N-Type Thermoelectric AgBiPbS 3 with Nanoprecipitates and Low Thermal Conductivity.

Inorganic chemistry(2023)

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摘要
Thermoelectric sulfide materials are of particular interest due to the earth-abundant and cost-effective nature of sulfur. Here, we report a new n-type degenerate semiconductor sulfide, AgBiPbS, which adopts a 3̅ structure with a narrow band gap of ∼0.32 eV. Despite the homogeneous distribution of elements at the scale of micrometer, AgS nanoprecipitates with dimensions of several nanometers were detected throughout the matrix. AgBiPbS exhibits a low room-temperature lattice thermal conductivity of 0.88 W m K, owing to the intrinsic low lattice thermal conductivity of AgS and the effective scattering of phonons at nanoprecipitate boundaries. Moreover, compared to AgBiS, AgBiPbS demonstrates a significantly improved weighted mobility of >16 cm V s at 300 K, leading to an enhanced PF of 1.6 μW cm K at 300 K. The superior electrical transport in AgBiPbS can be attributed to the high valley degeneracy of the point (the conduction band minimum), which is contributed by the Pb s and Pb p orbitals. Further, Ga doping is found to be effective in modulating the Fermi levels of AgBiPbS, leading to further enhancement of PF with a PF of 2.7 μW cm K in the temperature range of 300-823 K. Consequently, a relatively high ZT of 0.22 and a peak ZT of ∼0.4 at 823 K have been achieved in 3% Ga-doped AgBiPbS, highlighting the potential of AgBiPbS as an n-type thermoelectric sulfide.
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