Achieving high quality factor and enhanced thermoelectric performance in polycrystalline SnS by Ag doping and Se alloying

The polycrystalline SnS with a similar layered crystal structure and band structure to SnSe exhibits enormous commercial thermoelectric potential due to its lower cost and environmentally friendly characteristics. However, the wider bandgap of SnS leads to low carrier concentration and inferior electrical transport performance. The two-dimensional interlayer hinders carrier transport, leading to interesting and mysterious anisotropic thermoelectric properties. Herein, we reported the optimized electron-phonon transport in anisotropic polycrystalline SnS by Ag doping and Se alloying, realizing a high quality factor B by multiple strategies of optimizing carrier concentration, modifying band structure, and introducing various defects; further potential performance is predicted by the single parabolic band model. Specifically, Ag-doped SnS not only significantly increases the carrier concentration and weighted mobility mu(w) in both directions but also induces multi-scale precipitates proven by the Debye-Callaway model to suppress phonon transport. Moreover, additional Se alloying optimizes the electronic band structure and increases the Seebeck coefficient, further improving mu(W) and boosting the maximum power factor to similar to 3.72 mu W cm(-1) K-2 at 873 K in the out-of-plane direction. Consequently, the synergistic optimization of carrier and phonon transport achieved a high B of 0.7 and a maximum zT(max) of similar to 0.8 at 873 K in Ag0.02Sn0.98S0.99Se0.01. Additionally, the high B predicted a high zT(max)similar to 1.5 based on optimized carrier transport characteristics, demonstrating the potential great-performance polycrystalline SnS. This work provides a promising avenue for optimizing the zT of polycrystalline SnS by transport engineering.