Journal
CERAMICS INTERNATIONAL
Volume 47, Issue 1, Pages 111-120Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.ceramint.2020.08.113
Keywords
CaCu3Ti4O12 ceramics; Giant dielectric response; Relaxation behavior; Complex impedance spectroscopy; Electric modulus
Categories
Funding
- National Natural Science Foundation of China [51772242, 51621063]
- Fundamental Research Funds for the Central Universities [xjj2016017]
- 111 Project 2.0 [BP2018008]
- Innovative Research Team of Ministry of Education of China [IRT13034]
- China Scholarship Council [201906280157]
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This study developed a novel system of isovalent Zr4+ and donor Nb5+ co-doped CaCu3Ti4O12 (CCTO) ceramics to enhance dielectric response. The co-doping of Zr4+ and Nb5+ ions significantly reduced grain size and improved dielectric constant, leading to giant dielectric response within broader frequency and temperature ranges. The enhanced dielectric response is primarily attributed to the complex defect dipoles associated with oxygen vacancies by co-doping Zr4+ and Nb5+ ions into CCTO structure.
In this work, we developed a novel system of isovalent Zr4+ and donor Nb5+ co-doped CaCu3Ti4O12 (CCTO) ceramics to enhance dielectric response. The influences of Zr4+ and Nb5+ co-substituting on the colossal di-electric response and relaxation behavior of the CCTO ceramics fabricated by a conventional solid-phase synthesis method were investigated methodically. Co-doping of Zr4+ and Nb5+ ions leads to a significant reduction in grain size for the CCTO ceramics sintered at 1060 degrees C for 10 h. XRD and Raman results of the CaCu3Ti3.8-xZrxNb0.2O12 (CCTZNO) ceramics show a cubic perovskite structure with space group Im-3. The first principle calculation result exhibits a better thermodynamic stability of the CCTO structure co-doped with Zr4+ and Nb5+ ions than that of single-doped with Zr4+ or Nb5+ ion. Interestingly, the CCTZNO ceramics exhibit greatly improved dielectric constant (similar to 10(5)) at a frequency range of 10(2)-10(5) Hz and at a temperature range of 20-210 degrees C, indicating a giant dielectric response within broader frequency and temperature ranges. The di-electric properties of CCTZNO ceramics were analyzed from the viewpoints of defect-dipole effect and internal barrier layer capacitance (IBLC) model. Accordingly, the immensely enhanced dielectric response is primarily ascribed to the complex defect dipoles associated with oxygen vacancies by co-doping Zr4+ and Nb5+ ions into CCTO structure. In addition, the obvious dielectric relaxation behavior has been found in CCTZNO ceramics, and the relaxation process in middle frequency regions is attributed to the grain boundary response confirmed by complex impedance spectroscopy and electric modulus.
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