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研究生： 李朝明
Alvin - Casandra
論文名稱： 離子型界面活性劑之吸附動力學研究
The Adsorption Kinetic of Ionic Surfactants
指導教授： 林析右
Shi-Yow Lin
口試委員: 張鑑祥
Chien-Hsiang Chang
劉志成
Jhy-Chern Liu
陳立仁
Li-Jen Chen
楊明偉
Ming-Wei Yang
學位類別： 博士
Doctor
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2017
畢業學年度： 105
語文別： 英文
論文頁數： 96
中文關鍵詞： 吸附動力學 、離子型界面活性劑
外文關鍵詞： Adsorption kinetics, Ionic surfactant
相關次數： 點閱：345  下載：14 
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  •  上一筆

    • 本論文探討兩個議題：離子型界劑之吸附動力學和起始逼近法(short-time approximation method)之適用條件。離子型界劑吸附動力學的研究藉著使用懸掛氣泡影像數位化測量儀測量正癸酸與正十二烷胺水溶液之動態表面張力，並將實驗所測得的動態張力數據與部分解離之離子型界劑的理論動態表面張力曲線比較，以探討離子型界劑吸附至氣-液界面的吸附動力學。文獻上雖已有論文提出離子型界面活性劑之吸附等溫線模型，但僅有少數文獻將溶液中之靜電荷作用力或在氣-液界面附近形成之電雙層對吸、脫附程序作用之效應，導入動態模型中。
    起始逼近法(short-time approximation method)是一廣為應用的簡易方法，用於決定界劑之吸附動力機構和估計界劑之擴散係數。方法簡單方便，但其適用條件與基本假設卻未曾被詳細討論。本論文藉解析動態表面張力曲線，深入探討起始逼近法之假設和適用條件。

    This dissertation focusses on two general system of interest – The adsorption kinetics of ionic surfactant and an examination on the applicability of the short-time approximation method. First, the adsorption kinetics of ionic surfactant (decanoic acid and dodeyclamine) was examined. Dynamic and equilibrium surface tensions (ST) were measured using a video-enhanced pendant bubble tensiometer. The equilibrium ST data and the complete ST relaxation profiles were compared with theoretical profiles predicted by both non-ionic and ionic models. The quasi-equilibrium approach was used in the ionic model to describe the electric field in the electrical double layer. The adsorption of decanoic acid onto the air-water interface was determined to be diffusion controlled with diffusivity of 5.5×10-6 cm2/s. In the case of dodecylamine, it has a tendency to adsorb onto solid surfaces, including the quartz cell and stainless-steel needle used in the pendant bubble system. Two modifications on the pendant bubble system and methodology were proposed: the implementation of a pumping system and the use of a coated quartz cell instead of a normal quartz cell. These modifications minimized the error in the ST measurement of aqueous dodecylamine solutions. The fitted theoretical profiles produced a diffusivity value of 0.9 - 4.0×10-6 cm2/s, which is significantly lower than the diffusivity calculated using the Wilke-Chang equation, which was D = 5.6×10-6 cm2/s. Therefore, it could be concluded that in the low surface pressure regime, the controlling mechanism of the dodecylamine adsorption process is of mixed diffusive-kinetic control.
    The short-time approximation method is known as a simple way to determine the adsorption mechanisms and to estimate the surfactant diffusivity by simply linearly fitting experimental dynamic ST data. Despite its simplicity, the short-time approximation method should be validly applied only over a very specific range of time intervals or surface pressures. Therefore, general criteria for the applicability of this method and for error evaluation in diffusivity estimations is fundamental. A theoretical numerical simulation of the short-time approximation method was conducted, and general benchmarks for its accurate utilization were investigated. Simple rules were developed in terms of limiting surface pressure and dimensionless time as a function of dimensionless surfactant concentration. For values greater than the limiting conditions, the dynamic ST curve deviates from the short-time approximation straight line, and thus, the corresponding linear fitting could lead to significant errors in evaluating the diffusivity. The simple criteria proposed in this study thus define the range of applicability for the short-time approximation method.

    摘要 Abstract Acknowledgements Table of Contents List of figures List of tables Chapter 1 – Introduction 1.1 Objectives 1.2 Outline Chapter 2 –Literature Review 2.1 Surfactant 2.2 The classification of surfactant 2.2.1 Anionic surfactant 2.2.2 Cationic surfactant 2.2.3 Nonionic surfactant 2.2.4 Zwitterionic surfactant 2.3 Surface tension 2.4 Why surfactant reduce the surface tension? 2.5 The application of surfactants 2.6 How to measure surface tension? 2.7 Surface Tension Measurement Method 2.7.1 Wilhelmy plate and du-Nouy ring 2.7.2 Drop weight/volume method 2.7.3 Maximum bubble pressure method 2.7.4 Pendant Bubble/Drop method 2.8 Young-Laplace equation 2.9 Pendant Bubble apparatus Chapter 3 –Theoretical Framework 3.1 Surfactant mass transfer 3.2 Modified Ward-Tordai equation 3.3 Adsorption-desorption equation 3.4 Numerical solution Chapter 4 –Adsorption Kinetics of the Ionic Surfactant Decanoic Acid 4.1 Background and Introduction 4.2 Materials 4.3 Experimental procedure 4.4 Result 4.4.1 Surface tension 4.4.2 Model determination 4.4.3 Diffusion-controlled adsorption of decanoic acid 4.4.4 Dynamic surface properties and surface potential 4.4.5 Dissociation degree of decanoic acid 4.4.6 Critical K value for ionic surfactant 4.4.7 Equilibrium surface potential Chapter 5 –Adsorption Kinetics of Dodecylamine 5.1 Background and Introduction 5.2 Materials 5.3 Experimental procedure 5.3.1 Modified pendant bubble apparatus 5.3.2 Modified experimental procedure 5.3.3 Ellipsometer 5.4 Result 5.4.1 Quartz cell effect on the surface tension measurement 5.4.2 Needle effect on the surface tension measurement 5.4.3 Multilayer thickness 5.4.4 Dissociation degree of dodecylamine 5.4.5 Surface tension 5.4.6 Model determination 5.4.7 Diffusion-controlled adsorption of dodecylamine 5.4.8 Diffusion-controlled adsorption of dodecylamine - low surface pressure 5.4.9 Mixed-controlled adsorption of dodecylamine - low surface pressure 5.4.10 The effect of salt concentration on the adsorption of dodecylamine Chapter 6 –A Study on the Method of Short-Time Approximation 6.1 Background and Introduction 6.2 Short-time linear approximation method 6.3 Short-time approximation theoretical examination results 6.4 The effect of surfactant concentration on short-time approximation 6.5 Criteria for short-time approximation 6.6 The effect of surfactant activity (a) on short-time approximation 6.7 Criteria comparison with literature 6.8 The effect of interfacial curvature 6.9 An examination on the interfacial curvature effect on short-time approximation 6.10 An Examination on the three assumptions used in short-time approximation Chapter 7 –Conclusions and Future Work 7.1 Conclusion 7.2 Future work References

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