P-type thermoelectric oxides for low-power transverse thermoelectric generators (TTEGs)
IBRAHIM A. 1, BOCHMANN A. 1, LÖHNERT R. 1, TÖPFER J. 1
1 Ernst-Abbe-Hochscule Jena - University of Applied Sciences, Jena, Germany
Thermoelectric generators (TEGs) based on oxide materials are non-toxic, cost-efficient devices that convert thermal energy directly into electrical energy employing the Seebeck effect. In this work, two different p-type oxide thermoelectric (TE) materials were prepared by solid state reaction (SSR) for building transverse thermoelectric devices with enhanced output power for low-power applications. These TE materials are lanthanum copper oxide La2CuO4 (LCO) which is suitable for energy harvesting in the low temperature regime, and calcium cobalt oxide Ca3Co4O9 (CCO), which is suitable for applications at elevated temperatures up to 800°C.
For the optimization of the thermoelectric properties of LCO, strontium doping La1.99Sr0.01CuO4 (LSCO) increased the electrical conductivity from 1440 S/m to 2960 S/m compared to undoped LCO, leading to a power factor of PF=305 µW/(m.K2) at 100°C. On the other hand, the synthesis protocol of CCO was optimized by controlling the average particle size of the fine-milled powder. The electrical conductivity of CCO pellets sintered at 920°C for 24h increased from 6500 S/m for a powder of an aggregate particle size d(50) of 4.5µm to 12390S/m at 800°C for a powder of d(50) of 0.95 µm, respectively. Consequently, the power factor (PF) and zT reach 380 µW/(m.K2) and 0.17, respectively, for sintered pellets of the latter powder.
A transverse thermoelectric generator (TTEG) consists of alternating layers of a thermoelectric material and a metal tilted at an angle ? relative to the heat flux direction. For building a TTEG, analytical calculations of the maximum figure-of-merit ( ) and the maximum PF as a function of TTEG tilt angle ? and the metal-to-ceramic thickness ratio () were accomplished. From these quick analytical calculations, the optimal values of and ? for TTEGs with optimal efficiency and output power can be predicted. In addition, 3D FEM simulations of TTEGs and transverse multilayer TEGs (TMLTEGs) were carried out via COMSOL-Multiphysics software to overcome the limitations of the analytical calculations. In order to verify these analytical calculations and COMSOL simulations, TTEGs of LSCO pellets with screen-printed silver (Ag) layers, and TMLTEGs based on LSCO or CCO green tapes with screen-printed Ag stripes tilted at angle ?, and cofired at 900°C or 920°C, respectively, were fabricated and their thermoelectric performance was measured. Preliminary results of a 5-pellet TTEG with dimensions of 16.4*10.3*3.6 mm3, LSCO thickness of 1.4 mm, Ag layer-thickness of 58 µm, hence =3%, and ?=66°, show an output power of 2.1mW at ΔT=150°C. Moreover, for a TTEG with Ag layer-thickness of 144µm, and =8%, the output power is 3.3mW at ΔT=150°C. Other TTEGs with different LSCO thickness and number of layers are fabricated and tested. Alternatively, a TMLTEG with dimensions of 36.5*3.3*6.3 mm3 based on LSCO tapes with screen-printed Ag stripes tilted at 60° measures an output power of 9.3mW at ΔT=250°C. These experimentally measured results verify the analytical calculations and COMSOL simulations. This demonstrates that a generator design using the transverse thermoelectric effect and low-performance, but inexpensive thermoelectric oxide materials might prove useful for harvesting electric power in the mW range from temperature gradients.