Hydride Anion Substitution Boosts Thermoelectric Performance of Polycrystalline SrTiO 3 via Simultaneous Realization of Reduced Thermal Conductivity and High Electronic Conductivity

The development of environmentally benign thermoelectric materials with high energy conversion efficiency ( ZT ) continues to be a long‐standing challenge. So far, high ZT has been achieved using heavy elements to reduce lattice thermal conductivity (κ lat ). However, it is not preferred to use such elements because of their environmental load and high material cost. Here a new approach utilizing hydride anion (H − ) substitution to oxide ion is proposed for ZT enhancement in thermoelectric oxide SrTiO 3 bulk polycrystals. Light element H − substitution largely reduces κ lat from 8.2 W/(mK) of SrTiO 3 to 3.5 W/(mK) for SrTiO 3− x H x with x = 0.216. The mass difference effect on phonon scattering is small in the SrTiO 3− x H x , while local structure distortion arising from the distributed Ti−(O,H) bond lengths strongly enhances phonon scattering. The polycrystalline SrTiO 3− x H x shows high electronic conductivity comparable to La‐doped SrTiO 3 single crystal because the H − substitution does not form a grain boundary potential barrier and thus suppresses electron scattering. As a consequence, SrTiO 3− x H x bulk exhibits maximum ZT = 0.11 at room temperature and the ZT value increases continuously up to 0.22 at T = 657 K. The H − substitution idea offers a new approach for ZT enhancement in thermoelectric materials without utilizing heavy elements.