Silicon based thermoelectrics are promising candidates for high temperature energy scavenging applications. We present the properties of thermoelectrics made from highly boron doped silicon nanoparticles. The particles were produced by a continuous gas phase process in a scaled‐up synthesis plant enabling production rates in the kg h−1 regime. The silicon nanoparticles were compacted by direct current assisted sintering to yield nanocrystalline bulk silicon with average crystallite size between 40 and 80 nm and relative densities above 97% of the density of single crystalline silicon. The influence of the sintering temperature on the thermoelectric properties is investigated. It was found that high sintering temperatures are beneficial for an enhancement of the power factor, while the thermal conductivity was only moderately affected. The optimization of the compaction procedure with respect to the transport properties leads to zT values of the p‐type nanosilicon of 0.32 at 700 °C, demonstrating the potential of our method.
Here we present the realization of efficient and sustainable silicon‐based thermoelectric materials from nanoparticles. We employ a gas phase synthesis for the nanoparticles which is capable of producing doped silicon (Si) nanoparticles, doped alloy nanoparticles of silicon and germanium (Ge), SixGe1–x, and doped composites of Si nanoparticles with embedded metal silicide precipitation phases. Hence, the so‐called “nanoparticle in alloy” approach, theoretically proposed in the literature, forms a guideline for the material development. For bulk samples, a current‐activated pressure‐assisted densification process of the nanoparticles was optimized in order to obtain the desired microstructure. For thin films, a laser annealing process was developed. Thermoelectric transport properties were characterized on nanocrystalline bulk samples and laser‐sintered‐thin films. Devices were produced from nanocrystalline bulk silicon in the form of p–n junction thermoelectric generators, and their electrical output data were measured up to hot side temperatures of 750 °C. In order to get a deeper insight into thermoelectric properties and structure forming processes, a 3D‐Onsager network model was developed. This model was extended further to study the p–n junction thermoelectric generator and understand the fundamental working principle of this novel device architecture.
Gas phase synthesis of composite nanoparticles; nanocrystalline bulk with optimized composite microstructure; laser‐annealed thin film.
We present the fabrication of a high-temperature stable thermoelectric generator based on nanocrystalline silicon. Highly doped silicon nanoparticles were sintered by a current activated sintering technique to get nanocrystalline bulk silicon. The metalization of silicon was realized by (electro-)chemical plating and the specific electrical contact resistance ρc of the semiconductor-metal interface was measured by a transfer length method. Values as low as $\rho _C < 1 \cdot 10^{ - 6} \,\Omega cm^2 $ were measured. The metalized nanocrystalline silicon legs were sintered to metalized ceramic substrates using a silver-based sinter paste. The device figure of merit of the thermoelectric generator was determined by a Harman measurement with a maximum ZT of approximately 0.13 at 600 °C.
A new thermoelectric concept using large area silicon PN junctions is experimentally demonstrated. In contrast to conventional thermoelectric generators where the n-type and p-type semiconductors are connected electrically in series and thermally in parallel, we demonstrate a large area PN junction made from densified silicon nanoparticles that combines thermally induced charge generation and separation in a space charge region with the conventional Seebeck effect by applying a temperature gradient parallel to the PN junction. In the proposed concept, the electrical contacts are made at the cold side eliminating the need for contacts at the hot side allowing temperature gradients greater than 100K to be applied. The investigated PN junction devices are produced by stacking n-type and p-type nanopowder prior to a densification process. The nanoparticulate nature of the densified PN junction lowers thermal conductivity and increases the intraband traps density which we propose is beneficial for transport across the PN junction thus enhancing the thermoelectric properties. A fundamental working principle of the proposed concept is suggested, along with characterization of power output and output voltages per temperature difference that are close to those one would expect from a conventional thermoelectric generator.
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