光熱性銣鎢青銅奈米棒/三醋酸纖維素電紡纖維膜於光致蒸發、汙水處理與海水淡化研究.

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研究生：	Saba Naseem Saba Naseem
論文名稱：	光熱性銣鎢青銅奈米棒/三醋酸纖維素電紡纖維膜於光致蒸發、汙水處理與海水淡化研究. Study on Photothermally Activated Tungsten-bronze/ Recycled Cellulose Triacetate Porous Fiber Membranes for Light-Driven Water Evaporation, Sewage Treatment and Desalination
指導教授：	吳昌謀 Chang-Mou Wu
口試委員:	郭東昊 Dong-Hau Kuo 邱顯堂 Hsien-Tang Chiu 李貴琪 Kui-Chi Lee 鄭國彬 Kuo-Bin Cheng 鄭大偉 Ta-Wui Cheng
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：	2020
畢業學年度：	108
語文別：	英文
論文頁數：	165
中文關鍵詞：	三醋酸纖維素、二氧化鈦、氧化石墨烯、油水分離、鎢青銅、光熱轉化
外文關鍵詞：	Cellulose triacetate, Tungsten bronze, Photothermal conversion, Electrospinning, Water evaporation, Purification and Desalination
相關次數：	點閱：302 下載：0
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太陽能是一種可再生能源，因為它具有廣泛的可用性和取之不盡，用之不竭的優勢。太陽能的轉換和使用預期是解決全球能源和環境危機的主要解決方案之一。在各種太陽能源轉換方式中，太陽能熱轉換是最簡單，最有效的。在過去的十年中，光熱材料的使用引起了新的科學興趣，並且由於其簡單的操作以及非常高的能量轉換效率，導致此材料一些應用利基。在各種光熱材料中，半導體型金屬氧化物（例如氧化鎢基材料）是在光照明下將光能轉換為熱能的最有潛力的材料。本文重點介紹了具有光熱轉換性能的鎢青銅（MxWO3）材料，並探討於光驅動界面水蒸發以及全光譜太陽能光熱轉換以增強水氣蒸發。
在第二項工作中，我們製備光熱響應性鎢青銅/回收三醋酸纖維素多孔纖維膜，並探討此複合纖維膜用於光驅動界面水氣蒸發效能之研究。太陽能驅動水蒸氣產生是製備蒸餾水和廢水處理常見之策略。而氧化鎢基複合材料由於其優異近紅外(NIR)光吸收及能將其轉化為熱量之特性，近來於水氣蒸發應用上備受關注。此氧化鎢基材料的強表面電漿共振和間隔電荷轉移導致在寬NIR光譜中具有高光吸收率。本研究藉由溶液靜電紡絲法製備銣鎢青銅/回收三醋酸纖維素(RbxWO3/rTAC) 多孔纖維膜，且此纖維模無需支撐層，所得RbxWO3/rTAC多孔纖維膜由於重量輕且疏水性好而可漂浮在水面上。將不同比例RbxWO3(0、5、10、15和20wt%) 摻入回收三醋酸纖維素(rTAC)基材中，並探討其光驅動水氣蒸發的效率，結果顯示rTAC明顯有助於潤濕性能，而其多孔結構則有利於太陽光能驅動水氣蒸發。結果表明，RbxWO3納米棒的重量百分比為15％時，RbxWO3/rTAC纖維膜的水氣蒸發效率可達最佳化，約為90.4±2.1％，此效率遠高於純rTAC纖維膜和純水的蒸發效率。此外，本研究藉由模擬光源照射，也證明了此材料優異之應用潛力，其水氣轉換效率約為73.6％。因此，RbxWO3/rTAC光熱纖維膜可應用於水質淨化，海水淡化和蒸汽發電等領域。
論文的最後一章，以開發RbxWO3-Fe3O4混成材料，使之具有全光譜吸收功效的光熱轉換纖維膜為目的，而可有效地利用太陽能並驅動水氣蒸發。將太陽能有效利用並轉換為熱能是可再生能源研究的理想目標之一。因此，本研究開發了一混成奈米材料，而可從紫外線到可見光到近紅外光的全光譜能量範圍內進行高效率的水氣蒸發。使用廉價的Fe3O4奈米顆粒與銣鎢青銅納米棒進行混成，以使混成材料具備全光譜吸收功效並確保高水氣蒸發速率。光學結果證明，RbxWO3-Fe3O4奈米混成材料在全光譜範圍中表現出高吸收率，尤其是在可見光和近紅外區域有高效吸收表現。RbxWO3-Fe3O4奈米混成材料的光熱轉性能遠高於個別RbxWO3和Fe3O4奈米材料。本研究我們成功地通過化學沉澱法合成了不同比例之RbxWO3-Fe3O4奈米混成材料(摩爾比2:1,1:1,1:2, 1:4)。並使用靜電紡絲方法以控制纖維結構、孔隙率、取向和長度，配合RbxWO3-Fe3O4共混摻入rTAC基材中，直接進行電紡成多孔混成奈米纖維膜，配合界面加熱概念，將所形成的纖維膜用於光熱水氣蒸發研究。蒸發速率主要取決於新開發的自支撐雙層薄膜，其中上層為光熱轉換層而底部則為親水性支撐層，與前章所報導的銣鎢青銅/回收三醋酸纖維素多孔纖維膜之結果相比，具有親水性支撐層與高效全光譜吸收的RbxWO3-Fe3O4/rTAC光熱纖維膜顯示出較高的水氣蒸發效率。本研究實現利用太陽能於光熱水氣蒸發和脫鹽應用的巨大潛力。藉由本研究結過證明，RbxWO3-Fe3O4奈米混成光熱纖維膜是一種很有前途的光熱材料，可在全光譜太陽光照射下，顯著且有效升高其溫度。

Solar energy is a kind of renewable energy source open to mankind because of its wide availability and inexhaustibility. The conversion and use of solar energy is one of the main solutions for addressing the global energy and environmental crisis expected. The solar thermal energy conversion is the simplest and most effective amongst the various solar energy conversion pathways. The use of photo-thermal materials has gained renewed scientific interest over the last decade and has resulted in some niche applications due to its simple operation and more importantly extremely high energy conversion efficiency. Among various photo-thermal materials, semiconductor type metal-oxides such as tungsten-oxides based materials are the most promising candidates for converting light to heat energy under optical illumination. Herein, the dissertation highlights tungsten bronze (MxWO3) materials for photothermal conversion properties, applications for light-driven interfacial water evaporation and full-spectrum solar to heat conversion for enhanced steam generation, water purification and desalination.
In first section, we report photothermal-responsive tungsten bronze/recycled cellulose triacetate porous fiber membranes for efficient light-driven interfacial water evaporation. Solar-driven steam generation is a common strategy for clean water production and wastewater treatment. Tungsten-oxide-based composites have lately gained significant attention due to their capability of absorbing near-infrared (NIR) light and transforming it into heat for evaporating water. The strong surface plasma resonances and intervalence charge transfer of these composites result in high photoabsorption in a wide NIR spectrum. Here, we fabricate combined rubidium tungsten bronze and recycled triacetate cellulose (RbxWO3/rTAC) porous fiber membranes without any supporting components, via solution electrospinning. The as-prepared RbxWO3/rTAC porous fiber membranes float on the water surface because of their low weight and hydrophobicity. RbxWO3 (0, 5, 10, 15, and 20wt%) was incorporated into a recycled triacetate cellulose (rTAC) matrix, and its efficiency for light-driven water evaporation was calculated. The rTAC polymer, significantly contributes toward its desirable wetting properties and its porous structure, which are favorable for solar steam generation. The results showed that the evaporation efficiency of RbxWO3/rTAC fiber membranes with an optimized 15wt% of RbxWO3 nanorods reached 90.4±2.1%, which is considerably greater than that of pure rTAC fiber membranes and of pure water. A great potential has also been proved by simulating solar exposure, with a water conversion efficiency of approximately 73.6%. Thus, RbxWO3/rTAC photothermal fiber membranes can find applications in water purification, desalination, and steam power generation.
The final part of the thesis presents solar interfacial water evaporation using nanostructured photothermal material is an effective pathway for seawater desalination and waste water treatment. The utilization of inexpensive Fe3O4 with tungsten bronze is a convenient approach for accelerating the full spectrum absorption while ensuring a high evaporation rate. Therefore, this works present efficiency of water evaporation in different photonic energy range, from UV-to-vis-to-NIR. The optical results proved that the RbxWO3-Fe3O4 nanocomposites exhibit a high absorbance in a wide spectrum, especially in the visible and NIR region. Photothermal conversion property of RbxWO3-Fe3O4 nanocomposites are higher than individual RbxWO3 and Fe3O4 nanomaterials. In order to fabricate janus membrane with controlled fiber structure, porosity, orientations and lengths, the interest in the manufacture of microfibers using electrospinning method. RbxWO3-Fe3O4 nano-structured embedded into the rTAC matrix to further electrospun into porous fiber membranes and the formed film was used as a photothermal membrane for water evaporation based on a concept of interfacial solar heating. The rate of evaporation depends mainly on double-layer thin film on the water surface, in which the top photothermal light to heat conversion layer and the bottom hydrophilic supporting layer for pumping water. In addition, janus membrane with a unique characteristic of high thermal stability and excellent thermal insulation property (0.028 W.m-1K-1). The calculated evaporation rate for optimized 10wt% janus membrane found to be 3.56 kg.m-2.h-1 after 35 mins irradiation which was 2.12 times higher than pure water (1.44 kg.m-2.h-1) under 0.250 W.cm-2 of irradiation. This scalable janus membrane strongly evident for synergic photocatalytic activity for heavy metal degradation which made it possible to treat wastewater and can be used to generate clean water from contaminants like heavy metal ion and organic dyes with nearly 99% rejection. Moreover, multifunctional janus membrane shows great potential for seawater desalination with a very high rejection rate of 99.9% for Na+ and below 99.7% for other ions that complies fully with drinking standards. Our work highlights the great potentials for implementing solar energy driven photothermal janus membrane for fresh water production.

Table of Contents
中文摘要    IV
ABSTRACT    VII
Keywords:    ix
ACKNOWLEDGEMENT    X
CHAPTER 1. INTRODUCTION    1
1 Membrane Technology    1
2 The emergence of solar energy utilization    2
3 Motivation and objectives of the study    6
REFERENCES    12
CHAPTER 2: BACKGROUND AND LITERATURE REVIEW    19
1 Electrospinning    19
2 Electrospinning parameters    22
1.1 Voltage supply    23
1.2. Needle diameter (nozzle)    23
1.3. Distance between tip and collector    24
1.4. Flow rate    24
1.5. Collector    24
1.6. Ambient parameters    25
2 Surface morphology of recycled cellulose tricetate fiber membranes    25
2.1 Surface modification of rTAC fiber membranes for oil-water separation    27
2.2. Contact angle analysis    29
2.3 Performance of modified rTAC fiber membranes for oil-water separation    31
3 Photothermal nanomaterials:    34
4. Photothermal Conversion Properties of Tungsten-Oxide-based Materials.    35
5. Preparation of Tungsten-Oxide-Based Materials    39
5.1. Mechanochemical method    39
5.2. Chemical vapor transport (CVT)    40
5.3. Solid-phase reaction    40
5.4. Inductively coupled thermal plasma method (ICTP)    41
5.5. Hydrothermal method    41
5.6. Solvothermal method    42
6 Factors affecting solar driven steam generation    44
6.1 Conversion efficiency    45
7. Photothermal Conversion Materials    51
7.1 Plasmonic metals    51
7.2. Carbon-based nanomaterials    53
7.3. Conducting polymers    54
7.4. Semiconductor based nanomaterials    55
8 Applications of Tungsten-oxide-based Materials    58
8.1. Heat generation    58
8.2. Photocatalysts    63
8.3. Energy-related applications    67
8.4. Gas sensors    70
REFERENCES    72
CHAPTER 3: PHOTOTHERMAL-RESPONSIVE TUNGSTEN BRONZE/RECYCLED CELLULOSE TRIACETATE POROUS FIBER MEMBRANES FOR EFFICIENT LIGHT-DRIVEN INTERFACIAL WATER EVAPORATION    96
1. INTRODUCTION    96
2 EXPERIMENT    100
2.1 Materials    100
2.2 Synthesis of RbxWO3 nanorods    100
2.3 Preparation of RbxWO3/rTAC fiber membranes    100
2.4 Measurement of Water evaporation    101
2.5 Characterization    101
3 RESULTS AND DISCUSSION    102
3.1 Characterization of the RbxWO3/rTAC porous fiber membranes    102
3.2 Optical and Photothermal Properties of RbxWO3/rTAC porous fiber membrane    104
3.3 Photothermal evaporation performance of RbxWO3/rTAC porous fiber membranes    108
4.  SUMMARY    115
REFERENCES    117
CHAPTER 4. SOLAR THERMAL JANUS MEMBRANE PROMOTED SYNERGIC-PHOTOCATALYTIC PURIFICATION AND DESALINATION    123
1. INTRODUCTION    123
2 EXPERIMENT    126
2.1 Materials    126
2.2 Synthesis of RbxWO3-Fe3O4 nanocomposites    127
2.3 Preparation of the Janus membranes    127
2.4 Measurement of Solar-Enabled Water Evaporation Performance    128
2.5 Solar-enabled Water Purification, Desalination and Synergic Photocatalytic Membrane Performance    128
2.6 Characterization    130
3 RESULTS AND DISCUSSION    131
3.1 Characterization of the sample    131
3.2 Optical and Thermal Analysis    137
3.3 Fluid Transport and Thermal Insulation properties    141
3.4 Solar-to-Vapor Conversion Efficiency Measurement    143
3.5 Clean Water Generation with Synergic Photocatalysis    146
3.6 Solar Thermal Promoted Desalination    151
5. SUMMARY    154
REFERENCES    155
CHAPTER 5. CONCLUSION AND OUTLOOK    163
1 CONCLUSION    163
2 OUTLOOK    165
CURRICULUM VITAE    167
PROJECT UNDERTAKEN    168
PUBLICATIONS IN INTERNATIONAL JOURNALS    169
CONFERENCES/ORAL PRESENTATIONS    170


                                

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