Li2CO3 첨가에 따른 입방정 Bi1.5Zn1.0Nb1.5O7(c-BZN)의 상 변화 및 그에 따른 유전특성 변화 연구
A Study on the Phase Change of Cubic Bi1.5Zn1.0Nb1.5O7(c-BZN) and the Corresponding Change in Dielectric Properties According to the Addition of Li2CO3
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(1-4x)Bi1.5Zn1.0Nb1.5O7-3xBi2Zn2/3Nb4/3O7-2xLiZnNbO4(x=0.03-0.21) 조성의 새로운 저온 동시 소성 세라믹(LTCC) 유전체는 Bi1.5Zn1.0Nb1.5O7-xLi2CO3(x=0.03-0.21) 혼합물을 850oC~920oC에서 4 시간 반응성 액상소결(reactive liquid phase sintering)을 하여 제조하였다. 소결이 진행되는 동안 Li2CO3는 Bi1.5Zn1.0Nb1.5O7과 반응하여 Bi2Zn2/3Nb4/3O7 과 LiZnNbO4를 생성하였고 얻어진 소결체의 상대 소결밀도는 이론 밀도의 96% 이상이었다. 초기 Li2CO3 함량(x)을 조절하여 최종 소결체내에 존재하는 Bi1.5Zn1.0Nb1.5O7, Bi2Zn2/3Nb4/3O7 및 LiZnNbO4 상의 상대적인 함량을 제어함으로써높은 유전율(r), 낮은 유전손실(tan ) 및 NP0 특성(TC ≤ ±30 ppm/oC)의 유전율 온도계수(TC)를 갖는 유전체를 개발할 수 있었다. Li2CO3의 첨가가 x=0.03 mol에서 x=0.15 mol로 증가함에 따라 얻어진 복합체 내의 Bi2Zn2/3Nb4/3O7와LiZnNbO4의 부피 분율은 증가하였고, Bi1.5Zn1.0Nb1.5O7의 부피 분율은 감소하였다. 그 결과 복합체의 유전율(r)은 148.38 에서 126.99로 유전손실(tan )은 5.29×10-4에서 3.31×10-4로 그리고 유전율 온도계수(TC)는 -340.35 ppm/oC에서 299.67 ppm/oC로 변화되었다. NP0 특성을 갖는 유전체는 Li2CO3의 함량이 x=0.09일 때 얻을 수 있었고, 이 때의 유전율(εr)은143.06, 유전손실(tan )값은 4.31×10-4, 그리고 유전율 온도계수(TC)값은 -9.98 ppm/oC 이었다. Ag전극과의 화학적 호환성 실험은 개발된 복합 재료는 Ag 전극과 동시 소성 과정에서 전극과 반응이 없음을 보여주었다.
Abstract
A novel low-temperature co-fired ceramic (LTCC) dielectric, composed of (1-4x)Bi1.5Zn1.0Nb1.5O7-3xBi2Zn2/3Nb4/3O7- 2xLiZnNbO4 (x=0.03-0.21), was synthesized through reactive liquid phase sintering of Bi1.5Zn1.0Nb1.5O7-xLi2CO3 ceramic at temperatures ranging from 850°C to 920°C for 4 hours. During sintering, Li2CO3 reacted with Bi1.5Zn1.0Nb1.5O7, resulting in the formation of Bi2Zn2/3Nb4/3O7, and LiZnNbO4. The resulting sintered body exhibited a relative sintering density exceeding 96% of the theoretical density. By altering the initial Li2CO3 content (x) and consequently modulating the volume fraction of Bi1.5Zn1.0Nb1.5O7, Bi2Zn2/3Nb4/3O7, and LiZnNbO4 in the final sintered body, a sample with high dielectric constant (εr), low dielectric loss (tan δ), and the temperature coefficient of dielectric constant (TCε) characterized by NP0 specification (TCε ≤ ±30 ppm/°C) was achieved. As the Li2CO3 content increased from x=0.03 mol to x=0.15 mol, the volume fraction of Bi2Zn2/3Nb4/3O7 and LiZnNbO4 in the composite increased, while the volume fraction of Bi1.5Zn1.0Nb1.5O7 decreased. Consequently, the dielectric constant (εr) of the composite materials varied from 148.38 to 126.99, the dielectric loss (tan δ) shifted from 5.29×10-4 to 3.31×10-4, and the temperature coefficient of dielectric constant (TCε) transitioned from -340.35 ppm/°C to 299.67 ppm/°C. A dielectric exhibiting NP0 characteristics was achieved at x=0.09 for Li2CO3, with a dielectric constant (εr) of 143.06, a dielectric loss (tan δ) value of 4.31x10-4, and a temperature coefficient of dielectric constant (TCε) value of -9.98 ppm/°C. Chemical compatibility experiment with Ag electrode revealed that the developed composite material exhibited no reactivity with the Ag electrode during the co-firing process.
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