本博士論文，從臨床最主要的三個面向為出發點：診斷、治療、預防，針對神經外科臨床上可能遇到的困難問題做發想，結合奈米生醫材料的新穎技術，嘗試發展出解決方案。包括三個主題：表面增益拉曼光譜為基礎之腦脊髓液超靈敏檢測平台，臨床應用作為腦脊髓液即時藥物濃度監控；腦部惡性膠質瘤之奈米金水膠局部藥物釋放載體；泛用型塗層技術作為植入性醫材如腦室外引流管之抗菌應用。
腦脊髓液的生化分析與生物標記物的變化，往往較血漿更能精準反映中樞神經系統疾病所造成的影響。然而，除一般的生化因子外，臨床上並無一常規且靈敏準確的腦脊髓液化學分析工具。因此，本論文的第一部分為借助奈米金屬結構加強表面電漿共振效應，製作開發一表面增益拉曼光譜 (Surface enhanced Raman spectroscopy, SERS) 為基礎的檢測平台，並成功在臨床病人的腦脊髓液中達到即時藥物監控的成果。
腦部惡性膠質瘤是死亡率極高的癌症，其中最惡性的腦部膠質母細胞瘤，中位數存活時間更是只有14.6個月。本論文的第二部分則開發一種蠶絲水膠-金奈米粒子複合系統，作為腦部膠質瘤局部化療藥物的載體，利用蠶絲水膠的高度生物相容性以及金奈米粒子獨特的光熱效應，可在腫瘤原位以白光源進行成膠以傳遞藥物，並克服市售局部藥物載體 (Gliadel Wafer) 的缺點，如：水解不均、嚴重的局部發炎反應、攜帶治療藥物劑量需較大空腔、無法完全貼合手術切除後的接觸面等。最後，成功以小鼠動物模型驗證此蠶絲水膠奈米金複合物之藥物緩釋與腫瘤細胞毒殺的效果。
植入性醫材造成的醫源性感染，是臨床醫療中相當嚴重卻有機會避免的一項併發症。除了在醫療處置流程的無菌技術與抗生素的使用外，生物膜的生成被認為是植入性醫材感染的重要原因之一，因此有許多針對抑制生物膜的研究，但臨床上仍有許多瓶頸。本論文的第三部分則利用濕式化學法將奈米銀陣列自組裝於各式高分子與金屬植入性醫材上，展現對於臨床常見的院內感染菌，大腸桿菌、綠膿桿菌與金黃色葡萄球菌之抗生物膜(anti-biofilm)效果。
整體而言，從神經外科醫師角度出發，針對臨床醫療困難而未被滿足的需求，結合奈米生醫材料，在三個不同的面向：診斷、治療、預防，展現出具備潛力的研究成果。

This doctoral dissertation focuses on three main aspects of clinical practice: diagnosis, treatment, and prevention. We aim to address the challenging problems encountered in neurosurgery by integrating innovative biomedical nanomaterials to develop solutions. The study comprises three themes:
First, an ultra-sensitive cerebrospinal fluid (CSF) detection platform based on surface-enhanced Raman spectroscopy (SERS). The biochemical analysis of CSF and changes in biomarkers often provide a more accurate reflection of the impact of central nervous system (CNS) diseases compared to plasma analysis. However, apart from general biochemical factors, there is no routinely used, sensitive, and precise tool for CSF analysis in clinical settings. Therefore, we have developed a detection platform based on SERS by utilizing the enhancement of surface plasmon resonance effects through nanometallic structures. This platform has been successfully employed for real-time therapeutic drug monitoring in the CSF of clinical patients.
Second, a white-light activated nanogold-silk hydrogel complex serving as a localized drug delivery system for treating malignant gliomas. This section investigates the potential of this innovative system for therapeutic drug administration in glioblastoma after tumor resection. Malignant gliomas are highly fatal brain cancers, with the most aggressive form, glioblastoma, having a median survival time of only 14.6 months. We developed a silk hydrogel-gold nanoparticle (AuNPs) composite system as a local drug delivery system for the treatment of brain gliomas. Leveraging the high biocompatibility of silk fibroin hydrogels and the unique photothermal effects of AuNPs, I seek to overcome the limitations of commercially available local drug carriers, such as Gliadel Wafer. These limitations include uneven hydrolysis, severe local inflammation, the need for larger cavities to hold therapeutic drug doses, and the inability to fully conform to the contact surface following surgical resection. I validated the controlled drug release and cytotoxic effects of this silk hydrogel-nanogold composite on tumor cells using a mouse animal model.
Third, a universal coating technology employing nano-silver particles to inhibit biofilm formation in implantable medical devices, such as ventricular drainage catheters. Healthcare-associated infections (HAIs) caused by implanted medical devices are severe yet preventable complications in clinical medicine. In addition to aseptic techniques and antibiotic use during medical procedures, biofilm formation is considered one of the main causes of implant-associated infections. Although many studies have focused on inhibiting biofilm formation, clinical applications still face several bottlenecks. In this part, we utilized a wet chemical method to assemble nano-silver particle arrays on various polymer and metal implanted medical devices. This arrays demonstrate anti-biofilm effects against common nosocomial infection-causing bacteria, including Escherichia coli (E. coli), Pseudomonas aeruginosa (P. aeruginosa), and Staphylococcus aureus (S. aureus). This theme focuses on developing a novel coating method to prevent infections associated with implanted medical devices.
In summary, approaching from the perspective of a neurosurgeon, I address unmet clinical needs and challenges by integrating nanotechnology into our research. I demonstrate promising results in three distinct aspects: diagnosis, treatment, and prevention, showcasing the potential of these innovative solutions to improve patient outcomes and advance the field of neurosurgery.

摘要.............................................................I
ABSTRACT.........................................................III
LIST OF ABBREVIATION.............................................VI
TABLE OF CONTENTS................................................VIII
LIST OF FIGURES..................................................X
LIST OF TABLES...................................................XIV
CHAPTER 1 INTRODUCTION............................................1
1.1 Research Motivation...........................................1
1.2 Research Scheme...............................................3
CHAPTER 2 REVIEWS OF LITERATURES..................................5
2.1 Nanotechnology and Nanomaterials in Neurosurgery..............5
2.1.1 Nanoneurosurgery............................................5
2.2 Diagnostics:..................................................6
2.2.1 Clinical Unmet Need: Precision Medicine.....................6
2.2.2 Surface-enhanced Raman Sputtering (SERS)....................8
2.3 Treatment:....................................................10
2.3.1 Clinical Unmet Need: Glioblastoma Treatment.................10
2.3.2 Local Drug Delivery System..................................12
2.3.3 Hydrogel as Local Drug Delivery System......................14
2.4 Prevention: Clinical Unmet Need...............................17
2.4.1 Clinical Unmet Need: Healthcare-associated Infections.......17
2.4.2 Current Advancement of Nanotechnology in The Area of Infection Control ..........................................................19
CHAPTER 3.........................................................22
3.1 Introduction..................................................22
3.1.1 The Portable Raman Spectrometer and The Concept of Fabrication of Ultrasensitive SERS Substrate..................................22
3.1.2 Flexible Fibrous Substrates as SERS Substrate...............25
3.1.3 Our Work....................................................28
3.2 Materials and Methods.........................................31
3.3 Results and Discussions.......................................38
3.3.1 Mechanism of Nanoparticle Formation Mediated by Atomic Behavior on the Substrate..................................................38
3.3.2 Characteristics of Nanostructures Grown on the Surface......41
3.3.3 Optimization of SERS Paper..................................50
3.3.4 Confirmation of Paper-Based SERS Substrates.................55
3.3.5 Rapid Therapeutic Drug Monitoring in CSF Utilizing Paper-based SERS Substrates ..................................................64
3.3.6 Early Diagnosis of Pesticide Intoxication via Paper-Based SERS Substrates........................................................68
3.4 Conclusion....................................................72
CHAPTER 4.........................................................73
4.1 Introduction..................................................73
4.1.1 Silk Hydrogel...............................................73
4.1.2 Gelation Process for Silk Hydrogel..........................74
4.1.3 Exploitation of The Photothermal Phenomenon for Inducing Gelation..........................................................74
4.1.4 Our Study ..................................................76
4.2 Materials and Methods.........................................77
4.3 Results and Discussions.......................................84
4.4 Conclusion....................................................101
CHAPTER 5.........................................................102
5.1 Introduction..................................................102
5.1.1 Universal Coating Method....................................102
5.1.2 Ours Work ..................................................104
5.2 Materials and Methods.........................................107
5.3 Results and Discussions.......................................118
5.3.1 Substrate-Independent Immobilization of Monolayer Metal Nanoparticle Arrays Through TMS Silanization......................118
5.3.2 Characterization of TMS Layer on Various Surfaces...........121
5.3.3 Immobilization of Metal NP Arrays on TMS-Treated Surfaces...125
5.3.4 Anti-biofilm Activity of Monolayer AgNP Arrays..............130
5.3.5 Chemical activity of monolayer AgNP arrays..................136
5.3.6 Cytocompatibility of monolayer AgNP arrays..................140
5.3.7 Functionalization of monolayer metal NP arrays on various clinical devices..................................................142
5.4 Conclusion....................................................145
CHAPTER 6 CONCLUSION..............................................146
REFERENCE.........................................................151
PUBLICATION LIST..................................................167

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