This dissertation addresses the need to develop a scalable and standalone power generator for personal, commercial, and military transportation and communication systems. The standalone thermoelectric power generator (TPG) converts heat to electrical power in a unique way that does not draw on conventional power sources like batteries. A TPG is comprised of four main components: a heat source, thermoelectric modules, a heat sink, and thermal insulation. For system modeling and materials development purposes, the dissertation invented the first pyrophoric heated standalone TPG, solid-state renewable heat source, and two-component nanocomposite thermoelectric power generation material.

In this work, the first pyrophoric heated standalone thermoelectric power generator was designed, fabricated, and tested. The bases of the system were four porous silicon carbide combustors for the exothermic reaction of pyrophoric iron powder with oxygen. These combustors provided a heat source of 2,800 to 5,600 W to the heat sinks (through TE modules) at conditions suitable for a standalone, pyrophoric iron fueled TE power generator. The system integrated with 16 commercial bismuth telluride thermoelectric modules to produce 140 to 280 W of electrical power with a TE power conversion efficiency of ~5%. This demonstration represents an order-of-magnitude improvement in portable electrical power from thermoelectrics and hydrocarbon fuel, and a notable increase in the conversion efficiency compared with other published works.

To optimize the TE heat-to-power conversion performance of the TPG, numerical simulations were performed with computational fluid dynamics (CFD) using FLUENT. The temperature dependent material properties of bismuth telluride, effects of air flow rate (6 – 14 m/s) at 300 K, and effects of thermoelectric element thickness (4 – 8 mm) on temperature gradient generated across the module are investigated under constant power input (7.5 W). The obtained results reveal that all geometric parameters have important effect on the thermal performance of thermoelectric power generation module. The optimized single TE element thickness is 7 mm for electrical power generation of 0.47 W at temperature difference of 138 K. The TE heat-to-power conversion efficiency is 6.3%.

The first solid-state renewable heat source (without the use of hydrocarbons) were created with porous silicon carbide combustors coated with pyrophoric 1-3 micron-sized iron particles mixture. The thermal behavior and ignition characteristics of iron particles and mixtures were investigated. The mixture include activate carbon and sodium chloride, in which iron is the main ingredient used as fuel. The final mixture composition is determined to consist of iron powder, activate carbon, and sodium chloride with a weight ratio of approximately 5/1/1. The mixture generated two-peak DSC curves featured higher ignition temperatures of 431.53°C and 554.85°C with a higher heat generation of 9366 J/g than single iron particles.

The enhancement of figure-of-merit ZT or efficiency of thermoelectric materials is dependent on reducing the thermal conductivity. This dissertation synthesized and characterized the advanced two-component Si-Ge nanocomposites with a focus on lowering the thermal conductivity. The ball-milled two-component Si-Ge material demonstrated 50% reduction in thermal conductivity than the single component material used in the radioisotope thermoelectric generators and 10% reduction than the p-type SiGe alloy.