陰極沉積鎳鈷氫氧化物與擬電容器儲能機制探討

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研究生：	陳家慶
論文名稱：	陰極沉積鎳鈷氫氧化物與擬電容器儲能機制探討 Cathodic Deposition of Nickel Cobalt Hydroxides and the Charge Storage Mechanism of Pseudocapacitors
指導教授：	胡啟章
口試委員:	白育綸張國興胡啟章
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：	2013
畢業學年度：	101
語文別：	英文
論文頁數：	210
中文關鍵詞：	氫氧化鎳、氫氧化鈷、鎳鈷氫氧化物
相關次數：	點閱：1 下載：0
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　本研究在實驗討論的前兩部分主要闡述兩個在超級電容器的應用上基礎但很重要的觀念。其一，擬電容材料的電化學可逆性在能量效率與電容維持率的表現上扮演著關鍵的角色。此部分的實驗，我們也成功地利用陰極沉積法分別合成出高比電容且具有典型材料特性的氫氧化鎳和氫氧化鈷。其二，陽離子效應對氫氧化鎳的相轉變以及循環壽命有著顯著的影響。我們利用電化學石英晶體微天平和其他實驗技術證實陽離子的嵌入/嵌出是氫氧化鎳氧化還原反應的必要步驟。而鋰離子流動性最佳；反之，由拉曼圖譜和掃描式電子顯微鏡的分析發現鉀離子的出入造成阿爾法相(α phase)的不穩定與結構破壞。此外，陽離子效應對氫氧化鎳的電致變色行為以及氧氣還原的催化能力，在長期壽命上的影響，與相轉變和結構破壞具有相當一致的趨勢。本研究的最後一部分則分別探討陰極沉積的不同變因，對於鎳鈷複合氫氧化物的形貌與電容行為表現的影響。最後，我們找出最佳的沉積條件，且發現當複合材料中的鈷鎳元素比為二比一時，鎳鈷複合氫氧化物有最高的比電容同時維持良好的功率特性。經過X光繞射儀(XRD)以及X光能量散射譜(EDS)的分析，最佳沉積條件下合成的鎳鈷複合氫氧化物為Ni0.32Co0.68(OH)2。Ni0.32Co0.68(OH)2 有非常好的功率特性以及循環壽命，且在非對稱超級電容器的測試下，Ni0.32Co0.68(OH)2-GS的能量密度與Ni(OH)2-GS相當，而其能量效率則更加優越，使Ni0.32Co0.68(OH)2在超級電容器的應用上具有非常大的潛力。

Chapter 1 Introduction and Literature Review    1
1 Fundamentals of Electrochemistry    1
1.1 Electrochemical System and Reference Electrodes    1
1.2 Faradaic and Nonfaradaic Processes    6
1.3 Electrochemical Cells and Reaction Rate    6
1.4 Factors Affecting Electrode Reaction Rate and Current    10
1.5 Introduction to Mass-Transfer-Controlled Reactions    11
2 The Principle and Mechanism of Electrochemical Deposition of Transition Metal Oxides    15
3 Introduction of Supercapacitors    20
3.1 Classification of Supercapacitors    24
3.2 Key Factors of Electrode Materials Determining the Performance of Supercapacitors    28
4 Literature Review of Ni(OH)2, Co(OH)2 and Ni(OH)2/Co(OH)2 composites    35
4.1 Literature Review of Ni(OH)2    35
4.2 Literature Review of Co(OH)2    41
4.3 Literature Review of the Composites of Ni(OH)2 and Co(OH)2    43
5 Motive and Purpose    46
Chapter 2 Experimental Methods    48
1 Chemicals and Instruments    48
1.1 Chemicals    48
1.2 Instruments    48
2 Graphite Electrode Preparation and Pretreatment    49
3 Graphene Preparation    50
4 Electrodeposition Process    51
4.1 Three-Electrode System    51
4.2 Controlled-Current Techniques    53
5 Electrochemical Analysis Techniques    56
5.1 Linear Sweep Voltammetry (LSV)    56
5.2 Cyclic Voltammetry (CV)    60
5.3 Current-Reversal Chronopotentiometry (CD)    63
5.4 Electrochemical Quartz Crystal Microbalance (EQCM)    66
6 Textural Analysis    68
6.1 Scanning Electron Microscope (SEM)    68
6.2 Transmission Electron Microscopy (TEM)    69
6.3 X-ray Diffraction (XRD)    71
Chapter 3 Cathodic Deposition of Ni(OH)2 and Co(OH)2 for Asymmetric Supercapacitors    72
1 Introduction and Motive    72
2 Experimental    74
3 Electrochemical and Textural Characteristics of Ni(OH)2 and Co(OH)2 Synthesized by Cathodic Deposition    77
3.1 LSV Investigation    77
3.2 Chronopotentiograms (CPs) Investigation    79
3.3 Morphology and Crystalline Phase    84
3.4 Electrochemical Performance    88
4 The Influences of Electrochemical Reversibility of on the Performances of an Asymmetric Supercapacitor    96
4.1 Electrochemical Reversibility Effects on Charge-Discharge Performance    96
4.2 Electrochemical Reversibility Effects on Energy Efficiency and Ragone Plot    100
5 Conclusion    103
Chapter 4 Electrochemical Quartz Crystal Microbalance Studies of Cation Effect on Phase Transformation and Cycling Retention of Ni(OH)2    104
1 Introduction and Motive    104
2 Experimental    106
3 The Influence of Different Electrolytes on Capacitive Performances of Ni(OH)2    107
3.1 Cyclic Voltammetry Investigation and Crystalline phase    107
3.2 The Effect of Concentration of OH- in Different Electrolytes on Capacitive Performances    111
4 Electrochemical Quartz Crystal Microbalance (EQCM) Investigation of Cation Effect on Phase Transformation and Cyclic Retention    116
4.1 Mass Change during Redox Reactions of Ni(OH)2 in Different Electrolytes    116
4.2 Proposed Mechanism of Ni(OH)2 Redox Reaction and the Followed Theoretical Calculation    127
5 Cation Effect on the Morphology Destruction of Ni(OH)2    133
6 Exhibition of the Importance of Cations on Cycling Retention    139
7 Cation Effects on the Retention of the Capacity of Ni(OH)2    144
8 Conclusion    148
Chapter 5 The influences of different deposition factors on the morphology and the capacitive performance of Ni(OH)2 / Co(OH)2 composites    150
1 Introduction and Motive    150
2 Experimental    152
3 Effects of Deposition Current Density    153
4 Effect of Deposition Time    161
5 Effect of pH Value of Deposition Bath    165
6 Effect of Temperature of Deposition Bath    169
7 Effect of Co2+/Ni2+ Ratio in the Deposition Bath    177
8 Summary of the Effect of Deposition Factors on the Capacitive Performances and Morphology    179
9 Characterization and Exhibition of the Capacitive Performances of Ni0.32Co0.68(OH)2    182
10 Conclusion    191
Chapter 6 Conclusion and Future work    193
References…………………………………………………………..…197

                                

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