The misfit monolayered sulfides, (GdS)1.20NbS2, (DyS)1.22NbS2, (Gd0.1Dy0.9S)1.21NbS2, (Gd0.2Dy0.8S)1.21NbS2, and (Gd0.5Dy0.5S)1.21NbS2 and the misfit bilayered sulfide (GdS)0.60NbS2 were synthesized via sulfurization under flowing CS2/H2S gas and consolidated by pressure-assisted sintering. The thermoelectric properties of the monolayered and bilayered sulfides perpendicular (in-plane) and parallel (out-of-plane) to the pressing direction were investigated over a temperature range of 300–873 K. The crystal grains in all the sintered samples were preferentially oriented perpendicular to the pressing direction, which resulted in highly anisotropic electrical and thermal transport properties. All the sintered samples exhibited degenerate n-type semiconductor-like behavior, leading to a large thermoelectric power factor. The misfit layered structure yielded low lattice thermal conductivity. The evolution of the monolayered structures into bilayered structures affected their thermoelectric properties. The thermoelectric figure of merit (ZT) of monolayered (GdS)1.20NbS2 was higher than that of bilayered (GdS)0.60NbS2 due to the larger power factor and lower lattice thermal conductivity of (GdS)1.20NbS2. The lattice thermal conductivity of the monolayered sulfide was lower in (GdxDy1-xS)1.2+qNbS2 solid solutions. The large power factor and low lattice thermal conductivity allowed a ZT value of 0.13 at 873 K in (Gd0.5Dy0.5S)1.21NbS2 perpendicular to the pressing direction.
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