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With the rapid development of electronic industry, the demands for dielectric materials with high permittivities, low losses, and excellent electrical breakdown strengths prepared via low temperature fabrication techniques are increasing. Herein, we propose one-step cold sintering process route to improve the comprehensive performances of BaTiO3 based ceramics by integrating PEI. Dense BaTiO3-PEI nanocomposites can be prepared via cold sintering process at 250 °C using Ba(OH)2∙8H2O and H2TiO3 as the transient liquid phase. The grain growth of BaTiO3 is inhibited and thin PEI layers with less than 10 nm are located at the grain boundaries. The dissolution-precipitation process triggered by transient liquid phase and viscos flow assisted by PEI dominate the cold sintering mechanism of (1-x)BaTiO3-xPEI nanocomposites. The dielectric properties are stable over a broad temperature range up to 200 °C. Superior performances with a relative permittivity of 163 and a low dielectric loss of 0.014 are obtained in 80BaTiO3-20PEI nanocomposites, and the electrical breakdown strength is increased by 80.65% compared with BaTiO3. Overall, cold sintering process provides a potential way to develop dielectric nanocomposites with excellent comprehensive performances.
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