活性碳纖維應用於超級電容器電極高溫處理對電化學性質之研究

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研究生：	呂國維 Kuo-Wei Lu
論文名稱：	活性碳纖維應用於超級電容器電極高溫處理對電化學性質之研究 Investigation of Carbon Fiber Applied to Supercapacitor Electrode and Electrochemical Properties
指導教授：	吳昌謀 Chang-Mou Wu
口試委員:	蘇清淵 Ching-Iuan Su 陳幹男 Kan-Nan Chen 邱顯堂 Hsien-Tang Chiu 李貴琪 Kuei-Chi Lee 邱智瑋 Chih-Wei Chiu
學位類別：	博士 Doctor
系所名稱：	工程學院 - 材料科學與工程系 Department of Materials Science and Engineering
論文出版年：	2017
畢業學年度：	106
語文別：	英文
論文頁數：	123
中文關鍵詞：	活性碳纖維、超級電容電極、電化學性質
外文關鍵詞：	Supercapacitor, Activated carbon fiber, Electronic conductivity
相關次數：	點閱：313 下載：0
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本研究首先以嫘縈梭織布作為活性碳纖維原料，研究中以直立連續半開放式高溫爐，並以水蒸氣為活化源，經過氧化、碳化及活化工程，製造出活性碳纖維布，此研究中使用固定水蒸氣活化源供給量，但改變喂布速率，以及固定喂布速率，變化水蒸氣活化源供給量，並觀察活性碳纖維在1000oC下進行碳化及活化過程，結果顯示在不同製備條件的活性碳纖維布具有不同的比表面積和孔洞結構，並藉由三極式電化學反應系統，觀察活性碳纖維電極應用於超級電容器的電容性質。在製備活性碳纖維布過程中，發現降低喂布速率，可增加比表面積，並使活性碳纖維布具有較高之電容儲存量。當水蒸氣供給量增加時，可使活性碳纖維的比表面積及中孔百分率提高，電阻值下降。活化源供給量160 ml/min時，所製備的活性碳纖維布，其比表面積達2332.1 m2/g，中孔比率78.7%，在較慢的掃描速率(5mV/s)時，可得到電容值430.4 F/g，在快速充放電(100mV/s)下仍可保留60%的電容值。另一方面則以聚丙烯腈作為奈米纖維膜原料，經由兩段連續式氧化與1000oC碳化、活化工程，製造出奈米活性纖維膜後，在各溫度條件進行熱處理加工後，進而探討經入熱處理後的奈米活性碳纖維膜樣品放電速率的電容保留率，研究結果顯示熱處理溫度對奈米活性碳纖維膜特性有明顯的影響，且在超級電容器電極中可觀察放電速率對電容保留率的多寡。

This study uses rayon woven fabrics as the raw material for activated carbon fabrics, which were manufactured by oxidation, carbonization and activation engineering in a continuous semi-open high-temperature furnace. First, the activated carbon fabrics are prepared under two specific manufacturing conditions with different production rates and flow rates of steam activation at 1000 oC. Then the electrochemical prosperities of the activated carbon fabrics are evaluated by a threeelectrode device. The experimental results show that the BET specific surface area and electrical capacitance are higher with a lower production rate. Moreover, the steam activator higher flow rate under the proposed approach. Activated carbon fabrics with a 2332.1 m2/g specific surface area and 78.7 % mesopore ratio result in a higher electronic conductivity of 430.4 F/g at the low rate charge (5 mV/s) and with 60 % capacitance retention during the high-speed charging-discharging process (100 mV/s). On the other hand, polyacrylonitrile was used as the nanofiber membrane material. Through A two-stage continuous process, namely, oxidation process and carbonization and activation process, an activated nanofiber membrane material was fabricated. Subsequently, the membrane underwent high-temperature heat treatment (1100-1500 oC) to explore the effect of temperature on its properties. Charge/discharge rate was employed to determine the capacitance retention ratio to evaluate the applicability of the fabricated membrane in high-power super capacitor electrodes. The results revealed that in the treated membrane, the lattice size increased from 1.24 nm to between 3.20 and 4.72 nm. In addition, the volume resistivity was reduced from 6 Ω-cm to between 9.70E-2 and 3.85E-2 Ω-cm, substantially improving the electric conductivity. The activated carbon nanofiber membrane treated with high temperature at 1100 oC exhibited the highest capacitance of 704 F/g at a scan rate of 5 mV/s.

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博士學位考試委員審定書
摘要  I
Abstract   Ⅲ
致謝   V
Table of Contents    VI
List of Tables   IX
List of Figures   X
Chapter 1 Prolegomenon    1
1.1 Indtroduction    1
1.2 The Supercapacitors Technique    7
1.3 Electrochemical Double-layer Capacitors    10
1.4 Introduction to Activated Carbons Materials    12
1.5 Formation of Pore Structure    13
1.6 Adsorption Mechanism    15
1.6.1 Adsorption Mechanism of Silver Ion onActivated Carbon    15
1.6.2 Ion Exchange Adsorption    16
1.6.3 Reduction Adsorption of Silver Ions    17
1.6.4 Adsorption of Bacterium on Activated Carbon    21
1.6.5 Adsorbing Mechanism of Modified Absorbent    22
References    25
Chapter 2 Evaluation of Activated Carbon Fiber Applied in Supercapacitor Electrodes    29
Abstract    29
2.1 Introduction    30
2.2 Experimental    34
2.3 Results and discussion    38
2.3.1 Weight Yield    38
2.3.2 Nitrogen Absorption Isotherms with ACFs at 77ok    41
2.3.3 BET Surface Area and Pore Characteristics    44
2.3.4 Cycle Voltammograms    46
2.3.5 Capacitance Value of Cycle Voltammograms    51
2.3.6 Analysis of Electrochemical Impedance Spectroscopy    54
2.4 Conclusions    61
References    62
Chapter 3 Effect of High Temperature Treatment on Electrochemical Properties of CarbonNanofiber Membrane    64
Abstract    64
3.1 Introduction    65
3.2 Experimental    70
3.2.1 Nanaofiber Membrane Preparation    71
3.2.2 Oxidation    72
3.2.3 Carbonization and Activation    73
3.2.4 High-temperature Heat Treatment    74
3.2.5 Material Characteristic Analysis    76
3.2.5.1 X-ray Diffraction Analysis    76
3.2.5.2 Resistivity Analysis    77
3.2.5.3 Electrochemical Property Analysis    78
3.2.5.4 Cyclic Voltammetry    79
3.2.5.5 Electrochemical Impedance Spectroscopy    80
3.3 Results and Discussion    81
3.3.1 X-ray Diffraction Analysis    82
3.3.2 Analysis of the Activated Carbon Nanofiber Membrane Conductivity    85
3.3.3 Electrochemical Impedance Spectroscopy    88
3.3.4 Cyclic Voltammetry Curve    93
3.3.5 Capacitance Analysis of Cyclic Voltammetry    102
3.4 Conclusions    105
References    106
作  者  簡  歷    109
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