Sintering behavior,microstructure and thermoelectric properties of calcium cobaltite thick films for transversal thermoelectric multilayer generators

The sintering behavior and the thermoelectric performance of Ca₃Co₄O₉ multilayer laminates were studied, and a multilayer thermoelectric generator was fabricated. Compacts and multilayer samples with anisotropic microstructure and residual porosity were obtained after conventional sintering at 920 °C, whereas dense and isotropic multilayer samples were prepared by firing at 1200 °C and reoxidation at 900 °C. A hot-pressed sample has a dense and anisotropic microstructure. Samples sintered at 920 °C exhibit low electrical conductivity due to the low density, whereas the Seebeck coefficient is not sensitive to preparation conditions. However, thermal conductivity of multilayers is very low, and, hence acceptable ZT values are obtained. A transversal multilayer thermoelectric generator (TMLTEG) was fabricated by stacking layers of Ca₃Co₄O₉ green tapes, AgPd conductor printing, and co-firing at 920 °C. The TMLTEG has a power output of 3 mW at ΔT = 200 K in the temperature interval of 25 °C to 300 °C.