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研究生： 廖奕智
Liao, Yi-Chih
論文名稱： 具有高容量及開放結構之正極材料用於以鋅為基礎之儲能裝置
High-Capacity Open Framework Cathode for Zinc-Based Energy Storage Systems
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： 2019
畢業學年度： 107
語文別： 英文
論文頁數： 60
中文關鍵詞： 大規模儲能系統 、鋅離子電池 、普魯士藍相似物 、正極 、陰極
外文關鍵詞： large-scale energy storage systems, zinc-ion batteries, Prussian blue analogue, zinc-ion cathode materials
相關次數： 點閱：69  下載：0 
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    • 長久以來，可重複使用且可充電式之鋅離子電池的開發困難重重，特別是
    在非水溶液電解質方面更是如此。本實驗著重於鋅離子電池的正極（陰極）材料開發，並以應用於大型儲能設備為首要標的。
    本研究以普魯士藍相似物Na1.2Mn[Fe(CN)6]0.8 （NaMnFe-PB）作為鋅離子電池的陰極材料，在本研究中，感應耦合電漿、熱重分析儀及元素分析儀被用來測定樣品的化學式及其所含水重；X 光射線繞射儀及掃瞄、穿透電子顯微鏡則提供了樣品之形貌及結晶性之探討；充放電過程中晶格及過渡金屬氧化態之變化則透過非原位(ex-situ)之X 光射線繞射儀及X 光射線吸收光譜進行分析。
    本實驗所用之鋅離子電池組成成分為：鋅金屬負極、Zn(CF3SO3)2 於 1:4 比例之propylene carbonate (PC)/dimethylsulfoxide (DMSO) 為電解液以及NaMnFe-PB 為正極材料，此電池之工作電壓約在1.45 伏特且於30 mA g-1 之電流密度下其放電電容量可達90 mAh g-1。此外，本電池即便在高如820 mA g-1（9 C）之電流密度下仍可得到良好的電容量（56 mAh g-1），更使得其更接近實際市場應用。
    以地殼含量多且便宜的鋅金屬作為負極、容易合成且對環境友善的普魯士藍相似物作為正極，本研究提供了未來以鋅電池為方向之大型儲能系統之研究基礎且方向。

    The development of rechargeable zinc-ion batteries with good electrochemical performance for non-aqueous systems is a great challenge. This work demonstrates an organic-based rechargeable zinc-ion battery using a Prussian blue analogue (PBA) sodium manganese hexacyanoferrate, Na1.2Mn[Fe(CN)6]0.8 (NaMnFe-PB), as the cathode material.
    Inductively coupled plasma mass spectrometry, thermogravimetric analysis, and elemental analysis were used to determine the precise chemical formula and water content of the prepared sample. Powder X-ray diffraction, synchrotron X-ray diffraction, scanning electron microscopy, and transmission electron microscopy were used to identify the compound, describe the morphology, and prove the crystallinity. The changes of unit cell and of
    oxidation states of the transition metals, Mn and Fe, during charge/discharge were investigated by ex-situ PXRD and ex-situ synchrotron X-ray absorption near-edge structure.
    Cells, composed of zinc metal anode, Zn(CF3SO3)2 in 1:4 propylene carbonate (PC)/dimethylsulfoxide (DMSO) electrolyte and NaMnFe-PB cathode, exhibited a discharge
    plateau of ~1.45 V with a specific discharge capacity of about 90 mAh g-1 at 30 mA g-1. The cells also showed excellent rate capability with a satisfying 56 mAh g-1 discharge capacity at a high current density of 820 mA g-1 (9 C). The combination of an easily-synthesized and environmentally benign PBA cathode, with an affordable and non-toxic zinc anode provides new promising perspective to develop rechargeable zinc-ion batteries for applications in
    large-scale energy storage systems.

    摘要 I Abstract II Acknowledgments III Contents IV List of Tables VI List of Figures VII Chapter 1. Introduction and Research Motivation 1 1.1 Introduction 1 1.2 Motivation and Purpose 6 Chapter 2. General Background and Literature Review 8 2.1 Brief Introduction to Batteries 8 2.1.1 Definitions 8 2.1.2 Intercalation Chemistry 9 2.1.3 Battery Design 10 2.2 PBAs Cathode Materials for Non-aqueous SIBs 11 2.3 Cathode Materials for ZIBs 17 2.3.1 Mn-Based Cathodes 17 2.3.2 V-Based Cathodes 19 2.4 PBA Cathodes for ZIBs 20 2.4.1 Aqueous Electrolyte 20 2.4.2 Non-aqueous Electrolyte 21 Chapter 3. Experimental Section 24 3.1 Materials 24 3.2 Preparation of Sodium Manganese Hexacyanoferrate (NaMnFe-PB) 24 3.3 Preparation of NaMnFe-PB cell 25 3.4 Materials Characterization 26 3.4.1 Powder X-ray Diffraction (PXRD) 26 3.4.2 Synchrotron Powder X-ray Diffraction 26 3.4.3 Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) 27 3.4.4 Thermogravimetric Analysis (TGA) and Elemental Analysis (EA) 27 3.4.5 Raman Spectroscopy and Fourier-Transform Infrared Spectroscopy (FT-IR) 27 3.4.6 Scanning Electron Microscope (SEM) 28 3.4.7 High-Resolution Transmission Electron Microscopy (HR-TEM) 28 3.4.8 Ex-situ Synchrotron X-ray Absorption Near-Edge Structures (Ex-situ XANES) and Ex-situ Powder X-ray Diffraction (Ex-situ PXRD) 28 Chapter 4. Results and Discussion 29 4.1 Synthesis and Materials Characterization 29 4.1.1 Synthesis 29 4.1.2 Materials Characterization 29 4.2 Electrochemical Investigation 35 4.3 Ex-situ XRD Measurements 41 4.4 Ex-situ XANES Measurements 43 Chapter 5. Conclusions 45 Chapter 6. References 46

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