Oxygen partial pressure dependence of thermoelectric power factor in polycrystalline n-type SrTiO_3: Consequences for long term stability in thermoelectric oxides

摘要

The Seebeck coefficient and electrical conductivity have been measured as functions of oxygen partial pressure over the range of 10~(-22) to 10~(_1)atm at 1173K for a 10% niobium-doped SrTiO_3 ceramic with a grain size comparable to the oxygen diffusion length. Temperature-dependent measurements performed from 320 to 1275 K for as-prepared samples reveal metallic-like conduction and good thermoelectric properties. However, upon exposure to progressively increasing oxygen partial pressure, the thermoelectric power factor decreased over time scales of 24 h, culminating in a three order of magnitude reduction over the entire operating range. Identical measurements on single crystal samples show negligible changes in the power factor so that the instability of ceramic samples is primarily tied to the kinetics of grain boundary diffusion. This work provides a framework for understanding the stability of thermoelectric properties in oxides under different atmospheric conditions. The control of the oxygen atmosphere remains a significant challenge in oxide thermoelectrics.