自組裝電響應石墨烯-高分子薄膜用於可控及可切換的氣體分離機制

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研究生：	JANUAR WIDAKDO JANUAR WIDAKDO
論文名稱：	自組裝電響應石墨烯-高分子薄膜用於可控及可切換的氣體分離機制 Self-assembling electrically responsive graphene-polymer membranes for controlled and switchable gas separation mechanism
指導教授：	洪維松 Wei-Song Hung 賴君義 Juin-Yih Lai
口試委員:	Kueir-Rarn Lee Kueir-Rarn Lee Da Ming Wang Da Ming Wang Ying Ling Liu Ying Ling Liu Chien-Chieh Hu Chien-Chieh Hu Chih-Feng Wang Chih-Feng Wang Hsieh-Chih Tsai Hsieh-Chih Tsai Chung Tai-Shung Chung Tai-Shung
學位類別：	博士 Doctor
系所名稱：	應用科技學院 - 應用科技研究所 Graduate Institute of Applied Science and Technology
論文出版年：	2021
畢業學年度：	109
語文別：	英文
論文頁數：	168
中文關鍵詞：	PVDF β相、電響應薄膜、可調節模式、氣體分離機制、石墨烯 Polydopamine 、離子液
外文關鍵詞：	β-phase of PVDF, Electro responsive membranes, Switchable, Selective gas separation mechanism, Graphene, Polydopamine
相關次數：	點閱：501 下載：0
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上一筆

近年來，刺激響應材料因具有隨外部刺激改變材料特性的能力，在各個領域皆受到重視，其中包含氣體分離相關研究。在響應性材料中，以電能作為刺激源格外受到矚目，乃因其具備快速、非入侵性等特質。電響應材料在節能方面亦有極大的潛能，即便電響應材料含括上述多項優點，但在薄膜領域的研究仍非常少，更不用說應用在氣體分離的電響應材料，本文旨在探討電響應材料用於CO2氣體分離。
本文利用自組裝的(PG), (PVDF/G-PDA) 與 PVDF/Graphene-ion liquid進行一系列CO2氣體分離實驗。在PVDF/Graphene中加入10wt%離子液(BMIM)(BF4)，可發現PVDF的β相增加79.84%。此外，他們擁有高導電率和電容率，分別為15.10×10¬-3 S/cm和0.63×10-9F。薄膜中的氣體通道可隨著施加的外部電壓調整，使單一張膜具分離不同氣體的能力，而CO2的選擇性和滲透率會隨電壓的增加而上升。這些薄膜對於CO2的最大滲透率和選擇率分別為193.55 Barrier與129.03。根據DFT模擬，在系統中CO2較偏向吸引，而O2和N2較偏向排斥。總的來說，調節氣體通道內的自由體積和分子間作用力，讓通道成為分子篩來增加選擇性。本研究為下一代的響應性薄膜開創一個全新的領域。

In recent years, stimuli-responsive materials have garnered interest due to their ability to change properties when exposed to external stimuli, making them useful for various applications, including gas separation. Electricity is a very attractive trigger for responsive materials due to its speedy and non-invasive nature and the potential to reduce energy costs significantly. Even though electric volt is deemed an appealing stimulus for the development of stimuli-responsive materials, this avenue has yet to be extensively researched, as evidenced by the fewer works done on the electro-responsive membranes. Of these, there is even less research done on electro-responsive materials for gas separation. Thus, we have conducted some of the research that answers the criteria.
This dissertation covers the utilization of electro-responsive materials specifically for CO2 gas separation purposes. We self-assembled PVDF-Graphene (PG), PVDF/Graphene-Polydopamine (PVDF/G-PDA), and PVDF/Graphene-Ionic liquid membranes. The results obtained are using PVDF-Graphene with [BMIM][BF4] Ionic liquid (PG-BF410wt%). The β-phase percentage increases by about 79.84%, which displays a unique self-piezoelectric property. Additionally, those membranes exhibit excellent electrical conductivity and unique capacitive properties about 15.10 x 10-3 S/cm and 0.63 x 10-9 F. The resultant of interface channels in the membrane can be reversibly adjusted by external voltage applications (3 Volt), resulting in the tailored gas selectivity of a single membrane. Applying a voltage to the membrane, the permeability and selectivity toward CO2 increase simultaneously. Those membranes achieved the highest CO2 permeability and CO2/N2 selectivity about 193.55 Barrer and 129.03. Based on Density Functional Theory (DFT) simulation, CO2 has more attraction (adsorption takes place). However, O2 and N2 have repulsion (no adsorption) in the system. Overall, tuning the free volume and molecular interactions within the channels provides a rational molecular sieving approach to improve membrane selectivity. This research opens new avenues for the development of a new generation of responsive membranes.

ABSTRACT    i
摘 要    iii
CERTIFICATE    iv
DECLARATION    v
ACKNOWLEDGEMENT    vi
TABLE OF CONTENTS    viii
LIST OF FIGURES    x
LIST OF TABLES    xv
LIST OF ABBREVIATIONS    xvi
CHAPTER 1    1
1 INTRODUCTION    2
2 DISSERTATION GOALS AND OUTLINE    4
CHAPTER 2    7
1 MEMBRANE GAS SEPARATION MATERIAL SCIENCE PROGRESS    8
2 PERMEABILITY AND SELECTIVITY    11
3    TRADITIONAL MEMBRANE FOR GAS SEPARATION    14
3.1 Polymer (organic-inorganic) membrane    14
3.2 Mixed matrix membrane    15
3.3 Supported Ionic Liquid Membranes    17
4 RESPONSIVE AND SWITCHABLE MEMBRANE FOR GAS SEPARATION    18
5 MECHANISM OF ELECTRICAL-RESPONSIVE MEMBRANES    21
6 POLYVINYLIDENE FLUORIDE (PVDF)    22
7 GRAPHENE    24
8 POLYDOPAMINE    25
9 IONIC LIQUID    27
CHAPTER 3 Mechanism of A Self-Assembling Smart and Electrically Responsive PVDF-Graphene Membrane for Controlled Gas Separation     28
1 INTRODUCTION    29
2 EXPERIMENTAL SECTION    31
2.1 Materials    31
2.2 Fabrication of PVDF-Graphene Membranes    32
2.3 Characterization of the PVDF-Graphene Membranes    32
2.4 Switchable Gas Separation Performance of PVDF-Graphene Membranes    33
2.5 Determination of Free Volume    34
3 RESULTS AND DISCUSSION    35
3.1 Characterization of Graphene Sheets    35
3.2 Structural Morphology of PVDF-Graphene Membranes    36
3.3 Physicochemical Characterization of PVDF-Graphene Membranes    37
3.4 Electrical Properties of the PVDF-Graphene Membranes    43
3.5 Switchable Gas Separation Performance of the PVDF-Graphene Membranes    46
4 SUMMARY    53

CHAPTER 4 Tailoring of Graphene–Organic Frameworks Membrane to Enable Reversed Electrical-Switchable Permselectivity in CO2 Separation    55
1 INTRODUCTION    56
2 MATERIALS AND METHODS    59
2.1 Materials    59
2.2 Synthesis of Graphene-Polydopaminex (G-PDAx) composite powder    59
2.3 Fabrication of the smart graphene–organic frameworks membranes    60
2.4 Membrane Characterizations    61
2.5 Membrane separation performance    62
2.6 Digital Image Correlation (DIC) of membranes by Optical Microscope    63
3 RESULTS AND DISCUSSION    64
3.1 Characterization of the Graphene-Polydopamine (G-PDAx) composite    64
3.2 Morphological Characterization of the PVDF/(G-PDAx) Membranes    67
3.3 Mechanical and Physicochemical Characterization of the PVDF/(G-PDAx) Membranes    70
3.4 Electrical Properties of the PVDF/(G-PDAx) Membranes    80
3.5 Reversed Electrical-switchablilty of the PVDF/(G-PDAx) Membranes    82
4 SUMMARY    93

CHAPTER 5 Electric-Switchable Smart Ionic Liquid Molecular Sieving Membranes with Tunable and Enhanced Gas Separation Performance    94
1 INTRODUCTION    95
2 EXPERIMENTAL SECTION    98
2.1 Materials    98
2.2 Fabrication of the PG-Ionic liquid membranes    99
2.3 Characterization of the PG-Ionic liquid membranes    100
2.4 Controlled Gas Separation Performance of the PG-Ionic liquid membranes    101
2.5 Density Function Theory Simulation of Adsorption of CO2 and O2 on the Graphene with PVDF, BMIM, BF4, and BF6 system    102
3 RESULTS AND DISCUSSION    104
3.1 Physical and chemical test of PG-Ionic liquid membranes    104
3.2 Mechanical and electrical characterization of PG-Ionic liquid membranes    117
3.3 Tunable and electric-controllable membrane permeation    121
3.4 Density Function Theory Simulation    125
4 SUMMARY    127

CHAPTER 6    129
1 CONCLUSIONS    130
2 FUTURE PERSPECTIVE    131
3 LIST OF PUBLICATIONS    132
4 ACHIEVENEMT    132
REFERENCES    133

                                

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