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研究生： 李書蘋
Li, Shu-Pin
論文名稱： 二氧化錳結合碳的複合材料對電容去離子應用的表面化學行為
Surface chemical behavior of MnO2/carbon composite material in capacitive deionization
指導教授： 王竹方
Wang, Chu-Fang
口試委員: 蔣本基
Chiang, Pen-Chi
王清海
Wang, Tsing-Hai
學位類別： 碩士
Master
系所名稱： 原子科學院 - 生醫工程與環境科學系
Department of Biomedical Engineering and Environmental Sciences
論文出版年： 2019
畢業學年度： 107
語文別： 英文
論文頁數： 96
中文關鍵詞： 電容去離子 、二氧化錳 、電雙層電容
外文關鍵詞： Capacitive Deionization, MnO2, Double Layer Capacitance
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    • 深入瞭解關於二氧化錳(MnO2)以及微孔碳電容性質之間相互作用的電化學行為，對於進一步增強電容去離子(CDI)的表現是不可獲缺的。在此，一系列由不同MnO2/C重量比的電極被製作出來並比較它們在施加不同偏電壓下三組連續充電/放電循環的CDI性能表現。隨著MnO2含量的上升，電極中的電容和微孔洞體積分別以半對數和線性關係下降。更有趣的事是當施加小於水電解電位(1.23 VRHE)的偏壓時，電極的除鹽量會隨著MnO2含量上升而呈現半對數的下降；然而，當施加大於水電解電位的偏壓時，最大除鹽量落在30 weight%的MnO2電極。另外，除鹽量也隨著操作電壓的增加而增加，因此我們推測由微孔碳所產生的重疊電雙層(EDL)電容主要負責在低操作電位(<1.23 VRHE)下除鹽；相反地，在高施加電壓下的高CDI性能可能是來自於部分還原的MnO2所建立的增強電場。因此，可以利用在施加低電壓時增加EDL電容或在施加高電壓時增加法拉第電荷來達到CDI效率的提升。

    Deep understanding the interplay between the electrochemical behavior of associated manganese oxide (MnO2) and the capacitive property of microporous carbonaceous support is essential for further capacitive deionization (CDI) performance enhancement. A series of electrodes with different MnO2/carbon weight ratios were thus fabricated and their CDI performances at different applied potentials in three consecutive charging/discharging cycles were evaluated. It was noted that the capacitance and micropore volume of the electrodes decreased semi-logarithmically and linearly, respectively with increasing MnO2 content. Interestingly when applying a bias lower than the water electrolysis potential (1.23 VRHE), salt removal of electrodes also decreased semi-logarithmically with increasing MnO2 content. However, when a bias higher than the water electrolysis potential was applied, a maximum salt removal was noted at the electrode with 30 weight% MnO2. Provided that the salt removal also increased with increasing operation potential, we therefore speculated that the overlapped electric double layer (EDL) capacitance arisen by microporous carbonaceous supports was mainly responsible for salt removal at low operation potential (<1.23 VRHE). By contrary, high CDI performance under high applied potential was presumably through enhanced electric field established by the partially reduced MnO2. Accordingly, CDI efficiency enhancement can be achieved by increasing either the EDL capacitance when operated under low applied potential or the faradaic charge if high potential is applied.

    摘要 I Abstract II Chapter 1 Introduction 1 1.1 Background of the Study 1 1.2 Research Motivation 2 Chapter 2 Literature Review 5 2.1 Capacitive Deionization (CDI) 6 2.1.1 Brief Introduction of Capacitive Deionization 6 2.1.2 The Mechanisms of Capacitive Deionization 7 2.1.3 Types of CDI Architectures 13 2.2 Manganese Dioxide (MnO2) as Redox Active Material 15 2.2.1 Properties of Manganese Dioxide 16 2.2.2 The Development of Manganese Dioxide as Faradaic Electrodes 19 2.2.3 Conductive Additives 21 2.2.4 The Surface Charge of Electrodes 23 Chapter 3 Experimental Section 26 3.1 Chemical Reagents 26 3.2 Experimental Instruments 27 3.2.1 Electrochemical Workstation 27 3.2.2 Scanning Electron Microscopy (SEM) with Energy Dispersive Spectroscopy (EDS) 28 3.2.3 Specific Surface Area and Porosimetry Analyser (BET) 30 3.3 Details of Preparations and Experimental Methods 32 3.3.1 Synthesis of α-MnO2 material 32 3.3.2 Preparation of different weight ratios of α-MnO2 to CB and AC electrodes 32 3.3.3 Electrochemical Property Measurements 33 3.3.4 Characterization of Electrodes 34 3.3.5 Capacitive Deionization Experiments 35 Chapter 4 Results and Discussion 37 4.1 Fabrication of MnO2/CB composite electrodes 38 4.2 Electrochemical Behaviors of MnO2/CB composite electrodes 44 4.3 The CDI efficiency of MnO2/CB composite electrodes 58 Chapter 5 Conclusion and Future Works 79 5.1 Conclusion 79 5.2 Future Work 80 Reference 81 Appendix 90

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