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研究生：	黃景政 Huang, Ching-Cheng
論文名稱：	超低溫共燒陶瓷鈷-釩酸鹽系統微波介電特性與化學鍵特性之關聯性分析 Analysis of the Correlation Between Microwave Dielectric Properties and Chemical Bond Characteristics in Ultra-Low Temperature Co-Fired Cobalt-Vanadate Ceramic Systems
指導教授：	黃正亮 Huang, Cheng-Liang
學位類別：	博士 Doctor
系所名稱：	電機資訊學院 - 電機工程學系 Department of Electrical Engineering
論文出版年：	2025
畢業學年度：	113
語文別：	英文
論文頁數：	129
中文關鍵詞：	LTCCs 、ULTCCs 、微波介電特性、CoV2O6 、Co2V2O7 、P-V-L bond theory 、5G/6G 通訊系統
外文關鍵詞：	LTCCs, ULTCCs, Microwave dielectric properties, CoV2O6, Co2V2O7, P-V-L bond theory, 5G/6G Communication Systems
相關次數：	點閱：12 下載：0
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本研究旨在開發新型超低溫與低溫共燒微波介電陶瓷，以應對科技的快速進步，為高速通信應用提供創新的材料選擇，同時響應全球節能減碳的趨勢。第一部分探討微波介電陶瓷在科技發展與可持續發展中的角色與演變;第二部分介紹開發微波介電陶瓷的理論基礎，接下來的第三與第四部分則分別研究 CoO-V2O5 系統中的兩種基本組成——CoV2O6 和 Co2V2O7 陶瓷的微波介電特性與化學鍵之間的關係。這些陶瓷採用傳統固態法合成，其微波介電特性首次得到系統性的研究。
CoV2O6 陶瓷在 660°C 燒結時呈現 γ 相並且呈現最高的緻密性與最佳的微波介電特性:εr = 11.6、Q×f = 39,177 GHz、τf = -15 ppm/°C，但在 690 °C 發生相變化，從 γ 相轉變為 α 相，導致介電性能下降。Co2V2O7 陶瓷在 720 °C 呈現最高的晶粒緻密性並表現出最優異的介電性能:εr = 9.4、Q×f = 88,645 GHz、τf = -37 ppm/°C。值得注意的是，Co2V2O7 陶瓷的燒結溫度可降低至 660°C，且仍能保持良好的微波介電性能: εr = 7.7、Q×f = 75,887 GHz、τf = -58 ppm/°C。
本研究利用拉曼光譜與P-V-L 鍵理論分析微波介電特性與化學鍵特性之間的關係。研究結果顯示相同的在兩種陶瓷的晶格中 V–O 鍵可為主要晶格震動的代表，顯示 V–O 鍵的含量起到對極化率的關鍵影響。另外，對 CoV2O6 陶瓷以及 Co2V2O7 陶瓷而言，在不同的燒結溫度下，其各自的化學鍵特性的變化量相當微小，與其各自的外在因素相比其影響可以忽略。然而，當晶格結構改變以及化學鍵的比例改變時，化學鍵的特性對微波介電的影響則相當顯著。Co2V2O7 的低介電損耗源於 Co–O 鍵提供的較高晶格能;相較之下，CoV2O6 的燒結溫度較低，這是因為其較高的 V2O5 含量起到了有效燒結助劑的作用。
這兩種陶瓷均與鋁具有良好的化學相容性，成為低溫共燒陶瓷(LTCCs)和超低溫共燒陶瓷(ULTCCs)應用的潛力候選材料。它們適用於工作於微波頻率及更高頻率的器件，為可持續發展與先進通信技術做出重要貢獻。

This study aims to develop novel ultra-low-temperature and low-temperature co-fired microwave dielectric ceramics to address the rapid advancements in technology. These ceramics provide innovative material options for high-speed communication applications while aligning with global energy-saving and carbon-reduction trends. The first section explores the role and evolution of microwave dielectric ceramics in technological and sustainable development. The second section introduces the theoretical foundations for developing microwave dielectric ceramics. The third and fourth sections focus on the relationship between the microwave dielectric properties and chemical bonding characteristics of two fundamental compositions in the CoO-V2O5 system: CoV2O6 and Co2V2O7. These ceramics were synthesized using the traditional solid-state method, and their microwave dielectric properties were systematically investigated for the first time.
CoV2O6 ceramics exhibit the γ-phase when sintered at 660°C, achieving the highest densification and optimal microwave dielectric properties (εr = 11.6, Q×f = 39,177 GHz, τf = -15 ppm/°C). However, at 690°C, a phase transition occurs from the γ-phase to the α- phase, leading to a deterioration in dielectric properties. Co2V2O7 ceramics achieve maximum grain densification and excellent dielectric properties at 720°C (εr = 9.4, Q×f = 88,645 GHz, τf = -37 ppm/°C). Notably, the sintering temperature of Co2V2O7 ceramics can be lowered to 660°C while still preserving excellent microwave dielectric properties (εr = 7.7, Q×f = 75,887 GHz, τf = -58 ppm/°C).
The relationship between microwave dielectric properties and chemical bonding characteristics was analyzed using P-V-L bond theory and Raman spectroscopy. The results reveal that the V–O bond, present in the lattices of both types of ceramics, is representative of the primary lattice vibrations and plays a critical role in influencing polarizability. Moreover, for both CoV2O6 and Co2V2O7 ceramics, the changes in chemical bond characteristics at different sintering temperatures are relatively minor and negligible compared to the effects of external factors. However, when the lattice structure and the proportions of chemical bonds change, the impact of chemical bond characteristics on microwave dielectric properties becomes significant. The low dielectric loss of Co2V2O7 ceramics is attributed to the higher lattice energy provided by the Co–O bond. In contrast, CoV2O6 ceramics exhibit a lower sintering temperature due to the higher V2O5 content.
Both ceramics exhibit excellent chemical compatibility with aluminum, making them promising candidates for applications in low-temperature co-fired ceramics (LTCCs) and ultra-low-temperature co-fired ceramics (ULTCCs). These materials are suitable for devices operating in microwave frequencies and beyond, contributing significantly to sustainable development and advanced communication technologies.

摘要 I 
Abstract III 
致謝 VI 
Contents VII 
Table Captions IX 
Figure Captions X 
List o.f Symbols XIII 
Chapter 1 Introduction 16
1 Microwave Dielectric Properties and Applications of ULTCCs and LTCCs 18
2 Development of Cobalt Vanadate System. 20 
Chapter 2. Theory 23 
1 Microwave Dielectric Properties of Composites 23
1.1 Permittivity (εr) 23
1.2 Quality factor (Q) 28
1.3 Temperature coefficient of resonant frequency (τf) 32
1.4 Factors Influencing Dielectric Loss 33
1.5 Molecular Vibrational Modes and Ramanspectra 41
2 Sintering 43
2.1 Solid State Sintering 44
2.2 Liquid Phase Sintering 45
2.3 Sintering Stages and Grain Growth 47
3 Dielectric Resonator 49
4 P-V-L Theory 53
4.1 Bond Ionicity 54
4.2 Lattice Energy 55
4.2 Bond Energy 57 
Chapter 3. Experimental Procedures 57 
1 Preparation of Materials 58
1.1 Powder Preparation and Compound Synthesis 58
1.2 Bulk Preparation 58
1.3 Bulk Sintering 59
2 Measurement and Analysis 60 
2.1 X-ray Analysis and Refinement of Lattice Parameters 60 
2.2 SEM Analysis and Grain Size Distribution Measurement 60 
2.3 Raman SpectroscopyAnalysis 63 
2.4 Density Measurement 64 
2.5 Measurement of Microwave Dielectric Properties 64 
Chapter 4. Development of Microwave Dielectric Materials for ULTCC Applications 68
1 Microwave Dielectric Properties of CoV2O6 Ultra-Low Temperature Co-fired Ceramic (ULTCC) Materials 68
2 Microwave Dielectric Properties of Co2V2O7 Ultra-Low Temperature Co-fired Ceramic (ULTCC) Materials 80
3 Bond Valence Analysis of CoV2O6 and Co2V2O7 93
4 Correlation between Chemical Bond Characteristics and Microwave Dielectric Properties of the Cobalt Vanadate System 96
5 Chemical Compatibility of CoV2O6 and Co2V2O7 Ceramics 110
5.1 CoV2O6 Ceramic Chemical Compatibility with Al 110 
5.2 Co2V2O7 Ceramic Chemical Compatibility with Al 112 
Chapter 5. Conclusion 114 
Chapter 6. Future Work 117 
References 118
                                    

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