奈米藥物利用奈米科技改善治療成效，而中孔洞二氧化矽奈米顆粒（MSNs）為一極具潛力且備受矚目之發展中材料。本論文涵蓋功能化MSNs之設計於藥物輸送、造影與合併治療與診斷之生醫應用，以及血清蛋白與MSNs交互作用之研究。首先，我們合成表面帶有氟碳化合物之MSNs，並證明其在不同超音波參數設定下可分別應用於顯影與治療，同時探討研究材料表面性質對超音波響應之影響與機制。針對結合顯影與治療，我們設計之FePt 奈米顆粒與中空MSNs複合材料具良好生物相容性與降解性，可用於核磁造影與近紅外光熱治療，並增加癌細胞對孔洞中攜帶藥物之敏感度。
接著，我們附載Pt 氧化物（PtOx）於中空MSNs以研究Pt於生理條件下之釋放動力學以及PtOx表面之化學環境變化。結果顯示PtOx將於生理條件下逐漸釋放具毒殺癌細胞之Pt物種，可視為有潛力之新形態Pt藥物，但其治療效率將受血清蛋白吸附影響。最後，我們有系統地研究血清蛋白於一系列不同性質之MSNs之吸附行為，結果顯示吸附蛋白質總量與相對成份對血清濃度十分敏感，而表面官能基之影響僅能在相對低濃度血清觀察到，中孔結構之影響則幾可忽略。另一方面，MSNs溶解過程中形貌之變化也與血清濃度高度相關，詳細機制研究雖仍在進行中，但此現象之發現已為相關領域帶來重要新訊息。

Nanomedicine utilizes nanotechnology to provide better treatments and improve the quality of patients’ lives. Among the in progressing materials, mesoporous silica nanoparticles (MSNs) have shown great promise and are believed to be soon brought from bench to bedside. This thesis encompasses designing functionalized MSNs for drug delivery, diagnosis, theranostic, and the interplay between serum proteins and MSNs for closing knowledge gap between in vitro and in vivo conditions. Firstly, fluorocarbon functionalized MSNs were prepared and demonstrated as ultrasound (US) contrast agents, which could realize on-demand and longer-lasting imaging than clinical used MBs. Their potential uses for US-based therapy was also revealed under high-intensity focused US irradiation. Meanwhile, the mechanism and influences of textural and surface properties of MSNs on US responsiveness were also investigated. For theranostic application, a FePt NPs functionalized hollow MSNs was fabricated. The biocompatible and degradable composite could be used for MRI and NIR photothermal therapy, and the anticancer drug topotecan and photothermal effect exhibited significant synergistic effect. Next, Pt oxides (PtOx) on hollow MSNs was prepared to study the Pt releasing kinetics and changes in chemical state of the NPs for better understanding of the oxidation dissolution of the bioactive Pt species. The results unveiled dissolvable and toxic Pt releasable natures of PtOx and the potential influences from biomolecules in biological relevant media. Lastly, in attempt to provide implications for the in vivo behaviors of MSNs-based biomaterials, protein adsorption behaviors on a serial of MSNs in both in vitro and in vivo relevant conditions were investigated. The results showed that protein adsorption can be strongly affected by serum concentrations in terms of quantity and composition, whereas the surface functional group and textural property of MSNs play minor roles. In addition, it was also found that serum proteins significantly altered MSNs dissolution fashion.

Table of Content
Abstract I
Acknowledgement III
Abbreviation IV
Table of Content IX
List of Figures XIV
List of Tables XXI
Chapter 1 General Introduction 1
1.1 Nanomedicine 1
1.1.1 Brief overview 1
1.1.2 Long-established materials 2
1.1.3 In progressing silica materials 4
1.1.4 Envisagement 5
1.2 Mesoporous silica materials 6
1.2.1 Historical overview 6
1.2.2 Synthesis and mechanism 8
1.2.3 Nanonization 11
1.2.4 Structural diversity 12
1.2.5 Surface modification 13
1.2.6 Inclusion chemistry 15
1.3 Biomedical applications of functionalized MSNs 17
1.3.1 Drug delivery system 17
1.3.2 Multipurpose theranostic agents 20
1.3.3 Challenges and perspectives 21
1.4 Motivation and scope of the thesis 23
Chapter 2 Preparation of Superhydrophobic Silica Nano-particles for Ultrasound-based Biomedical Applications 26
2.1 Introduction 26
2.2 Experimental section 29
2.2.1 Chemicals 29
2.2.2 Particle synthesis and functionalization 29
2.2.3 Characterization 31
2.2.4 Ultrasound responsiveness assessment 32
2.2.5 High-speed photography 34
2.2.6 Theoretical simulation 34
2.3 Results and discussion 35
2.3.1 Characterization of particles for ultrasound imaging 35
2.3.2 Contrast efficiency 37
2.3.3 Concentration dependency and stability 38
2.3.4 Surface and textural properties on ultrasound responsiveness 39
2.3.5 Visualizing with high-speed photography 42
2.3.6 Theoretical simulation 43
2.4 Conclusions 44
Chapter 3 Hollow Mesoporous Silica Nanosphere-supported FePt Nanoparticles for Potential Theranostic Applications 45
3.1 Introduction 45
3.2 Experimental section 47
3.2.1 Materials and characterization 47
3.2.2 Sample preparations 48
3.2.3 Photothermal properties of the metal-containing samples 49
3.2.4 Metal degradation of the metal-containing samples 49
3.2.5 Cytotoxicity and in vitro photothermal efficacy 50
3.2.6 TPT loading and in vitro release 50
3.2.7 In vitro evaluation of synergistic chemo-/thermotherapy 51
3.3 Results and discussion 51
3.3.1 Preparation and characterization 51
3.3.2 Magnetic and photophysical properties 54
3.3.3 Metal degradation in buffered solutions 59
3.3.4 In vitro evaluation of photothermal efficiency 63
3.3.5 In vitro evaluation of TPT releasing and synergistic chemo/thermotherapy 65
3.5 Conclusions 67
Chapter 4 Study on the Dissolution of Hollow Mesoporous Silica Nanosphere-Supported Nanosized Platinum Oxide in Biorelevant Media for Evaluating its Potential as Chemotherapeutics 68
4.1 Introduction 68
4.2 Experimental section 71
4.2.1 Chemical and reagents 71
4.2.2 Preparation of PtOx@MMT-2 71
4.2.3 Materials characterizations 71
4.2.4 Dissolution studies 72
4.2.5 H2O2 decomposition tests 72
4.2.6 Studies on cytotoxicity and cellular uptake of PtOx@MMT-2 73
4.3 Results and discussion 74
4.3.1 Preparation and characterization of PtOx@MMT-2 74
4.3.2 PtOx@MMT-2 dissolution in biological relevant media 77
4.3.3 Changes in Pt chemical states during dissolution 82
4.3.4 Catalase-like activity 85
4.3.5 Correlation between cytotoxicity and dissolution. 86
4.4 Conclusions 88
Chapter 5 Study of Serum Protein Adsorption on Mesoporous Silica Nanoparticles 89
5.1 Introduction 89
5.2 Experimental section 92
5.2.1 Materials and characterization 92
5.2.2 Particle synthesis 93
5.2.3 Particle functionalization 94
5.2.4 Protein adsorption and complex characterization 95
5.2.5 SDS-PAGE 95
5.2.6 Cell culture and cell viability assay 96
5.3 Results and discussion 96
5.3.1 Particle characterization 96
5.3.2 Complex analysis 100
5.3.3 Analyses of the protein corona 103
5.3.3.1 Total protein quantification 103
5.3.2.2 Relative protein compositions 108
5.3.4 Influences of protein adsorption on MSNs 112
5.3.4.1 Textural properties 112
5.3.4.2 Cytotoxicity 117
5.4 Conclusions 118
Chapter 6 Conclusions and perspective 120
Chapter 7 References 122
List of Publications 147

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