BiCuSeO thermoelectric ceramics were fabricated using self-propagating high-temperature synthesis (SHS) combined with spark plasma sintering (SPS), and their phase compositions, microstructure, electrical properties, and thermal properties were systematically characterized and analyzed. The experimental results demonstrate that applying high-pressure condition during the sintering process will effectively restrict grain growth, reduce porosity, and lead to an increase in electrical conductivity. Simultaneously, high pressure sintering conditions reduce grain size and introduce additional grain boundaries and defects, which strengthens phonon scattering, thereby further decreasing both lattice thermal conductivity and total thermal conductivity. As a result, the high-pressure conditions significantly improve the thermoelectric figure of merit (ZT) of BiCuSeO. In brief, the samples sintered at 600 °C under 200 MPa achieve a maximum ZT value of 0.64 at approximately 792 K.
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