Abstract
Transition-metal dichalcogenide WSe2 has attracted increasing interest due to its large thermopower (S), low-cost, and environment-friendly constituents. However, its thermoelectric figure of merit, ZT, of WSe2 is limited due to its large lattice thermal conductivity (κL) and low electrical conductivity. In view of WSe2 and MoS2 having the same crystal structure, here we designed and prepared Nb-doped quarternary mixed crystal (MC) Nb0.05W0.95-xMox(Se1-xSx)2 (0 ≤ x ≤ 0.095). The results indicate that the κL of the MC can reach as low as 0.12 W m K-1 at 850 K, being 93% smaller than that of WSe2. Our analysis reveals that its low κL originates chiefly from intense scattering of both high-frequency phonons from point defects (mainly alloying elements) and mid/low-frequency phonons from MoS2 inclusions residual within MC. In addition, the alloying of WSe2 with MoS2 causes a 5-fold increase in cation vacancies (VW‴'), leading to a large increase in hole concentration and electrical conductivity, which gives rise to a ∼7.5 times increase in power factor (reaching 4.2 μ W cm-1 K-2 at 850 K). As a result, a record high ZTmax = 0.63 is achieved at 850 K for the MC sample with x = 0.076, which is 20 times larger than that of WSe2, demonstrating that MC Nb0.05W0.95-xMox(Se1-xSx)2 is a promising thermoelectric material.
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