Stabilization of high-performance rock-salt LiMnSbTe3 thermoelectrics with embedded van der Waals-like gaps

Rock-salt-structured compounds like lead chalcogenides are promising thermoelectrics, as their high symmetry, strong anharmonicity, and favorable phase behavior collectively lead to high performance by enabling large power factors and ultralow thermal conductivity. Here, we report LiMnSbTe3, a new rock-salt semiconductor stabilized through targeted chemical design by combining hexagonal MnTe with cubic LiSbTe2. Embedded in the high-symmetry matrix, van der Waals-like gaps form due to Sb2Te3 nanoscale segregation, which acts as effective phonon-scattering centers, leading to a low lattice thermal conductivity of 0.37 Wm-1K-1 at 873 K with alloy scattering from disordered cations. The ordered local structure of Sb2Te3-type vdW-like gaps and the cross-gap interaction facilitate the carrier transport. Aided by energy-converged valence bands and a paramagnon drag effect, high Seebeck coefficients and enhanced power factor can be achieved, leading to a high ZT of 1.2 at 873 K. Furthermore, introducing Mn deficiency increases ZT to 1.5, highlighting the potential for higher performance through optimized doping or alloying. A segmented single-leg thermoelectric module achieves an output power density of 0.52 Wcm-2 and an efficiency of 8.7% under ∆T of 478 K, further demonstrating its promising thermoelectric applications. The authors synthesize rock-salt-structured LiMnSbTe3, in which Sb2Te3-type van der Waals-like gaps are embedded as ordered local structures that both scatter phonons and enhance charge-carrier transport.