臺灣博碩士論文加值系統

現今在輪胎橡膠材料中混入二氧化矽奈米填充粒子已是主流，相較於傳統的碳黑作為橡膠的無機填充顆粒，擁有較好的機械性質以擴大的應用範圍。但是二氧化矽奈米填充粒子與橡膠相容性不好(二氧化矽表面有許多羥基較親水，而有長碳鏈的橡膠較親油)，再加上粉體顆粒細小表面能高又與橡膠沒有化學鍵結，更容易有團聚的現象產生，若直接用於產品將有應力集中導致材料脆弱的問題。克服的方法為加入矽烷偶合劑，該藥品分子的一端可與二氧化矽顆粒上的羥基反應並利用另一端與橡膠結合，達到形成化學鍵的目的。另外，矽烷偶合劑的添加量也是重要的考量之一，本研究先從找出適合的矽烷偶合劑添加量，再以加入增粘劑和不同的混煉製程方法來製作系列樣品，並利用熱裂解氣相層析質譜儀(Py-GC/MS)、動態機械分析儀(Dynamic Mechanical Analysis)、小角度散射(Small Angle X-ray Scattering)、穿透式電子顯微鏡(Transmission Electron Micropscope)、密煉機功率數據來分析矽烷偶合劑的反應性、奈米填充粒子分散性與最終動態性質結果。

Nowadays, it is a mainstream to use silica nanoparticles as fillers for tire rubber materials. Compared to the traditional carbon black (CB) as filler for tire rubber, silica nanoparticles have better effect on the mechanical properties of tire rubber for wider range of applications. But silica nanoparticles can not be dispersed well in rubber because the compatibility between silica and rubber is not good enough. To overcome this problem, a silane coupling agent with more than one alkoxy group at its both ends has been used for the modification. In addition, the amount of silane coupling agent is also needed to be considered. In this study, a suitable amount of coupling agent was found, and then a series of hybrid compounds were prepared by adding a tackifier and using different mixing process methods. The reactivity of the silane coupling agent, dispersibility of the silica nanoparticles and dynamic properties of tire rubbers were studied by using various techniques of Pyrolysis-GCMS, SAXS, TEM, mixing sequence and DMA.

總目錄
中文摘要…………………………………………………………….……........……i
英文摘要…………………………………………………………….…….….……..ii
致謝……………………………………………………………………………….…iv
總目錄………………………………………………………………………………....v
表目錄…………………………………………………………………….………….vi
圖目錄………………………………………………………………………….…viii
第一章 緒論……………………………………………………………………….1
1.1 前言…………………………………………………………………..1
1.2 研究動機……………………………………………………………..2
第二章 文獻回顧…………………………………………….……………………3
2.1矽烷偶合劑的添加量與反應性……………………………….....…….3
2.2矽烷偶合劑的混煉時間與反應性……………………………………..4
2.3潘恩效應(Payne effect) ………………………………………………..5
2.4矽烷偶合劑………………………………………………………….….6
2.5硫化促進劑………………………………………………………….….7
2.6混煉工藝…………………………………………………………….….8
第三章 實驗……………………………………………………………………..…10
3.1實驗藥品………………………………………………………….…...10
3.2分析儀器………………………………………………………….…...12
3.3實驗步驟………………………………………………………….…...17
3.3.1混煉實驗…………………………………………………..…...17
3.4測試方法………………………………………………………….…...19
第四章 結果與討論………………………………………………………………23
4.1矽烷偶合劑反應性………………………………………………………….…...23
4.2加入增黏劑………………………………………………………………….…...32
4.3延長混煉時間……………………………………………………………….…...44
4.4再現性………………………………………………………………….………...56
第五章 結論………………………………………………………………………65
第六章 未來工作……………………………………………………………………67
參考文獻………………………………………………………………………...….68

1.Choi, Sung-Seen. "Influence of storage time and temperature and silane coupling agent on bound rubber formation in filled styrene–butadiene rubber compounds." Polymer Testing 21.2 (2002): 201-208.

2.Baeza, Guilhem P., et al. "Multiscale filler structure in simplified industrial nanocomposite silica/SBR systems studied by SAXS and TEM." Macromolecules 46.1 (2012): 317-329.

3.Le, H. H., et al. "Effect of molecular structure on carbon black dispersion in rubber compounds: Characterization using the online measured electrical conductivity." KGK. Kautschuk, Gummi, Kunststoffe 58.11 (2005): 575-580.

4.Wang, Meng-Jiao, and Yakov Kutsovsky. "Effect of fillers on wet skid resistance of tires. Part II: experimental observations on effect of filler-elastomer interactions on water lubrication." Rubber Chemistry and Technology 81.4 (2008): 576-599.

5.Reuvekamp, Louis AEM, et al. "Effects of time and temperature on the reaction of TESPT silane coupling agent during mixing with silica filler and tire rubber." Rubber Chemistry and Technology 75.2 (2002): 187-198.

6.Clement, F., L. Bokobza, and L. Monnerie. "Investigation of the Payne effect and its temperature dependence on silica-filled polydimethylsiloxane networks. Part I: Experimental results." Rubber chemistry and technology 78.2 (2005): 211-231.

7.Ten Brinke, J. W., et al. "Mechanistic aspects of the role of coupling agents in silica–rubber composites." Composites Science and Technology 63.8 (2003): 1165-1174.

8.SUNG-HO HA , SUNG-WOO KIM and HO-KYUN JEONG. "Investigation of Reaction Rate of Bis(triethoxysilylpropyl)tetrasulphide in Silica-Filled Compound Using Pyrolysis-Gas Chromatography/Mass Spectrometry." Asian Journal of Chemistry; Vol. 25, No. 9 (2013), 5245-5250

9.K. Sengloyluan, Kannika Sahakaro, Wilma K. Dierkes, Jacobus W.M. Noordermeer. "Reinforcement Efficiency of Silica in Dependence of Different Types of Silane Coupling Agents in Natural Rubber-based Tire Compounds." Elastomer Technology and Engineering, Faculty of Engineering Technology 69 (2016): 44-53.

10.Xia, Lin, et al. "Preparation of epoxidized Eucommia ulmoides gum and its application in styrene‐butadiene rubber (SBR)/silica composites." Polymers for Advanced Technologies 28.1 (2017): 94-101.

11.鄭有舜. "X-光小角度散射在軟物質研究上的應用." 物理雙月刊 26.2 (2004): 416-424.