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xBi2/3Cu3Ti4O12/(1-x)CaCu3Ti4O12 composites were prepared by traditional solid-state reaction method. Extremely high nonlinear coefficient of 25 and breakdown field of 18.92 kV·cm−1 were obtained in small current range of 0.1−1 mA·cm-2. In addition, reduced dielectric loss of 0.055 was achieved with high dielectric constant of 1369. Optimized nonlinear and dielectric properties were integrated to make the composites a promising dual-function varistor-capacitor candidate. Microstructure analysis discovered two areas with various Bi/Ca ratio, designated as Bi-H and Bi-L respectively. It was found that the maximum ratio of Bi-H/Bi-L heterogeneous interface corresponded to optimized nonlinear and dielectric performance, which was associated with elevated potential barrier height and huge grain boundary resistance. Combined with relaxation analysis, a core-shell structure was proposed to elaborate microstructure evolution in xBi2/3Cu3Ti4O12/(1-x)CaCu3Ti4O12 composite. According to the core-shell model, variation of heterogeneous interface was illustrated on how to influence nonlinear properties, which was well fitted to experimental results.  相似文献   
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