唑來膦酸三水合物的初始溶劑篩選和在羥基磷灰石之表面吸附行為

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林貫雲(Kuan-Yun Lin) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

唑來膦酸三水合物的初始溶劑篩選和在羥基磷灰石之表面吸附行為
(Initial Solvent Screening and Adsorption Behaviors of Zoledronic Acid Trihydrate on Hydroxyapatite Surface)

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摘要(中)

雙膦酸鹽Bisphosphonate（BP）是一類用於治療和預防很多種骨疾病重要的藥物，尤其是用於骨質疏鬆症，由於這些藥物對鈣離子的親和力很強，磷酸鈣（如羥基磷灰石（HA））是研究吸附行為的理想材料。我們的目的是通過TGA、DSC和PXRD技術研究不同的固態形態的唑來膦酸水合物，並通過一些動力學模型和等溫吸附模型研究唑來膦酸三水合物對羥基磷灰石的吸附行為。唑來膦酸水合物的固態可通過加濕，乾燥或冷卻方法轉化為任何型態的唑來膦酸水合物，我們還針對唑來膦酸三水合物，其為唑來膦酸水合物的穩定形式，進行初始溶劑篩选和溶解度測試，以找出吸附實驗的最佳參數。研究了初始唑來膦酸三水合物濃度，接觸時間，溫度，pH值對羥基磷灰石吸附量的影響。Pseudo-second-order模型(R2>0.99) 可以很好地描述吸附動力學，表明了化學吸附的發生，吸附動力學可能是受邊界層擴散控制。同時，實驗數據使用Languir等溫模型(R2>0.99)比Freundlich和Dubinin-Radushkevich等溫模型可以更好的擬合本研究的吸附行為，表現出吸附特徵是單層吸附。吸附焓為40.3kJ / mol，表明吸附為吸熱過程。

摘要(英)

Bisphosphonates (BPs) are well established as an important class of drugs for the treatment and prevention of several bone disorders especially for osteoporosis. Due to the great affinity of these drugs for calcium ions, calcium phosphates such as hydroxyapatite (HA) are the ideal material for studying behaviors of the adsorption. Our aims are to investigate different solid-state forms of zoledronic acid hydrates by TGA, DSC and PXRD techniques, and to study the adsorption behaviors of zoledronic acid trihydrate on hydroxyapatite by several kinetics and isotherm models. The solid-state of zoledronic acid hydrate could be transformed into any desired form by using humidification, drying or cooling method. We also aimed to zoledronic acid trihydrate, which is the stable form of zoledronic acid hydrate, conducting initial solvent screening and solubility test in order to find out the optimal parameters for the adsorption experiment. Effects of initial zoledronic acid trihydrate concentration, contact time, temperature, pH on the adsorption capacity of hydroxyapatite were investigated in detail. The adsorption kinetics could be well described by the pseudo-second-order model (R2>0.99) which indicated the occurrence of chemisorption, and the adsorption kinetics might be controlled by boundary layer diffusion. Meanwhile, the experimental equilibrium data were fitted the best by using the Langmuir model (R2>0.99) rather than the Freundlich and Dubinin-Radushkevich isotherm models, suggesting that the adsorption feature might be in the fashion of monolayer. The adsorption enthalpy was 40.3 kJ/mol depicting the adsorption exhibited endothermic process.

關鍵字(中)

★ 雙膦酸鹽
★ 唑來膦酸
★ 羥基磷灰石
★ 吸附

關鍵字(英)

★ bisphosphonates
★ zoledronic acid
★ hydroxyapatite
★ adsorption

論文目次

Table of Contents
摘要 I
Abstract II
Acknowledgement III
Table of Contents IV
List of Figures VII
List of Tables XII
Chpater 1 Executive Introduction 1
1.1 Brief Introduction of Adsorption 1
1.2 Brief Introduction of Bone Resorption 3
1.3 Bisphosphates 4
1.4 Calcium Phosphates as Delivery Systems 8
1.5 Conceptual Framework 10
1.6 References 11
Chpater 2 Materials and Experiments 15
2.1 Materials 15
2.2 Experimental Methods 17
2.2.1 Preparation of Zoledronic Acid Trihydrate by Humidification 17
2.2.2 Initial Solvent Screening 18
2.2.3 Cooling Crystallization 19
2.2.4 Adsorption of Zoledronic Acid Trihydrate on Hydroxyapatite 19
2.3 Isotherm Adsorption Models 21
2.3.1 Langmuir Adsorption Isotherm 21
2.3.2 Freundlich Adsorption Isotherm 23
2.3.3 Dubinin-Radushkevich Isotherm 25
2.4 Instruments 27
2.4.1 Microscopic Methods 27
2.4.2 Thermal Analysis Methods 32
2.4.3 Spectroscopic Methods 37
2.4.4 Crystallographic Analysis Methods 40
2.4.5 Surface Analysis Method 42
2.5 References 44
Chpater 3 Results and Discussion 47
3.1 Characterization of Anhydrous Zoledronic Acid, Zoledronic Acid Monohydrate, and Zoledronic Acid Trihydrate 47
3.1.1 Thermal Analysis 47
3.1.2 Crystal Habits 51
3.1.3 PXRD Patterns 52
3.1.4 Solubility 55
3.2 Characterization of Hydroxyapatite 58
3.2.1 PXRD Patterns 58
3.2.2 SEM Images and BET Surface Analysis 59
3.2.3 FTIR Analysis 62
3.3 Adsorption Behaviors of Zoledronic Acid Trihydrate of Hydroxyapatite surface 64
3.3.1 pH Study 64
3.3.2 Adsorption Kinetics 66
3.3.3 Adsorption Isotherms 70
3.3.4 Thermodynamic study 74
3.4 References 76
Chpater 4 Conclusions and Future Work 79
4.1 Conclusions 79
4.2 Future work 81

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指導教授

李度(Tu Lee)

審核日期

2019-7-25

推文