Microstructure and thermoelectric properties of pristine and Al-doped ZnO ceramics fabricated by cost-effective and eco-friendly wet chemistry methods

ZnO has potential as a thermoelectric material for high-temperature applications, but its performance is limited by the strong interconnection between electrical and thermal transportation. In this study we proved that ZnO bulk samples produced from cost-effective and environmentally friendly nitrates via ultrasonic spray pyrolysis and modified chemical precipitation methods followed by spark plasma sintering, demonstrate significantly higher thermoelectric performance than those fabricated from commercially available ZnO powder. To further explore the potential of the developed chemical precipitation technique, we synthesized a series of Al-doped samples with a nominal composition of Zn1-xAlxO (x = 0.02, 0.04, 0.06). The substitutuion of Al into the ZnO structure led to two significant effects: (i) a partial substitution of Zn with Al boosts the power factor; (ii) the formation of the ZnAl2O4 spinel phase acting as scattering center for phonons in addition to the mass and strain fluctuations induced by the partial Zn-Al substitution, both leading to the thermal conductivity reduction. As a result, Al doping led to a threefold enhancement of the thermoelectric performance with zT value of similar to 0.12 achieved at 1100 K for the Zn0.94Al0.06O sample.