its simplicity and low cost. However, the measurement of the thermoelectric properties of electrodeposited films is challenging because of the conducting seed layer underneath the film. Here, we develop a method to directly measure the thermoelectric properties of electrodeposited bismuth telluride thin films, grown on indium tin oxide. Using this technique, the temperature dependent thermoelectric properties (Seebeck coefficient and electrical conductivity) of electrodeposited thin films have been measured down to 100 K. A parallel resistor model is employed to discern the signal of the film from the signal of the seed layer and the data are carefully analysed and contextualized with literature. Our analysis demonstrates that the thermoelectric properties of electrodeposited films can be accurately evaluated without inflicting any damage to the films.
Development of nanoscale multicomponent solid inorganic materials is often hindered by slow solid diffusion kinetics and poor precursor mixing in conventional solid-state synthesis. These shortcomings can be alleviated by combining nanosized precursor mixtures and low temperature reaction, which could reduce crystal growth and accelerate the solid diffusion at the same time. However, high throughput production of nanoparticle mixtures with tunable composition via conventional synthesis is very challenging. In this work, we demonstrate that ∼10 nm homogeneous mixing of sub-10 nm nanoparticles can be achieved via spark nanomixing at room temperature and pressure. Kinetically driven Spark Plasma Discharge nanoparticle generation and ambient processing conditions limit particle coarsening and agglomeration, resulting in sub-10 nm primary particles of as-deposited films. The intimate mixing of these nanosized precursor particles enables intraparticle diffusion and formation of Cu/Ni nanoalloy during subsequent low temperature annealing at 100 °C. We also discovered that cross-particle diffusion is promoted during the low-temperature sulfurization of Cu/Ag which tends to phase-segregate, eventually leading to the growth of sulfide nanocrystals and improved homogeneity. High elemental homogeneity, small diffusion path lengths, and high diffusibility synergically contribute to faster diffusion kinetics of sub-10 nm nanoparticle mixtures. The combination of ∼10 nm homogeneous precursors via spark nanomixing, low-temperature annealing, and a wide range of potentially compatible materials makes our approach a good candidate as a general platform toward accelerated solid state synthesis of nanomaterials.
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