Abstract

Seeking new strategies to tune the intrinsic defect and optimize the thermoelectric performance via no or less use of external doped elements (i.e., plain optimization) is an important method to realize the sustainable development of thermoelectric materials. Meanwhile, creating dislocation defects in oxide systems is quite challenging because the rigid and stiff ionic/covalent bonds can hardly tolerate the large strain energy associated with dislocations. Herein, taking BiCuSeO oxide as an example, the present work reports a successful construction of dense lattice dislocations in BiCuSeO by self-doping of Se at the O site (i.e., SeO self-substitution), and achieves plain optimization of the thermoelectric properties with only external Pb doping. Owing to the self-substitution-induced large lattice distortion and the potential reinforcement effect by Pb doping, high-density (about 3.0×1014 m-2) dislocations form in the grains, which enhances the scattering strength of mid-frequency phonon and results in a substantial low lattice thermal conductivity of 0.38 W m-1 K-1 at 823 K in Pb-doped BiCuSeO. Meanwhile, PbBi doping and Cu vacancy markedly improve the electrical conductivity while maintaining a competitively high Seebeck coefficient, thereby contributing to a highest power factor of 942 μW m-1 K-2. Finally, a remarkably enhanced zT value of 1.32 is obtained at 823 K in Bi0.94Pb0.06Cu0.97Se1.05O0.95 with almost compositional plainification. The high-density dislocation structure reported in this work will also provide a good inspiration for the design and construction of dislocations in other oxide systems.

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