本研究著眼於利用新穎且低成本的技術進行表面潤濕性之改質，從親水表面改質成超親水表面，抑或是液體抗沾表面（即具備超疏水或疏油特性）於空氣中或是油/水系統中。吾人成功研發出以大氣電漿束合成自我組裝的多階層奈米結構，由於沉積速率快，在數秒之內即可均勻地沉積出薄膜，且此技術適用於各式基板表面，如玻璃、金屬、紙張、高分子表面等。利用大氣電漿束所沉積出來具有奈米結構的薄膜本質上為超親水，經過利用過氟矽烷長鏈修飾的氟化過程，可表現出優異的超疏水性及疏油性，且具有好的耐久性質。此外，透過將部分區域以矽氧樹脂膠帶封閉，可達到選擇性修飾基板為超疏水或超親水。而不同於一般的液體抗沾表面（在空氣中），水中疏油表面也可直接透過所合成的多階層結構薄膜以水先浸潤，即可達到良好的水中疏油性質，毋須進一步的化學表面改質。由於該多階層結構薄膜有著極大的表面積，所捕捉住的液體層可以提供非常優異的抗沾特性，使表面不被油汙所沾染，可進一步將此薄膜搭配不銹鋼網利用於重力驅動之油水分離。而有關油水分離的實驗重要因子，也在本研究中有詳細討論。另一方面，為了探討同時在水相與油相中同時能具備抗沾特性的表面，吾人利用冷凍鑄造法合成的矽藻土多孔膜以進一步研究。由於矽殼擁有精細複雜的奈米多孔結構，經由冷凍鑄造，形成規則排列的微米通道，此多階層結構造成了此多孔膜得以同時在油相與水相表現出液體抗沾特性。此外，即使該多孔膜受到外力破壞其表面結構，其抗沾特性仍能維持。綜合以上，本研究提供了對於設計抗沾表面的創見與重要準則，可望應用於自潔表面，減少拖曳力，以及油水分離等領域。

This study focuses on manipulating surface wettability from hydrophilic to superhydrophilic or super-liquid repellent in air or oil/water system by using a novel and cost-effective approach. The hierarchically structured surfaces are synthesized by a plasma-assisted nanofabrication method under atmospheric pressure. Due to the fast deposition rate of nanoparticles, a uniformed thin film can be formed on various substrates within a few seconds. After fluorination with perfluoroalkylsilane, it becomes a superhydrophobic and oleophobic surface with good durability. This versatile methodology can even selectively render the surface superhydrophobic by simply blocking area with silicone tapes. Distinguished from the liquid-repellent surfaces in air, the underwater superoleophobic surface can be obtained directly by pre-wetting the as-synthesized structures by water. Owing to the hierarchical structure and large surface area, the entrapped liquid layer is able to avoid the contamination by oils. The critical factors for the membrane used for oil/water separation are also discussed in this research. On the other hand, to further investigate surfaces with dual superlyophobicity in oil/water system by the effect of hierarchically porous structures, which has not been comprehensively studied in literature, a bio-inspired diatomite membrane is synthesized by a freeze casting method. The synergistic effect of sophisticated nano-porous structures of frustules and the micro-channels induces super-liquid repellent property in both oil and water system. This research provides insights for rational designs of a liquid repellent surface either in air or liquids (oils or water), and might further lead to practical applications in self-cleaning, drag reduction and oil/water separation.

Abstract 2
摘 要 3
Acknowledgement 4
致 謝 6
Table of Content 7
Chap 1 Introduction 10
1.1 Super-liquid repellent surfaces in air 10
1.2 Underwater Super-liquid repellent Surfaces 12
Chap 2 Motivation and Outline 15
Chap 3 Theory 17
3.1 Definition of Wettability 17
3.1.1 Static and dynamic contact angles 17
3.1.2 Morphology affecting super-liquid repellency 20
3.2 Approaches for fabricating super-liquid repellent surfaces 25
3.2.1 Randomly hierarchical structured coatings 26
3.2.2 Overhanging micro-structures in periodic array 30
3.3 Plasma technique and its applications for non-wetting surfaces 33
3.3.1 Plasma polymerization for superhydrophobic surfaces 34
3.3.2 Atmospheric pressure plasma-assisted nanofabrication 35
Chap 4 Principle of Characterization Methods 37
4.1 Electron microscopy (EM) 37
4.2 Atomic force microscopy (AFM) 39
4.3 X-ray photoelectron spectroscopy (XPS) 41
Chap 5 Research Project (I): Stalagmite-like Self-cleaning Surfaces Prepared by Silanization of Plasma-assisted Metal-oxide Nanostructures 44
5.1 Introduction 45
5.2 Experimental Section 47
5.2.1 Customized Atmospheric Pressure Plasma System 47
5.2.2 Coating Procedure 48
5.2.3 Material Characterization 49
5.2.4 Contact Angle Measurements 50
5.2.5 Dynamic Behaviour Observations of a Water Bouncing Drop 50
5.3 Results and Discussion 51
5.3.1 Preparation and Characterization of Hierarchically Structured Coatings 51
5.3.2 Multilayer Growth of FAS 62
5.3.3 Dynamic Behaviour of Water Droplets on SCWO Surfaces 66
5.3.4 Evaluation of Stability and Multifunctional Properties 70
5. 4. Summary 84
Chap 6 Research Project (II): Rapid Deposition of Superhydrophilic Stalagmite-like Protrusions for Underwater Selective Superwettability 85
6.1 Introduction 86
6.2 Experimental section 88
6.2.1 Materials and Reagents 88
6.2.2 Fabrication of underwater superoleophobic surface 88
6.2.3 Material Characterizations 88
6.2.4 Contact angle measurements (in air and underwater) 89
6.2.5 Gravity oil-water separation 89
6.3 Results and discussion 90
6.3.1 Superhydrophilic surfaces for underwater super-antiwettability 90
6.3.2 Robust underwater superoleophobicity 96
6.3.3 The effect of surface roughness and pore size 102
6.3.4 Summary 108
Chap 7 Research Project (III): Bioinspired Diatomite Membrane with Selective Superwettability for Oil/Water Separation 110
7.1 Introduction 111
7.2 Experimental Section 113
7.2.1 Materials and Reagents 113
7.2.2 Preparation of diatomite scaffold and diatomite membrane 113
7.2.3 Characterization techniques 114
7.2.4 Oil/water separation 116
7.3 Results and Discussions 116
7.3.1 Bioinspired diatomite membrane 116
7.3.2 Selective wettability in liquid systems 120
7.3.3 Intrusion Pressure Measurement 128
7.3.4 Mechanical durability and anti-fouling property 129
7.3.5 Water Flux Measurement 131
7.4 Summary 134
Chap 8 Conclusions and Outlook 136
8.1 Conclusions 136
8.2 Outlook 138
References 140

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