4.7 Article

Regulation of exciton for high thermoelectric performance in (Bi, Sb)2Te3 alloys via doping with Pb and multi-scale microstructure

Journal

JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
Volume 41, Issue 15, Pages 7703-7710

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.jeurceramsoc.2021.08.041

Keywords

(Bi,Sb)(2)Te-3 alloys; Melt-spinning; Thermoelectricity; Selective scattering; Bipolar thermal conductivity

Funding

  1. Natural Science Foundation of China [51972256, 51872219, 51632006, 51521001]
  2. National Key Research and Development Program of China [2019YFA0704900]
  3. 111 Project of China [B07040]
  4. Wuhan Frontier Project on Applied Research Foundation [2019010701011405]
  5. Fundamental Research Funds for the Central Universities [WUT: 2020IVB056, 20201h0028a]
  6. Fundamental Research Funds for the Central Uni-versities [WUT: 2021III016GX]
  7. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing

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A significant improvement in the thermoelectric performance of BiSbTe alloy was achieved through dynamically regulating excitation behavior, doping with lead, and inducing refined grains and nanostructures through melt-spinning. This led to enhanced power factor and reduced thermal conductivity, resulting in the highest ZT value and conversion efficiency compared to a commercial ZM-based module under the same temperature gradient.
Herein, we report a reproducible improvement of the thermoelectric performance in BiSbTe alloy via kinetically and dynamically regulating excitation behavior in the intrinsic excitation regime. Doping with Pb increases the carrier concentration to the optimal value, kinetically pushing the onset temperature for the intrinsic excitation from 350 K for Bi0.46Sb1.54Te3 sample to 450 K for Pb-0.01(Bi0.46Sb1.54)(0.995)Te-3 sample. Moreover, the refined grains, nanostructures as well as dense dislocations induced by the melt-spinning process not only lower the lattice thermal conductivity via intensifying the interfacial phonon scattering but also selectively block the migration of minority carrier, modifying the dynamic process of the charge carrier and resulting in a smaller ratio of (mu(e)/mu(h)). This improves the power factor in the measured temperature range and suppresses the bipolar thermal conductivity in the intrinsic excitation regime. Thus, a maximum power factor of 4.44 mW m(-1) K-2 and the lowest thermal conductivity of 1.06 W m(-1) K-1 are attained for the sample with refined grains and nano structures. All these contribute to the highest ZT value of 1.31 at 380 K and the highest average ZT value of 1.17 from 300 K to 500 K for Pb-0.002(Bi0.46Sb1.54)(0.999)Te-3 sample. This improved thermoelectric property was further verified in a thermoelectric module with the conversion efficiency of 4.38 % under a temperature gradient of 175 K, which is 20 % higher than that of the commercial ZM-based module under the same temperature gradient.

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