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研究生： 傅上媛
Fu, Shang-Yuan
論文名稱： 三維混價銅金屬有機框架作為鋰離子電池之陰極材料
Three-dimensional Mixed-valence Cu-based Metal-organic Frameworks as Cathode Materials for Li-ion Batteries
指導教授： 柯碧蓮
Watchareeya Kaveevivitchai
學位類別： 碩士
Master
系所名稱： 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年： 2021
畢業學年度： 109
語文別： 英文
論文頁數： 101
中文關鍵詞： 三維 、混價銅 、金屬有機框架 、鋰離子電池 、陰極材料
外文關鍵詞： Three-dimension, Mixed-valence copper, Metal-organic frameworks, Li-ion batteries, Cathode materials
相關次數： 點閱：189  下載：0 
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    • 為確保綠色環境和乾淨空氣，發展替代性可再生能源技術越來越備受矚目。鋰離子電池（LIBs）被認為是最有前途的儲能係統之一，但商業鋰離子電池的能量和功率密度仍有待提高，以用於電動汽車和電網儲能的發展。我們研究的目標是設計用於永續能源存儲的先進功能金屬有機框架 (MOF)。這些材料可用於電極材料並同時使用金屬和有機部分的氧化還原化學，從而產生高比容量。在這項研究中，有機配體1,4-二氰基-2,3,5,6-四羥基苯(LH4)與銅離子反應形成三維 (3D) 混價銅 CuI/CuIII MOF NCKU-52。混價材料已被廣泛研究用於許多進階應用中，但 CuI/CuIII 混合物是前所未有的。NCKU-52還填充有N,N-二甲基甲酰胺 (DMF) 分子和 Cu(iq)3 複合物（iq =異喹啉），分別得到 NCKU-52-DMF 和 NCKU-52·Cu(iq)3。這些材料被應用於鋰離子電池的陰極，並表現出出色的能量和功率密度以及倍率性能。在 200 mA g–1 的速率下，NCKU-52、NCKU-52-DMF 和 NCKU-52·Cu(iq)3 的初始容量分別為 350、300 和 290 mAh g–1。此外，儘管循環速率增加，但這些材料的容量仍能穩定在約150 mAh g–1。這些材料在放電/充電過程中的氧化還原機制可以通過各種表徵技術來闡明，例如傅里葉變換紅外光譜(FT-IR)、X射線光電子能譜 (XPS)、X射線吸收光譜 (XAS) 和高分辨率透射電子顯微鏡(HR-TEM)。這項工作提出了一種獨特的混合價MOF作為鋰離子電池的新型陰極材料，並為下一代鋰離子電池的開發奠定基礎。

    To ensure a green environment and clean air, the development of alternative renewable energy technology must be the top priority. Li-ion batteries (LIBs) are considered as one of the most promising energy storage systems, however, the energy and power density of commercial LIBs still need to be improved for the development of electric cars and grid energy storage. The goal of our research is to design advanced functional metal-organic frameworks (MOFs) for sustainable energy storage. These materials can serve as electrode materials and allow the use of redox chemistry of both metal and organic moieties, which will give rise to a high specific capacity. In this study, the organic ligand 1,4-dicyano-2,3,5,6-tetrahydroxybenzene (LH4) reacts with copper ions to form a three-dimensional (3D) CuI/CuIII mixed-valence MOF NCKU-52. Mixed-valence materials have been widely studied for many advanced applications, but the CuI/CuIII mixture is unprecedented. NCKU-52 is also filled with N,N-dimethylformamide (DMF) molecules and Cu(iq)3 complex (iq = isoquinoline) to afford NCKU-52-DMF and NCKU-52·Cu(iq)3, respectively. These materials are applied as cathode materials for LIBs and exhibit outstanding energy, power density, and rate capability. At rates of 200 mA g–1, NCKU-52, NCKU-52-DMF, and NCKU-52·Cu(iq)3 can perform initial capacities about 350, 300, and 290 mAh g–1, respectively. In addition, the capacities of these materials stabilize at about 150 mAh g–1 despite increasing cycling rates. The redox mechanisms of these materials during discharge/charge processes are elucidated by various characterization techniques such as Fourier-transform infrared (FT-IR) spectra, X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and high-resolution transmission electron microscopy (HR-TEM). This work presents a unique mixed-valence MOF as novel cathode material for LIBs and sheds light on the development of next-generation LIBs.

    摘要 I Abstract II Acknowledgments IV Table of Contents V List of Figures VIII List of Tables XVI Chapter 1 1 Introduction 1 1.1 Coordination Polymers and Metal-organic Frameworks 2 1.2 The Elucidation and Evaluation of CuIII Materials 4 1.2.1 The XPS Characterization of CuIII 4 1.2.2 The XAS Characterization of CuIII 6 1.3 Mixed-valence MOF Materials 10 1.4 General Studies of Li-ion Batteries 10 1.4.1 Energy Storage 10 1.4.2 Definitions 12 1.4.3 Battery Design 15 1.4.4 Intercalation Chemistry 17 1.4.5 Quinone-based Materials in Li-ion Batteries 18 1.5 Literature Review 20 1.5.1 Examples of Cu-based MOFs in Li-ion Batteries 21 1.5.2 Comparison of 2D and 3D MOFs as Cathode in Li-ion Batteries 25 Chapter 2 30 Three-dimensional Mixed-valence Cu-based Metal-organic Frameworks as Cathode Materials for Li-ion Batteries 30 2.1 Introduction 30 2.2 Experimental Section 31 2.2.1 Materials 31 2.2.2 Synthesis of 3D Mixed-valence Cu-based Metal-organic Framework 32 2.2.3 Preparation of NCKU-52 Cells 34 2.2.4 Materials Characterization 36 2.2.5 Ex-situ and In-situ Electrochemical Studies 37 2.3 Results and Discussion 38 2.3.1 Structure of 3D Metal-Organic Frameworks 38 2.3.2 Materials Characterization 42 2.3.3 Electrochemical Investigation 48 2.3.4 Mechanistic Investigation 57 2.3.4.1 Dissolution Test 57 2.3.4.2 Ex-situ XRD Measurements 58 2.3.4.3 Ex-situ FT-IR Measurements 60 2.3.4.4 Ex-situ XPS Measurements 63 2.3.4.5 Ex-situ and In-situ XANES Measurements 74 2.3.4.6 HR-TEM Measurements 81 Chapter 3 84 Conclusions 84 References 86

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