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研究生： 張逸群
Chang, I-Chun
論文名稱： 簡易製備銅及氧化銅奈米材料應用於能源儲存元件
Facile Synthesis of Copper and Copper Oxide Nanomaterials for the Applications in Energy Storage Devices
指導教授： 李紫原
Lee, Chi-Young
口試委員: 徐文光
黃暄益
裘性天
陳金銘
學位類別： 博士
Doctor
系所名稱： 工學院 - 材料科學工程學系
Materials Science and Engineering
論文出版年： 2014
畢業學年度： 102
語文別： 英文
論文頁數： 93
中文關鍵詞： 氧化亞銅 、鋰離子電池 、電解液 、奈米銅帶 、氫氧化鎳 、膺電容
外文關鍵詞： Cuprous oxide, Li-ion battery, Electrolyte, Copper nanobelts, Nickel hydroxide, Pseudocapacitor
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    • 本本工作是關於理想的儲能裝置內部電極的開發，我嘗試去找出便宜、製成簡易並且高性能的材料。在進來的研究中，鋰離子電池(Li-ion batteries)和超級電容器(supercapacitor)是兩種最重要的儲能裝置。鋰離子電池表現出高能量(specific energy)而超級電容器表現出高功率(specific power)。金屬銅及氧化亞銅(cuprous oxide)在此被選為研究對象由於產量豐富、價格便宜且容易製備。在鋰離子電池陽極材料的開發，我運用一個快速且簡易並在低溫下進行化學還原法並控制其及時成核的數目(in-situ nucleation)來制備小於100奈米的氧化亞銅方塊(nanocube)並能控制其大小。其中，邊長為80奈米的樣品表現出優良的鋰離子電池表現。而在超級電容器電極材料的開發，我利用兩次鋁金屬(aluminum)的自發性氧化反應在碳電極上成長出具核殼結構的銅-氫氧化鎳奈米帶(Cu@Ni(OH)2 nanobelts)，利用核心奈米銅帶的導電性和結構作為集電器(current collector)來提供快速導電。這樣的核殼奈米帶展現出極高的贋電容值(pseudocapacitance)並維持高速充放電的特性(rate capability)。這兩個工作都成功的發展出次世代儲能裝置可能的電極材料，同時具有高能量和高功率的特性。

    The focus of my work is to find the possibility of synthesizing cheap materials by simple approaches for high performance energy storage devices. Li-ion batteries and electrochemical capacitor are considered two important future energy storage systems. Copper and cuprous oxide is chosen as electrode materials for accomplishing this purpose and synthesized by simple and cost-effective approaches. In developing Li-ion battery anode material, uniform and monodispersed with tunable sized Cu2O nanocubes were synthesized by a low-temperature in-situ nucleation aqueous chemical reduction. The nanocubes with an edge length of approximately 80 nm used as an anode exhibit excellent lithium storage behavior. In the development of electrochemical capacitor electrode, Cu@Ni(OH)2 nanobelts were fabricated by two aluminum-driven spontaneous electrochemical depositing on carbon/aluminum electrodes. The CuNB acts as a three dimension nanosized current collector for fast electron transport. The Cu@Ni(OH)2 NBs function as pseudocapacitive electrodes, which exhibit a high specific capacitance and a remarkable rate performance. Both of these two studies show a possible electrode material for next generation high-energy and high-power energy storage devices.

    ABSTRACT i ABSTRACT (in Chinese) ii Table of Contents iii List of Tables vii List of Figure Captions viii Chapter 1 Introduction 1 Chapter 2 Literature Review 5 2.1 Li-ion batteries 6 2.1.1 Three type of anode materials base on Li ion insertion and exertion 9 2.1.2 Copper oxide as anode in LIB 11 2.2 Synthesis of Cu2O nanostructrue 13 2.2.1 Polyol method 13 2.2.2 Electrochemical deposition 14 2.1.3.4 Aqueous chemical reduction 15 2.3 Electrochemical capacitors 17 2.3.1 Electrostatic capacitors (EDLC) 18 2.3.2 Pseudocapacitors (FC) 19 2.3.3 Metal oxide and hydroxide as electrode for FCs 20 2.4 Synthesis of Ni(OH)2 nanostructure 21 2.4.1 Chemical method 22 2.4.2 Electrochemical deposition 23 2.5 Improvement in performance of LIBs and FCs 24 2.5.1 Nanostructured materials 24 2.5.2 Current collector 25 Chapter 3 Large-scale Synthesis of Uniform Cu2O Nanocubes with Tunable Sizes by In-situ Nucleation and Its Li-ion Storage Properties 27 3.1 Abstract 27 3.2 Introduction and motivation 28 3.3 Method 30 3.3.1 The detailed procedure of Cu2O nanocube synthesis 30 3.3.2 Spectroscopic characterizations 31 3.3.3 Electrochemical evaluation 31 3.4 Characterizations 33 3.5 Li-ion storage properties 38 3.5.1 The effect of electrolyte on Li-ion storage 38 3.5.2 The effect of Size on Li-ion storage 45 3.6 Summary 48 Chapter 4 Self-powered Electrochemical Deposition of Cu@Ni(OH)2 and Cu@CoxNi1-x(OH)2 Nanobelts for High Performance Pseudocapacitors 49 4.1 Abstract 49 4.2 Introduction and motivation 50 4.3 Method 53 4.3.1 Chemicals 53 4.3.2 Preparation of carbon/aluminum substrate 53 4.3.3 Preparation of Cu@Ni(OH)2 nanobelts 53 4.3.4 Material characterizations 54 4.3.5 Electrochemical evaluation 55 4.4 Morphological studies of Cu@Ni(OH)2 nanobelts 56 4.5 Pseudocapacitance of Cu@Ni(OH)2 nanobelts 63 4.6 Pseudocapacitance of Cu@ CoxNi1-x(OH)2 nanobelts 70 4.7 Summary 73 Chapter 5 Conclusions 74 5.1 Conclusion of this study 74 Appendix – Growth of Cu Nanobelts on Copper Foil and Its Potential Applications 76 A.1 The effect of each ions in the growth solution 77 A.1.1 The effect of chloride 77 A.1.2 The concentration of CTAC and nitric acid 78 A.1.3 Brief summary 80 A.2 Growth of Cu nanobelts on copper foil 81 A.2.1 Galvanic deposition on Cu foil 81 A.2.2 Electrodeposition of CuNBs on Cu foil 82 Reference 84 Publication List 92

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