本論文係關於近紅外光光熱轉換複合奈米粒子之製備並探討其表面增強拉曼散射顯影引導光熱轉換效應於致病菌及癌細胞光熱治療及顯影的應用。本論文內容包括兩個主題(一)製備Fe3O4/Au/PPy(-PVP)複合奈米粒子，並探討其在SERS顯影引導近紅外光光熱殺菌之應用。(二) 製備有機金屬骨架(MIL-100)披覆Fe3O4/Au/PPy(-PVP)複合奈米粒子，並探討其在SERS顯影引導近化學/光熱對癌症合併治療之應用。
第一部分研究製備Fe3O4/Au/PPy(-PVP)複合奈米粒子。利用顯影技術來引導光熱治療提升光熱治療時的精確度以及治療效率，表面增強拉曼散射(surface-enhanced Raman scattering，SERS) 顯影因其具高穩定度、低背景值干擾與深層組織顯影的優點，其應用於癌症顯影及細菌偵測方面的應用已被廣泛討論，而要發展具低毒性、簡單製備、結構穩定的SERS標定分子以及結合電漿奈米粒子為未來發展的重點。本研究利用簡單的方式將聚吡咯披覆於氧化鐵/金複合奈米粒子來開發一種具SERS顯影以及光熱轉換效果的多功能奈米粒子。Fe3O4/Au/PPy(-PVP)具有優良的近紅外光吸收及光熱轉換效果，此外Fe3O4/Au/PPy(-PVP)在照射785 nm雷射下表面出現聚吡咯之SERS訊號，因此可證明聚吡咯確實可做為SERS的標定分子，藉由聚吡咯的SERS訊號，與Fe3O4/Au/PPy(-PVP)結合的E.coli即可產生SERS顯影，另外，在照射近紅外光下，Fe3O4/Au/PPy(-PVP)利用光熱效果有效的降低細菌的生存率。本研究開發出Fe3O4/Au/PPy(-PVP)確實具有應用於SERS顯影引導近紅外光光熱殺菌之功能。
第二部分研究製備有機金屬骨架(MIL-100)披覆Fe3O4/Au/PPy(-PVP)複合奈米粒子。發展具有診斷以及治療功能的複合奈米粒子成為癌症治療藥物已受到許多的關注，本研究欲結合有機金屬骨架(MOF)與功能性奈米粒子作為發展多功能奈米平台的藥物，MIL-100為以鐵為中心元素的MOF結構，其具有生物相容性、多孔洞的特性能夠作為藥物的載體，因此本研究將第一部分的Fe3O4/Au/PPy(-PVP)進一步披覆MIL-100來發展一種具有光熱-化學治療以及SERS顯影的多功能奈米平台。Fe3O4/Au/PPy/MIL-100保有SERS特性、優良的近紅外光吸收及光熱轉換效果，在近紅外光照射下，裝載DOX藥物的Fe3O4/Au/PPy/MIL-100產生光熱效果消融癌細胞，同時加速藥物的釋放，因此可大幅提升癌症治療的效果。另外，在Fe3O4/Au/PPy/MIL-100被HeLa吞噬後，在拉曼光譜儀使用785 nm雷射光下能夠顯現聚吡咯的SERS訊號，因此可證明Fe3O4/Au/PPy/MIL-100複合奈米粒子能夠進行癌細胞的SERS顯影。本研究開發的Fe3O4/Au/PPy/MIL-100具有SERS顯影引導化學/光熱癌症合併治療，在開發癌症治療藥物具有十分的潛力。

This thesis concerns the fabrication of multifunctional nanomaterials for SERS imaging-guided photothermal therapy. The contents include two parts. (1) Fabrication of multifunction Fe3O4/Au/PPy(-PVP) composite nanoparticles for SERS imaging-guided NIR photothermal ablation of bacteria (2) Fabrication of multifunction Fe3O4/Au/PPy/MIL-100 composite nanoparticles for SERS imaging-guided NIR chem/photothermal therapy.
In the first part concerns the fabrication of fabrication of multifunction Fe3O4/Au/PPy(-PVP) composite nanoparticles. The imaging-guided therapy largely enhaces the therapeutic efficiency of photothermal therapy. Also, SERS imaging is emerging as attractive bioimaging techniques due to its photostability, low background signal interference and high penetration into tissue, thus, the application of SERS imaging for cancer or bacteria diagnosis have been widely investigated. To develop the SERS probe with the properties of low toxicity, simple fabrication and structure stability is the future challenge. In this study, the simple method to integrate SERS probe and functional nanomaterial was developed. The combination of Fe3O4/Au/PPy(-PVP) have been fabricated as a magnetically manipulable multifunctional platform for the SERS imaging-guided NIR photothermal killing of bacteria. The Fe3O4/Au/PPy(-PVP) were demonstrated that Fe3O4/Au/PPy(-PVP) indeed possessed an excellent NIR photothermal conversion ability and Fe3O4/Au/PPy(-PVP) exhibited the remarkable Raman signal of polypyrrole under 785 nm laser because Fe3O4/Au composite nanoparticles were SERS active and polypyrrole could act as a probe. By SERS analysis, the E. coli with and without the binding of Fe3O4/Au/PPy(-PVP) could be differentiated. This demonstrated their potential application in the SERS imaging. Under the 808-nm laser irradiation, their presence could effectively lead to the death of E. coli, revealing their capability in NIR photothermal ablation of bacteria. Accordingly, the Fe3O4/Au/PPy(-PVP) developed in this study are expected to be useful in the SERS imaging-guided NIR photothermal killing of bacteria.
In the second part, the multifunctional therapeutic nanoplatforms via integrating diagnosis and therapy have attracted broad attention. Also, integrating metal-organic frameworks and other functional material is a promising way to develop the multifunctional therapeutic nanoplatforms. The MOF structure of MIL-100 possesses high porosity and biocompatibility which is of great value as nanocarriers for drug delivery. Hence, the novel Fe3O4/Au/PPy/MIL-100 have been successfully fabricated as a multifunctional platform for the chem/photothermal tharapy and SERS imaging. It was demonstrated that the Fe3O4/Au/PPy/MIL-100 indeed possessed an excellent NIR photothermal conversion ability and they still maintain the SERS property of polypyrrole. Under the 808 nm laser irradiation, Fe3O4/Au/PPy/MIL-100-DOX were able to photothermally ablate cancer, and the DOX release dramatically increase at the same time which further improved the efficiency of therapy. By SERS analysis, it showed the remarkable Raman signal of polypyrrole in cancer cell. This demonstrated their potential application in the SERS imaging. Accordingly, the novel Fe3O4/Au/PPy/MIL-100 developed are expected to be multifunctional therapeutic nanoplatforms with the capability of SERS imaging-guided chem/photothermal therapy combinational therapy of cancer.

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