經二十餘年的發展，多孔性金屬有機骨架化合物（MOF）或配位聚合物，已成為化學等領域的重要研究平台與工業的潛在應用材料。由於其高孔隙率、較大表面積和可調節的結構等特性，這些具有新穎拓撲結構且性能卓越的MOF逐漸顯現在光電、微電子的應用價值。本論文研究中，我們選取含羧酸基團或含氮配體，合成了鋇、銦、鋅和銅基等新型金屬有機骨架聚合物，並研究了它們的光學、介電和半導體特性。自發光MOF可應用於光學領域，我們合成了一種新型發光的二維鋇基金屬有機骨架{[Ba(2,6-ndc)(H2O)2]•H2O} (1)，該晶體為單斜晶系，空間群為P21/n。化合物1表現出顯著的寬帶白光光譜，於374 nm處激發時，其國際照明（CIE）坐標為（0.32，0.33），低色溫為6113 K，其相應的高顯色指數（CRI）為84。這種白光發射可歸因於化合物1晶體結構內的π–π*堆疊和金屬到配體的電荷轉移機制引起的。此外，我們設計了一種發光二極體，使用Ba-MOF（1）作為活性材料，表現出白色電致激發光譜。這種出色的單成份MOF的白光LED發光材料較為環保、具高熱穩定性與低成本，和使用鑭系元素、過渡金屬的雙成分LED產品相比較，具有顯著優勢。另外，本研究也探討介電MOF的合成與特性，於水熱條件下合成了兩個銦基MOF： Na[In3(odpt)2(OH)2(H2O)2](H2O)4（2）和{[In(btc)(H2O)2]•2H2O}n（3），並研究了它們的高介電性質。化合物2晶體為三斜晶系，空間群為P1 ̅，其中包含三個In3+為中心，四個客體和兩個配位水分子；而化合物3晶體為單斜晶系，空間群為C2/c，具有一個In3+中心與兩個配位水分子，並含有兩個客體水分子。 2的介電研究證實，它具有很高的介電常數（在1 kHz時κ = 40.5），而化合物3表現出更高的介電性質（在1 kHz時κ = 56.3），從而驗證了這兩種化合物都有望使用於新興柵極電介質中。化合物3除去溶劑，當客體和配位的水分子被排除後（化合物3ꞌ），測量觀察到介電值發生了實質變化（45.2），表明水分子對化合物介電性質有很大影響。密度泛函理論（DFT）計算也支持了實驗結果，並且顯示這兩種化合物的介電行為與水分子多寡相關，並具有特異寬能隙。此外，本論文研究還探討了鋅基MOF化合物[Zn(Aip)(Pbim)]n （4）與 [Zn(Nip)(Pbim)]n （5）的合成及其介電性質。化合物4和化合物5的晶體均為單斜晶系，空間群分別為P21/n 和C2/c。介電研究的結果表明，4的介電常數非常高（在1 kHz時κ = 65.5），而化合物5的介電常數更高（在1 kHz時κ = 110.3）。兩種化合物在420 °C的溫度下均具有出色的熱穩定性，這些高熱穩定性使化合物4和5成為高溫應用中高介電的候選材料。我們還合成了一種具有Cu―S籠狀的金屬有機配位化合物[Cu6(mpy)6]n（6），具有獨特槳葉式奈米結構以及半導體性質。通過實驗和理論方法，我們證實這種材料是一種很有前景的0D半導體。實驗量測獲得的能隙為1.9 eV，而計算的能隙為1.8 eV，兩者非常吻合，其能隙大小亦與已知的半導體材料（例如CdSe，CdTe，ZnTe，GaP）相當。該錯合物具有半導體性質的主要原因可以歸因於銅的d軌域與槳輪狀奈米結構中有機配基中的硫原子p軌域之間的較佳混成。這些結果說明金屬有機骨架化合物具有獨特的結構，並顯示有趣的白光、介電與半導體特性。

Over the last two decades, a class of porous materials identified as Metal–Organic Frameworks (MOFs), also known as coordination polymers, have emerged as potential candidates for a wide spectrum of applications in academic and industrial research throughout the world. A larger variety of inorganic and organic components can be used to construct MOFs having novel topologies with exceptional properties. Their versatile features such as porosity, larger surface areas and tunable structural properties make them a desirable family of materials for use in the next-generation opto/ microelectronic applications. In this thesis, we report on the synthesis of barium, indium, zinc and copper-based novel metal–organic frameworks (MOFs) and complexes and the investigation of their optical behavior, dielectric and semiconducting properties. Luminescent MOFs have the potential for being used in optical applications. We synthesized a new luminescent two dimensional barium-based metal–organic framework {[Ba(2,6-ndc)(H2O)2]•H2O} (1), which crystallizes in the monoclinic space group P21/n space group. Compound 1, upon excitation at 374 nm, exhibits remarkable broad band white light emission spectrum with Commission International ed’Eclairage (CIE) coordinates at (0.32, 0.33) and a low color temperature of 6113 K with a corresponding high color rendering index (CRI) of 84. This white light emission can be attributed to ligand-based emission, raised by π–π* stacking and metal to ligand charge transfer mechanisms within the crystal structure of 1. In addition, we designed a light-emitting diode using the Ba-MOF (1) as an active material which exhibited a white electroluminescence spectra. This remarkable single component MOF-based white light LED system represents a significant advancement in two-component LEDs systems that involve the use of lanthanides, transition metals, thus demonstrating the potential of this material for being an environmentally friendly, highly thermally stable and low cost source for solid-state white-light applications.
Furthermore, inspired by examples of low dielectric MOFs, we synthesized two indium-based MOFs Na[In3(odpt)2(OH)2(H2O)2](H2O)4 (2) and {[In(btc)(H2O)2]•2H2O}n (3) under hydrothermal conditions and evaluated their high dielectric properties. Compound 2 crystallized in the triclinic space group (P1 ̅) containing three In3+ centers, four guest and two coordinated water molecules while compound 3 crystallized in the C2/c monoclinic space group with one In3+ center to which two water molecules are attached and also contains two guest water molecules. Dielectric studies of 2 revealed that it has a very high dielectric constant (κ = 40.5 at 1 kHz), while compound 3 exhibited an even higher dielectric constant (κ = 56.3 at 1 kHz) thus confirming that both compounds represent promising candidates for use in gate dielectrics. The dielectric properties of 3 containing solvated guest and coordinated water molecules were also measured after eliminating both guest and coordinated water molecules (3ꞌ) and a substantial change in the dielectric value was observed (45.2). Theoretical results from density functional theory (DFT) calculations, were also consistent with the experimental findings, and showed that both compounds displayed distinct electronic behavior with diverse wide bandgaps, which was associated with the removal of the water molecules. We also investigated the dielectric properties of two solvated molecules free zinc-based MOFs [Zn(Aip)(Pbim)]n (4) and [Zn(Nip)(Pbim)]n (5). Both compound 4 and compound 5 crystallized in the monoclinic space groups P21/n and C2/c, respectively. The results of dielectric studies showed that 4 display a very high dielectric constant (κ = 65.5 at 1 kHz), while compound 5 showed an even higher dielectric constant (κ = 110.3 at 1 kHz). Both compounds were remarkably thermally stable at temperatures in the range of 420 °C. The high thermal stabilities of both compounds 4 and 5 make them appropriate contenders for use as high dielectric constant materials in high temperature applications.
We also highlighted the semiconducting property of a metal–organic complex [Cu6(mpy)6]n (6) having a unique paddle-wheel nanostructure based on a compact Cu–S cage. Using both experimental and theoretical approaches, we were able to demonstrate that properties of this material make it a promising 0D semiconductor. The experimentally obtained bandgap was 1.9 eV. The computed bandgap was 1.8 eV, which is in a good agreement with the measured value. The estimated bandgap size is comparable to those of previously reported semiconducting materials (e.g., CdSe, CdTe, ZnTe, GaP). The main reason for the semiconducting characteristics of this complex can be attributed to the strong hybridization between the d-orbitals of copper and the p-orbitals of organic atoms in the paddle-wheel like nanostructure. These results provide encouragement for more advanced studies of Cu-based metal–organic complexes, which will lead to the fabrication of even more fascinating semiconducting materials in the future.

Contents
摘要 i
Abstract iii
Acknowledgements vi
Contents viii
List of Figures xiii
List of Tables xxiiii
List of Publications xxiii
Chapter 1. Introduction 1
1.1 Background 1
1.2 Design and Self-assembly of Metal–Organic Frameworks 4
1.3 Pre and Post Modification 7
1.4 Applications of MOFs as Luminescent Materials 9
1.4.1 Introduction to Luminescent Materials 9
1.4.2 Luminescent Properties of MOFs 9
1.4.3 White Light Emitting MOFs 17
1.5 Dielectric Properties of MOFs 20
1.5.1 Introduction to Dielectric Materials 20
1.5.2 Applications of MOFs as Dielectric Materials 27
1.6 Semiconducting Properties of MOFs 34
1.6.1 Introduction to Semiconducting Materials 34
1.6.2 Semiconducting MOFs 35
1.7 Research Motivation 38
Chapter 2. Phosphor-Free Barium–Organic Framework as White Light Emitter 39
2.1 Introduction 39
2.2 Experimental Section 40
2.2.1 General Information 40
2.2.2 Synthesis of {[Ba(2,6-ndc)(H2O)2]·H2O} (1) 40
2.2.3 Simulation Details 42
2.3 Results and Discussion 42
2.3.1 Crystal Structure of Ba-based MOF (1) 42
2.3.2 Thermogravimetric Analysis and Powder X-ray Diffraction Studies 45
2.3.3 Photoluminescence Properties 46
2.3.4 Density Functional Theory (DFT) Calculations 50
2.3.5 Device Fabrication 52
2.4 Conclusions 58
Chapter 3. Thermally Stable High-Dielectric In-based MOFs 59
3.1 Introduction 59
3.2 Experimental Section 60
3.2.1 General Information 60
3.2.2 Synthesis of Na[In3(odpt)2(OH)2(H2O)2](H2O)4 (2) 61
3.2.3 Synthesis of {[In(btc)(H2O)2]·2H2O}n (3) 62
3.2.4 Computational Details of DFT Study 63
3.3 Results and Discussion 64
3.3.1 Crystal Structures of Compound 2 64
3.3.2 Crystal Structures of Compound 3 68
3.3.3 Powder X-ray Diffraction and Thermogravimetric Analysis 72
3.3.4 Dielectric Properties 75
3.3.5 Electrical Conductivity and Impedance Studies 80
3.3.6 Electronic Structures by Theoretical DFT Study 81
3.3.7 Diffuse Reflection Studies 85
3.4 Conclusions 86
Chapter 4. Guest Free High Dielectric Zinc-based Metal–Organic Frameworks 88
4.1 Introduction 88
4.2 Experimental Section 90
4.2.1 General Information 90
4.2.2 Synthesis of [Zn(Aip)(Pbim)]n (4) 90
4.2.3 Synthesis of [Zn(Nip)(Pbim)]n (5) 91
4.3 Results and Discussion 91
4.3.1 Synthesis of Compounds 4 and 5 91
4.3.2 Crystal Structure of Compound 4 92
4.3.3 Crystal Structure of Compound 5 96
4.3.4 Powder X-ray Diffraction and Thermogravimetric Analysis 99
4.3.5 Dielectric Investigation 100
4.3.6 Electrical Conductivity and Impedance Studies 104
4.4 Conclusion 105
Chapter 5. Cu-Based Metal–Organic Complex as a Semiconductor 106
5.1 Introduction 106
5.2 Experimental Section 107
5.2.1 General Information 107
5.2.2 Synthesis of [Cu6 (mpy)6]n (6) 108
5.2.3 Computational Details of DFT Study 108
5.3 Results and Discussion 108
5.3.1 Crystal Structure of Compound 6 109
5.3.2 Powder X-ray Diffraction and Thermogravimetric Analysis 111
5.3.3 Electrical Characterization 112
5.3.4 Electrochemical Measurements 114
5.3.5 Diffuse Reflectance Spectrum 116
5.3.6 Theoretical DFT Study 117
5.4 Conclusion 119
Chapter 6. Conclusion 120
References 123
Addendum I: Crystal Data and Structure Refinement 155

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