A study on superhydrophilic copolymers for the application of moisture management and sewage treatment

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研究生：	Shamik Chaudhuri Shamik Chaudhuri
論文名稱：	A study on superhydrophilic copolymers for the application of moisture management and sewage treatment A study on superhydrophilic copolymers for the application of moisture management and sewage treatment
指導教授：	吳昌謀 Chang-Mou Wu
口試委員:	吳昌謀 Chang-Mou Wu 今榮東洋子 Toyoko Imae Ching-Yuan Su Ching-Yuan Su Chi-Chin Kuo Chi-Chin Kuo 郭東昊 Dong-Hau Kuo Bin-Chang Kuo Bin-Chang Kuo Chi-Hsu Yao Chi-Hsu Yao
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：	2021
畢業學年度：	109
語文別：	英文
論文頁數：	161
中文關鍵詞：	智能聚合物、熱響應、低臨界溶液溫度、潤濕性、智能紡織品、聚合物膜、靜電紡絲、螢光、金屬離子感測、氣凝膠、光催化
外文關鍵詞：	Smart polymers, Thermoresponsive, Lower critical solution temperature, Wettability, Smart textile, Polymer membranes, Electrospinning, Fluorescence, Metal ion sensing, Aerogel, Photocatalysis
相關次數：	點閱：384 下載：0
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上一筆

超親水聚合物，它們在不同的結構中可以有很多不同的應用，其中水吸收是主要被關注的應用。由於其對水的高親和性，該聚合物可以根據我們的要求來調整。本文重點介紹了超親水性聚合物及其在水分控制，金屬離子感測和光催化活性降解水溶液中的有機污染物。
在第一部分中，我們通過自由基聚合反應合成了 poly[(N-isopropylacrylamide)-co-(2- hydroxyethylmethacrylate)-co-(N-methylolacrylamide)] [poly(NIPAAm-co-HEMA-co- NMA)]的無規共聚物。以 NIPAAm，HEMA 和 NMA 為架構，分別提供熱響應性，吸水率和水分保留率控制以及化學交聯，以實現在水性介質中的穩定性。
由於NIPAAm 低臨界溶液溫度的特性，其在 25℃至 40℃之間會顯著的體積變化（親水/疏水性），該共聚物也表現出隨溫度變化，其光透射率也跟著改變。接著我們將共聚物線棒塗佈在聚對苯二甲酸乙二酯（PET）織物上，並測試了塗層織物在不同溫度下的濕潤性及水分吸收和釋放。其結果在 20°C 和 37°C 下，P2 共聚物具有最高的吸濕和釋放能力。因此，具有定制性能的共聚物可以用作特定活動服裝的智能紡織品。
在第二部分中，我們開發出對 Co2 +和 Cu2 +離子具有高靈敏度的開/關可切換的新型奈米纖維膜。其研究通過電紡製備 poly[(2-hydroxyethylmethacrylate-co-N- methylolacrylamide)]

[poly(HEMA-co-NMA)]的奈米纖維膜並在其中混摻不同含量的 2,2’- bipyridine-3,3’-diol (BPDO)，其中通過自由基聚合反應合成不同摩爾比的 Poly(HEMA-co-NMA)。添加HEMA 和 NMA 以促進親水性和交聯反應，最終支持水性介質中的機械穩定結構。並以電紡奈米纖維膜 S1-0.5 (HEMA：NMA = 77:23, BPDO 的 0.5 wt％) 於濃度範圍為 10-7 M 至 10-4 M 的 Co2 +和 Cu2 +離子時，顯示出強光致發光猝滅。當添加 Cu2 +離子和乙二胺四乙酸（EDTA）時，奈米纖維膜表現出可逆的開/關螢光發光特性。這些結果以簡單的製程方式製造奈米纖維膜，且該膜具有對金屬離子的實時感測具有相當的潛力。
在第三部分中，我們通過冷凍乾燥法製備了高比表面積，低密度的乙烯醇(PVA)/奈米纖維素(CNF)摻混 WO2.72-Fe3O4 粉體的氣凝膠（NC-CNF），並研究了其對於甲基橙再模擬太陽光催化降解的特性。在該系統中，WO2.72-Fe3O4 是奈米複合光催化劑並結合聚乙烯醇（PVA）的高親水性，使其增強了吸收污水以提高光催化性能的能力。此氣凝膠也利用戊二醛使纖維素奈米纖維和 PVA 進行化學交聯，以使其在水溶液中結構穩定。此研究探討了 MO 的降解動力學並比較了 WO2.72-Fe3O4 粉末（NC），纖維素奈米纖維氣凝膠（CNF）和 NC-CNF 的光催化性能。

Superhydrophilic polymers, in their different structural forms can be utilized in wide range of applications where water absorption is the prime interest. Due to their high affinity towards water, such polymers can be tuned according to our requirement. Herein, the dissertation highlights superhydrophilic polymers and their tunable structure-property relation for moisture management, metal ion sensing and photocatalytic activity for the degradation of organic pollutants in aqueous solution.

In first section, we synthesized a random poly[(N-isopropylacrylamide)-co-(2- hydroxyethylmethacrylate)-co-(N-methylolacrylamide)] [poly(NIPAAm-co-HEMA-co- NMA)] copolymer through free-radical polymerization. The NIPAAm, HEMA and NMA moieties were framed to provide thermoresponsiveness, water absorption and retention control, and chemical cross-linking to achieve stability in aqueous medium, respectively. The copolymer showed a significant change in optical transmittance with a variation in temperature due to the change in volume (i.e., hydrophilic/hydrophobic) between 25 °C and 40 °C, attributed to the lower critical solution temperature property of the NIPAAm moiety. The copolymers were wire-bar-coated onto knitted polyethylene terephthalate (PET) fabric. Variation in the water contact angle affirmed the switchable wettability due to the change in temperature. We tested the coated fabrics for moisture absorption and release at different temperatures. The results at 20 °C and 37 °C indicated that the P2 copolymer had the highest moisture absorption and release capability. Therefore, the copolymers with tailored properties can be used as smart textiles for activity specific clothing.
In the second section, the study presents new on/off switchable nanofiber membranes with high sensitivity for detecting Co2+ and Cu2+ ions. The nanofiber membranes were fabricated by electrospinning the poly[(2-hydroxyethylmethacrylate-co-N-methylolacrylamide)] [poly(HEMA-co-NMA)] copolymer with different quantities of 2,2’- bipyridine-3,3’-diol

(BPDO). Poly(HEMA-co-NMA) random copolymers with various molar ratios of the HEMA and NMA monomers were synthesized by free radical polymerization. The HEMA and NMA moieties were specifically selected to promote hydrophilicity and cross-linking reactions, which ultimately support a mechanically stable structure in aqueous media. ES nanofiber membranes S1-0.5, with a HEMA:NMA molar ratio of 77:23 and 0.5 wt% of BPDO showed strong photoluminescence quenching upon exposure to Co2+ and Cu2+ ions at concentrations ranging from 10-7 M to 10-4 M. Moreover, the nanofiber membranes exhibited reversibile on/off fluorescence emission properties upon the sequential addition of Cu2+ ions and ethylenediaminetetraacetic acid (EDTA). These results demonstrate a simple fabrication strategy for nanofiber membranes that have the potential to be effective for the real-time sensing of metal ions.
In the third section, we fabricated a high specific surface area, low density WO2.72-Fe3O4 nanocomposites-blended polyvinyl alcohol/ cellulose nanofiber aerogel (NC-CNF) through freeze drying method and photocatalytic performance of the aerogel has been studied considering methyl orange (MO) as a model pollutant in aqueous solution under solar irradiation. In this system, WO2.72-Fe3O4 is nanocomposite photocatalyst. Polyvinyl alcohol (PVA) enhanced the ability of absorbing polluted water to increase the photocatalytic performance due to its high hydrophilicity. The aerogel has been chemically cross-linked with cellulose nanofiber and PVA by glutaraldehyde in order to make it structurally stable in aqueous solution. The photocatalytic performance of WO2.72-Fe3O4 powder (NC), cellulose nanofiber aerogel (CNF) and NC-CNF has been compared and also kinetics of degradation of MO has been studied.

摘要    i
Abstract    iii
Acknowledgement    vi
Table of Contents    vii
Index of symbol    x
List of Figures    xi
List of Tables    xiii
0.    INTRODUCTION    1
1.    Superhydrophilicity and superhydrophobicity    1
2.    Sewage water treatment    2
3.    Motivation and objective    6
0.    BACKGROUND AND LITERATURE REVIEW    9
1.    Stimuli-responsive polymers    9
1.1.    Thermoresponsive polymers    10
1.2.    pH responsive polymers    11
1.3.    Photo-responsive polymers    13
1.4.    Electric and magnetic field responsive polymers    14
2.    LCST property of PNIPAAm    16
3.    Application of PNIPAAm based polymers    19
3.1.    Biomedical application    19
3.2.    Moisture control and smart textile application    21
3.3.    Other applications    22
4.    Poly(2-hydroxyethylmethacrylate) [poly(HEMA)]    23
5.    Cross-linking phenomena    24
6.    Metal-ion sensing materials    25
7.    Metal-ion sensing mechanism    26
8.    Electrospinning    28
9.    Photocatalysis and photocatalyst materials    29
10.    CNF aerogels    30
10.1.    Synthesis of CNF aerogels    30
10.2.    Properties of CNF aerogels    32
11.    Application of CNF aerogels    33
11.1.    Thermal insulation and flame retardancy    33
11.2.    CO2 capture    34
11.3.    Oil-water separation    34
11.4.    Photocatalysis    35
0.    SWITCHABLE WETTABILITY OF POLY (NIPAAM-CO-HEMA-CO-NMA) COATED PET FABRIC FOR MOISTURE MANAGEMENT    37
1.    Introduction    37
2.    Experiment    41
2.1.    Materials    41
2.2.    Synthesis of poly(NIPAAm-co-HEMA-co-NMA)    41
2.2.1.    Synthesis of P1    42
2.2.2.    Synthesis of P2    42
2.3.    Fabrication of copolymer coated knitted PET fabrics    43
2.4.    Characterization    43
3.    Results and discussion    45
3.1.    NMR spectroscopy    45
3.2.    FTIR spectroscopy    47
3.3.    Thermal behavior    48
3.4.    LCST...    50
3.5.    Swelling test    52
3.6.    Surface wettability    52
3.7.    Moisture management    55
3.8.    Mechanical property    56
4.    Summary    57
0.    HIGHLY SENSITIVE ELECTROSPUN POLY(HEMA-CO-NMA)/BPDO NANOFIBER MEMBRANES FOR SENSING METAL IONS IN AQUEOUS MEDIA    58
1.    Introduction    58
2.    Experiment    62
2.1.    Materials    62
2.2.    Synthesis of poly(HEMA-co-NMA)    62
2.3.    Fabrication of cross-linked ES nanofiber membranes    65
2.4.    Characterization    66
3.    Result and discussion    67
3.1.    NMR spectroscopy    67
3.2.    FTIR spectroscopy    69
3.3.    Metal ion selection by BPDO…………………………………………………………....70
3.4.    Morphology of ES nanofiber membranes    .71
3.5.    Detection of different concentration of metal ions by BPDO    73
3.6.    Detection of metal ions by S1-0.5 ES nanofiber membranes    77
3.7.    Comparison of the fluorescence responses of ES nanofiber membranes and BPDO in solution state    79
3.8.    Reversibility and stability of the ES S1-0.5 nanofiber membranes    81
3.9.    Schematic of S1-0.5 ES nanofiber membranes for sensing application    82
4.    Summary    85
0.    ADSORPTION AND DEGRADATION OF ORGANIC DYE BY WO2.72-Fe3O4 MODIFIED CNF AEROGEL    87
1.    Introduction    87
2.    Experimental    90
2.1.    Materials    90
2.2.    Synthesis of WO2.72-Fe3O4 (NC) nanocomposites    91
2.3.    Fabrication of NC-CNF and CNF aerogel    91
2.4.    Characterization    92
2.5.    Evaluation of photocatalytic activity    92
3.    Result and discussion    92
3.1.    Morphology    92
3.2.    Physical properties    93
3.3.    Photocatalytic activity    94
4.    Summary    96
0.    CONCLUSION AND OUTLOOK    97
1.    Conclusion    97
2.    Outlook    99
References    100

                                

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全文公開日期 2024/02/05 (校內網路)
全文公開日期 2026/02/05 (校外網路)
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