Constructing cell-membrane-mimic grain boundaries for high-performance n-type Ag2Se using high-dielectric-constant TiO2

The coupling of charge carrier and phonon transport limits the application of Ag2Se as a low-toxic near-room-temperature thermoelectric material. Strategies that reduce the thermal conductivity via enhancing the phonon scattering usually lead to reduced carrier mobility due to high grain boundary potential barrier. In this study, we developed a cell-membrane-mimic grain boundary engineering strategy for decoupling the charge carrier and phonon scattering through decorating high-dielectric-constant rutile TiO2 at Ag2Se grain boundaries to enable the charge carrier/phonon selective permeability. The nano-sized TiO2 with high dielectric permittivity can secure the charge carrier transport by shielding the interfacial Coulomb potential to lower the energy barrier of grain boundaries, rendering an enhanced power factor. Additionally, benefited from the enhanced phonon scattering by TiO2 nanoparticles, a significantly decreased lattice thermal conductivity of ∼0.20 W m−1 K−1 and a high zT of ∼0.97 at 390 K are obtained in the Ag2Se-based nanocomposites. This work demonstrates that such cell-membrane-mimic grain boundary engineering strategy may shed light on developing high-performance thermoelectric materials.