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Cd-containing polycrystalline Bi0.46Sb1.54Te3 samples with precisely controlled phase composition were synthesized by conventional melting-quenching-annealing technique and a melt-spinning method. The pseudo ternary phase diagram for Cd–Bi/Sb–Te in the region near Bi0.46Sb1.54Te3 was systematically studied. Cd serves as an acceptor dopant contributing holes, whereas for samples doped with CdTe, the combined effects of the substitution of Sb/Bi with Cd and the formation of Sb/BiTe antisite defects leads to the increase in hole concentration. Moreover, upon doping with Cd, the lattice thermal conductivity decreases significantly owing to the intensified point defect phonon scattering. The sample with Cd content of 0.01 attains the maximum ZT of 1.15 at 425 K. The utilization of melt-spinning method brings about the in situ nanostructured CdTe and grain size refinement, which further reduce the lattice thermal conductivity while preserving excellent electrical performance. As a result, a higher ZT of 1.30 at 425 K is realized with CdTe content x = 0.005.

Bi2Te3 films always exhibit n-type transport characteristics even under the Bi-rich condition, which, however, was not clarified clearly. Herein, by virtue of advanced techniques such as scanning tunneling microscopy, angle-resolved photoelectron spectroscopy, scanning transmission electron microscopy, and x-ray photoelectron spectroscopy, we are able to identify the structural evolution on the atomic scale for Bi-rich Bi2Te3 films. The excess of Bi content will lead to the formation of p-type BiTe antisite defects; however, there is a doping limit for the excess of Bi to form BiTe antisites. Beyond this limit, the excess of Bi will form the n-type Bi2 planar defects in the van der Waals gap, the excellent electron donors, which can enhance the electron density by over one order of magnitude and up to the 1021 cm−3 range for Bi-rich Bi2Te3 films. Benefiting from the remarkable increase in the electron density and the suppression of carrier intrinsic excitations, Bi2Te3 films with Bi2 planar defects possess a much improved thermoelectric power factor, with a maximum value of 1.4 mW m−1 K−2 at 450 K, showing about 130% enhancement compared to that of the film without Bi2 intercalations. The discovery opens a new avenue to improve the thermoelectric properties of Bi2Te3 films utilizing the Bi2 planar defects.

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