TiO2自潔薄膜往往因為材料本身的高折射率造成不透明及暗處存放時造成親水性的喪失，而成為應用時的缺憾。本研究的目的就是嘗試解決這兩個問題。本研究運用全奈米粒子 (all-nanoparticle) 靜電逐層 (electrostatic layer-by-layer, ELbL) 組裝技術，在玻璃基板上交替沉積7 nm TiO2與 22 nm SiO2奈米粒子，並透過以每30個雙層為一週期的週期性鍛燒製程，製備多雙層的奈米粒子薄膜： (TiO2/SiO2)x 及 (TiO2/SiO2)x+0.5，其中x=1-120。除了抗反射及自潔特性之外，也探討這種多功能奈米粒子薄膜的表面潤濕永續性。
由UV-vis穿透光譜的結果顯示本研究製備的奈米粒子薄膜都具有抗反射特性且平均穿透度皆高於玻璃。此外由橢圓偏光儀所測得的平均折射率為1.25±0.06，也驗證了製備低折射率薄膜的可能性及不同外層材料薄膜的結構相似性。然而，比較兩種不同外層材料薄膜在光催化降解膜上之矽烷自組裝單分子層展現接觸角變化時，發現外層材料具有主導性的影響。此外，本研究製備的奈米粒子薄膜不但具有天然超親水性 (靜態接觸角皆小於5o)，與純粹是TiO2的奈米粒子薄膜相比，更顯現出優異的表面潤濕永續性。實驗結果也顯示，隨著薄膜雙層數的增加，表面潤濕永續性也隨之增加。當薄膜雙層數 (x) 小於30時，SiO2為外層材料的薄膜：(TiO2/SiO2)x在暗處存放的過程中，其靜態接觸角隨時間爬升的程度相較於以TiO2為外層材料的薄膜： (TiO2/SiO2)x+0.5小，展現較佳的表面潤濕永續性。然而當 x≧60時，兩種不同外層材料的薄膜都表現出極佳的表面潤濕永續性，不同外層材料在表面潤濕永續性上的差異很小。上述薄膜雙層數及外層材料對表面潤濕永續性的影響，本研究嘗試以「外層材料效應」及「TiO2/SiO2界面效應」加以解釋。雙層數低於30的奈米粒子薄膜因為TiO2/SiO2界面不多，表面酸度提升不大，促進表面潤濕永續性的程度較小，因此表面潤濕永續性決定於「外層材料效應」。反之高達60個雙層的奈米粒子薄膜已經具備足夠的TiO2/SiO2界面，「TiO2/SiO2界面效應」主導了促進表面潤濕永續性的程度，使得不同外層材料的影響變得不顯著。本研究所製備的120.5個雙層奈米粒子薄膜，不僅平均穿透度高達94 % ；經過矽烷自組裝單分子層改質的薄膜在5.5 mW/cm2紫外光照射30分鐘後，其靜態接觸角即可從125o下降至0o；暗處存放7個月，接觸角仍然不超過13o。

Lack of transparency due to the high refractive index of TiO2 and loss of hydrophilicity in the dark are two disadvantages for TiO2 thin films in applications. The main purpose of this work is to resolve these problems. All-nanoparticle thin film coatings by electrostatic layer-by-layer (ELbL) assembly of 7 nm TiO2 and 22 nm SiO2 nanoparticles were performed on glass substrates. Followed by periodic calcination process after every 30 bilayers, multibilayer nanoparticulate thin films (TiO2/SiO2)x and (TiO2/SiO2)x+0.5 with x=1-120 can then be fabricated. Besides the antireflective and self-cleaning properties, the surface wetting sustainability in the dark is another property of the as-fabricated nanoparticulate thin films to be investigated.
Antireflective property was exhibited by all of the nanoparticulate thin films fabricated as revealed by UV-vis transmittance spectra. In addition, average refractive index of 1.25±0.06 was determined by ellipsometer. The results showed that conformal structures of multibilayer with low refractive indices can be successfully fabricated. However, the (TiO2/SiO2)x and (TiO2/SiO2)x+0.5 thin films displayed the different self-cleaning property, which was revealed by the change of the water contact angle on dodecyltrichlorosilane (DDTS)-modified surfaces as a function of time under UV illumination. The photocatalytic degradation rates were found to be strongly dependent on the top-layered material of the nanoparticulate thin films. Furthermore, experimental results showed that TiO2/SiO2 nanoparticulate thin films possess superior natural superhydrophilicity (as represented by static contact angle) as well as surface wetting sustainability (as represented by the variation of contact angle with dark storage time) than those of TiO2 nanoparticulate thin films. Experimental results also revealed that the surface wetting sustainability is enhanced with the increasing of bilayer number. When the bilayer number (x) was less than 30, SiO2 top-layered thin films, (TiO2/SiO2)x, displayed the better surface wetting sustainability than TiO2 top-layered thin films, (TiO2/SiO2)x+0.5. Nevertheless, both (TiO2/SiO2)x and (TiO2/SiO2)x+0.5 thin films showed the outstanding surface wetting sustainability when x was larger than 60. In this case, insignificant influence of top-layered materials on surface wetting sustainability is observed. The “top-layered material effect” and “TiO2/SiO2 interface effect” were then proposed to explain the results mentioned above. When the x was less than 30, the “top-layered material effect” was the dominant factor in surface wetting sustainability due to the slight influence of surface acidity in the less TiO2/SiO2 interface. On the other hand, the “TiO2/SiO2 interface effect” was the dominant factor in surface wetting sustainability due to the enough TiO2/SiO2 interface in the films when the x was larger than 60. The most satisfactory case was found for the nanoparticulate thin films with 120.5 bilayers. Average transmittance higher than 94%, static contact angle on DDTS-modified surface decreased from 125o to 0o under UV (5.5 mW/cm2) illumination in 30 min, and contact angle no exceeded 13o after the dark storage for 7 months can be realized by this nanoparticulate thin film.

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張鑑祥，楊毓民，分子層級的薄膜表面型態控制─逐層組裝技術，化工技術第12卷第9期，135-144頁，2004。

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