4.8 Article

Ultralow Lattice Thermal Conductivity and Improved Thermoelectric Performance in Cl-Doped Bi2Te3-xSex Alloys

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 29, Pages 33567-33579

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c0868633567

Keywords

bismuth telluride; thermoelectric properties; anisotropy; bipolar conduction; two-band Kane model; bonding inhomogeneity; lone-pair electrons

Funding

  1. Foundation for Polish Science [TEAM-TECH/2016-2/14]
  2. European Union under European Regional Development Fund
  3. Excellence Initiative - Research University ?
  4. AGH University of Science and Technology

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This study systematically investigates the microstructure and thermoelectric properties of Cl-doped Bi2Te3-xSex alloys and finds that Cl atoms act as electron donors to regulate the carrier concentration and effectively suppress minority carrier transport in Bi2Te3-xSex alloys. By manipulating the polarity of Bi-(Te/Se)1 and Bi-(Te/Se)2 bonds as well as the lone-pair (Te/Se) interactions, a significant reduction of lattice thermal conductivity in both pressing directions is achieved. As a result, a maximum ZT value of 1.0 is obtained at 473 K in the Bi2Te2.385Se0.6Cl0.015 sample.
Bi2Te3-based alloys are the main materials for the construction of low- and medium-temperature thermoelectric modules. In this work, the microstructure and thermoelectric properties of Cl-doped Bi2Te3-xSex alloys were systematically investigated considering the high anisotropy inherent in these materials. The prepared samples have a highly oriented microstructure morphology, which results in very different thermal transport properties in two pressing directions. To accurately separate the lattice, electronic, and bipolar components of the thermal conductivity over the entire temperature range, we employed a two-band Kane model to the Cl-doped Bi2Te3-xSex alloys. It was established that Cl atoms act as electron donors, which tune the carrier concentration and effectively suppress the minority carrier transport in Bi2Te3-xSex alloys. The estimated value of the lattice thermal conductivity was found to be as low as 0.15 Wm(-1) K-1 for Bi2Te3-x-ySexCly with x = 0.6 and y = 0.015 at 673 K in parallel to the pressing direction, which is among the lowest values reported for crystalline materials. The large reduction of the lattice thermal conductivity in both pressing directions for the investigated Bi2Te3-xSex alloys is connected with the different polarities of the Bi-(Te/Se)1 and Bi-(Te/Se)2 bonds, while the lone-pair (Te/Se) interactions are mainly responsible for the extremely low lattice thermal conductivity in the parallel direction. As a result of the enhanced power factor, suppressed bipolar conduction, and ultralow lattice thermal conductivity, a maximum ZT of 1.0 at 473 K has been received in the Bi2Te2.385Se0.6Cl0.015 sample.

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