Abstract
Donor-doped TiO2-based materials are promising thermoelectrics (TEs) due to their low cost and high stability at elevated temperatures. Herein, high-performance Nb-doped TiO2 thick films are fabricated by facile and scalable screen-printing techniques. Enhanced TE performance has been achieved by forming high-density crystallographic shear (CS) structures. All films exhibit the same matrix rutile structure but contain different nano-sized defect structures. Typically, in films with low Nb content, high concentrations of oxygen-deficient {121} CS planes are formed, while in films with high Nb content, a high density of twin boundaries are found. Through the use of strongly reducing atmospheres, a novel Al-segregated {210} CS structure is formed in films with higher Nb content. By advanced aberration-corrected scanning transmission electron microscopy techniques, we reveal the nature of the {210} CS structure at the nano-scale. These CS structures contain abundant oxygen vacancies and are believed to enable energy-filtering effects, leading to simultaneous enhancement of both the electrical conductivity and Seebeck coefficients. The optimized films exhibit a maximum power factor of 4.3 × 10-4 W m-1 K-2 at 673 K, the highest value for TiO2-based TE films at elevated temperatures. Our modulation strategy based on microstructure modification provides a novel route for atomic-level defect engineering which should guide the development of other TE materials.
Original language | English |
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Pages (from-to) | 5071-5085 |
Number of pages | 15 |
Journal | ACS Applied Materials and Interfaces |
Volume | 15 |
Issue number | 4 |
Early online date | 19 Jan 2023 |
DOIs | |
Publication status | Published - 1 Feb 2023 |
Keywords
- crystallographic shear structure
- energy filtering
- Nb doping
- oxygen deficiency
- thermoelectric thick film