(Ca,Sr)ZrO3 陶瓷因高介電常數和低損耗特性，使其在C0G 型的MLCC中受到了廣泛的應用。其中，(Ca0.6Ba0.01Sr0.39)ZrO3 陶瓷在1450 ℃ 燒結下表現出良好的介電性能，包括在高頻 (9~10 GHz) 下量測的εr ∼ 28.38，tanδ ∼ 4.0×10-4，Q×f ∼ 22988 GHz，τf ∼ -58.3。故本研究以(Ca0.6Ba0.01Sr0.39)ZrO3 陶瓷為基礎，分別按(Ca0.6-xMgxSr0.39Ba0.01)ZrO3、(Ca0.6-xMgxSr0.39Ba0.01)(Zr1-xTix)O3 (X=0~0.05) 的比例摻雜MgO和MgTiO3，藉此探討Mg和Ti離子取代對CSBZ陶瓷密度、相結構、顯微結構和介電特性的影響。
研究結果顯示，摻雜MgTiO3之陶瓷中，存在Mg2+ 和Ti4+互相競爭至B位置之情形，而MgO的摻雜雖助燒效果明顯，卻易造成二次相增加。在1350 °C 燒結下，添加 1 mol% MgO 和 MgTiO3皆能改善(Ca0.6Ba0.01Sr0.39)ZrO3陶瓷的燒結緻密性並提升介電性能，其中，添加MgTiO3可更進一步降低燒結溫度，於1250 ℃燒結下，(Ca0.59Mg0.01Sr0.39Ba0.01)(Zr0.99Ti0.01)O3陶瓷的介電性能表現仍優於在1350 ℃ 下燒結之(Ca0.6Ba0.01Sr0.39)ZrO3 陶瓷，其介電性能包括在1 MHz下量測εᵣ ∼ 35.8，tanδ ∼ 2×10-4，IR ∼ 3.5×1013 Ω，以及高頻(8~10 GHz)下量測的εᵣ ∼ 34.8、Q×f ∼ 19697 GHz、和τf ∼ -25.1 ppm/C。
通過增加元素種類，提高系統亂度，可以有效降低(Ca,Sr,Ba,Mg)(Zr,Ti)O₃陶瓷的燒結溫度至1250℃，同時提升介電性能。該結果表明，熵工程是調整CSZ基材料介電性能的有效策略，具廣泛的應用前景，可為新型介電陶瓷材料的設計提供參考。

(Ca,Sr)ZrO3 ceramics, known for their high dielectric constant and low loss characteristics, are widely used in C0G-type MLCCs. Among them, (Ca0.6Ba0.01Sr0.39)ZrO3 ceramics sintered at 1450°C exhibit excellent dielectric properties, including εᵣ ∼ 28.38, tanδ ∼ 4.0×10-4, Q×f ∼ 22988 GHz, τf ∼ -58.3 at high frequencies (9~10 GHz). Therefore, this study focuses on (Ca0.6Ba0.01Sr0.39)ZrO3 ceramics, examining the effects of doping with MgO and MgTiO3 in proportions of (Ca0.6-xMgxSr0.39Ba0.01)ZrO3 and (Ca0.6-xMgxSr0.39Ba0.01)(Zr1-xTix)O3 (X=0~0.05) on the density, phase structure, microstructure, and dielectric properties of CSBZ ceramics. H
The results indicate that in MgTiO3-doped ceramics, there is a competitive substitution of Mg²⁺ and Ti⁴⁺ at the B-site. While the addition of MgO significantly enhances the sintering process, it also tends to promote the formation of secondary phases. At a sintering temperature of 1350 °C, the inclusion of 1 mol% MgO and MgTiO3 improves the densification and dielectric properties of (Ca0.6Ba0.01Sr0.39)ZrO3 ceramics. Notably, the introduction of MgTiO3 further reduces the sintering temperature, resulting in (Ca0.59Mg0.01Sr0.39Ba0.01)(Zr0.99Ti0.01)O3 ceramics exhibiting superior dielectric performance at 1250 °C compared to (Ca0.6Ba0.01Sr0.39)ZrO3 sintered at 1350 °C. The dielectric properties at 1250 °C include εᵣ ∼ 35.8, tanδ ∼ 2×10⁻⁴ at 1 MHz, IR ∼ 3.5×10¹³ Ω, and at high frequencies (8–10 GHz), εᵣ ∼ 34.8, Q×f ∼ 19697 GHz, and τf ∼ -25.1 ppm/°C.
Increasing the variety of elements enhances the system's entropy, effectively reducing the sintering temperature of (Ca,Sr,Ba,Mg)(Zr,Ti)O₃ ceramics to 1250 °C, while simultaneously improving their dielectric properties. This study demonstrates that entropy engineering is a powerful approach for tuning the dielectric performance of CSZ-based materials, offering broad application potential and valuable insights for designing new dielectric ceramic materials.

論文審定書 i
誌謝 ii
摘要 iii
Abstract iv
目錄 vi
圖目錄 x
表目錄 xix
第一章 前言 1
1.1 研究背景 1
1.2 研究動機 3
第二章 文獻回顧 5
2.1 積層陶瓷電容 5
2.2 微波介電陶瓷材料 9
2.2.1 微波介電陶瓷的分類 9
2.2.2 評估微波介電陶瓷性能的主要參數 10
2.3 高熵陶瓷材料 12
2.3.1 高熵的定義 12
2.3.2 高熵效應 15
2.3.3 高熵陶瓷的設計 17
2.4 鈣鈦礦結構 20
2.5 M2+ZrO3 (M= Ca,Sr,Ba) 系統介紹 22
2.6 (Ca,Sr)ZrO3系統介紹 23
2.7 (Ca,Sr,Ba)ZrO3系統介紹 25
2.8 (Ca,Sr,Ba)ZrO3系統改質 27
2.8.1 摻雜Mg元素之介電性質介紹 27
2.8.2 摻雜Ti元素之介電性質介紹 28
2.9 缺陷化學 29
2.10 燒結理論 32
2.11 晶粒生長 35
第三章 實驗設計 36
3.1 實驗參數 36
3.1.1 實驗粉末介紹 36
3.1.2 粉末製備 37
3.1.3 陶瓷生胚製備 38
3.1.4 陶瓷燒結體製備及量測 39
3.1.5 燒結參數設定 41
3.1.6 電極固化參數 42
3.2 實驗設備介紹 43
3.2.1 球磨機 43
3.2.2 研磨拋光機 45
3.2.3 油壓式壓力機 46
3.2.4 自然對流烘箱 47
3.2.5 高溫燒結爐 48
3.2.6 噴霧造粒機 49
3.2.7 離子濺鍍機 51
3.3 材料特性分析 52
3.3.1 阿基米德密度分析 52
3.3.2 X光繞射儀 (X-ray diffraction, XRD) 53
3.3.3 場發射型掃描式電子顯微鏡 (Field Emission-Scanning Electron Microscopy, FE-SEM) 55
3.3.4 能量散佈光譜儀(Energy-dispersive X-ray spectroscopy, EDS) 56
3.3.5 介電性質分析 57
3.3.6 電容溫度係數量測(Temperature coefficient of capacitance, TCC) 59
3.3.7 高階三束型聚焦離子束顯微鏡 (Three-beams focused ion beam, TB-FIB) 60
3.3.8 穿透式電子顯微鏡(Transmission electron microscopy, TEM) 61
第四章 結果與討論 62
4.1 改變MgO含量對 Ca0.6-xMgxSr0.39Ba0.01ZrO3陶瓷的影響 62
4.1.1 煆燒CMSBZ陶瓷之相結構分析 62
4.1.2 燒結CMSBZ陶瓷之相結構分析 64
4.1.3 CMSBZ陶瓷之密度分析 68
4.1.4 CMSBZ陶瓷之晶體結構分析 70
4.1.5 CMSBZ陶瓷之顯微結構分析 72
4.1.6 CMSBZ陶瓷之介電性質分析 83
4.1.7 CMSBZ陶瓷之高頻介電性質分析 92
4.2 改變MgTiO3含量對(Ca0.6-xMgxSr0.39Ba0.01)(Zr1-xTix)O3陶瓷的影響 95
4.2.1 煆燒CMSBZT陶瓷之相結構分析 95
4.2.2燒結CMSBZT陶瓷之相結構分析 97
4.2.3 CMSBZT陶瓷之密度分析 101
4.2.4 CMSBZT陶瓷之晶體結構分析 103
4.2.5 CMSBZT陶瓷之顯微結構分析 107
4.2.6 CMSBZT陶瓷之介電性質分析 116
4.2.7 CMSBZT陶瓷之高頻介電性質分析 127
4.3 綜合比較MgO和MgTiO3添加對 CSBZ陶瓷的影響 130
4.3.1 相結構分析 130
4.3.2 二次相分析 132
4.3.3 燒結密度分析 135
4.3.4 顯微結構分析 137
4.3.5 介電性質分析 140
第五章 結論 144
參考文獻 147

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