以磁性奈米顆為基礎之腫瘤治療方法，近年來逐漸為世人所關注。其特點在於可利用外部直流磁場固定顆粒位置，藉由其在交流磁場下自發熱性質，將腫瘤加熱至42 oC ~46 oC，以達到抑制及殺死腫瘤之目的。此種具標靶性、集中性、非侵入性及無副作用之治療技術，稱之為磁性腫瘤溫熱法。近年來利用磁性奈米顆粒作為藥物載體，於體外控制藥物釋放，不僅可有效去除腫瘤，也可大量降低藥物之投入劑量，因此利用磁性顆粒進行發熱，成為各國發展腫瘤治療技術之ㄧ。
整合各項研究得知，為了獲得高發熱能力之磁性奈米顆粒，必須同時考慮顆粒尺寸、尺寸分佈、磁異方性三者因子。最新的研究證實，利用有機相高溫高壓方法，合成出尺寸在15 nm、尺寸分佈極窄且磁異方性在15000 Jm-3~18000Jm-3範圍內之奈米顆粒，在其分散狀態下所產生之發熱能力已遠遠高於臨床應用最低所需。然而in vitro及in vivo研究顯示，奈米顆粒不可避免會受到腫瘤細胞吞噬/吸附作用聚集在細胞內/外，如此強烈抑制顆粒之發熱能力，也可能影響藥物釋放效率。雖然如此問題可藉由增加磁場強度而解決，但往往必須施加必須超過人體十幾倍之始可產生治療效果。因此為了實現磁性溫熱法臨床應用目標，如何在安全磁場下提高聚集態顆粒之發熱能力，成為急待克服之問題。
根據磁性奈米顆粒應用於高密度資料儲存裝置之研究，利用正交型雙磁場取代傳統單一磁場源，可在低磁場下達到資料高速讀取/儲存之實用目標。根據此原理，我們提出以雙磁場系統概念來改善目前顆粒聚集低發熱能力之問題。為了系統性調查雙磁場所產生之效應，我們利用Landau-Lifshitz-Gilbert方程式，計算奈米顆粒磁矩在不同磁場下之動態發熱行為。模擬結果顯示，顆粒在雙磁場之發熱能力明顯高於施加傳統單一磁場。藉由模擬條件，我們設計製造正交型相位同步雙磁場系統，利用簡單、便宜及具環保之化學共沉降法，合成出各種不同之磁性奈米顆粒，比較這些顆粒聚集狀態時在雙磁場與傳統磁場之發熱能力。實驗結果顯示，在相同磁場條件下，聚集態超順磁性顆粒，其在雙磁場之發熱能力明顯高於單磁場4~5倍之多。隨著顆粒尺寸增加至鐵磁性性質範圍，單磁場強度必須超越矯頑力顆粒始可產生熱能，但使用雙磁場卻不受矯頑力所限制。另外，在單磁場下顆粒發熱能力隨著尺寸分佈加寬而大受影響，然而在雙磁場下，樣品發熱能力不僅顯著提高，同時尺寸分佈之影響僅為單磁場1/10。再者，高磁異方性磁性材料(例如CoFe2O4)在單磁場之低發熱能力，卻在雙磁場下可提高11倍。最後，我們利用修飾幾丁聚醣之磁性奈米顆粒作為藥物載體，進行酚酸類抗氧化劑釋放試驗，結果顯示雙磁場不僅快速提高介質溫度，同時也加速藥物釋放速率，此結果聯想到，利用雙磁場系統具有治療急性疾病之可能性。總和上述結果，雙磁場系統之優勢，在於高發熱能力之磁性奈米顆粒，無須藉由昂貴、耗能及高污染方法合成。即使使用寬的尺寸分佈及磁異方性範圍之顆粒，均可使用作為發熱種子，簡化了磁性溫熱法發展過程，更重要的降低病人治療時負擔。因此我們預期，雙磁場系統可能成為未來腫瘤治療之利器。

The self-heating property of magnetic nanoparticles (MNPs) under single magnetic field has been a promising candidate for tumor therapy due to its non-invasive and targetable property. Recent studies showed that the heating ability of MNPs under single field was significantly influenced by particle size, size distribution and magnetic anisotropy. MNPs were prepared under these optimal parameters to maximize heating ability. However, the present challenge lies in the fact that the heating ability of MNPs was inevitably attenuated by the immobilization and aggregation of MNPs in tumor cells. To improve the problem, we proposed a new orthogonally synchronous bi-directional AC magnetic field (OSB field). The concept of the system was derived from the application of MNPs to the high density storage device. The numerical and experimental investigations showed that the poor heating ability of aggregated MNPs with superparamagnetic property under single field was significantly enhanced by applying OSB field. The large MNPs in size used could generate strong heating ability and reduce the influence of biocompatible surfactant under OSB field. We found that the enhanced effect on the heating ability of ferromagnetic MNPs was not limited even though applying lower strength than the coercivity. Moreover, applying OSB field could significantly weaken the influence of size distribution to only 1/10 of that under single field. We also proved that poor heating ability of CoFe2O4 MNPs under single field were not suitable as thermal seeds due to its high magnetic anisotropy. However, such the magnetic material could generate heat 11 times more than that under single field. Finally, we firstly used OSB field to magnetically control the phenolic acid release from Fe3O4@chitosan nano-carriers. The results showed that applying OSB field promoted the release of model drug from nano-carriers and the rate of drug release was about 3 times quicker than that under single field without increasing field strength. In addition to Fe3O4, CoFe2O4 MNPs were also suitable as nano-carriers for drug-release. This major was attributed to the outstanding heating abilities of both MNPs under the OSB field. From the results, the advantage of applying OSB field lies in the fact that a variety of MNPs can be served as strong thermal seeds even though these nanoparticles are prepared by simple and low-cost procedures and present a broad size distribution and magnetic anisotropy. Therefore, we expect that OSB field is a promising tool for tumor therapy.

論文審定書 i
謝誌 ii
中文摘要 iii
Abstract v
TEXT CONTENT vii
Figure Content x
Table Content xv
1 Introduction 1
1.1 Magnetic hyperthermia (MHT) 1
1.2 Heating mechanisms of magnetic nanoparticles on MHT 1
1.3 The influences of parameters on the heating abilities of MNPs 2
1.4 The current issues of MHT under the traditional magnetic field 3
1.5 Our study 6
2 Materials and Methods 9
2.1 Simulation method and conditions 9
2.2. The simulated magnetic properties and power dissipation of MNPs under AC field 12
2.3. Construction of OSB magnetic field system 15
2.4. The preparation and characterization of superparamagnetic nanoparticles 17
2.5. The preparation and characterization of different iron oxide MNPs in size distribution 20
2.6. Preparation and characteristics of Fe3O4 and Fe3O4@chitosan nanoparticles 20
2.7. The measurement of AC magnetization curve of MNPs 21
2.8. Preparation and characterization of chitosan coated magnetic nanoparticles for drug release experiments 22
2.9. The preparation of phenolic acid functionalized MNPs 22
2.10. Determination of the scavenged amount of DPPH by phenolic acid 22
2.11. D Measurement of the amount of released drug under OSB and single field 23
3 Results and Discussion 24
3.1 The numerical simulation of magnetic nanoparticles under OSB and single field 24
3.1.1 Heating and magnetization property of aggregated MNP 24
3.1.2 Imaginary susceptibility 27
3.1.3 Internal energy 29
3.1.4 Summary 29
3.2 Construction of OSB field 31
3.2.1 Output waveforms of OSB field 31
3.2.2 Summary 33
3.3 The effect of superparamagnetic nanoparticles on the heating properties under OSB field 35
3.3.1 Magnetic properties of synthesized MNPs 35
3.3.2 Heating abilities of synthesized MNPs under single field 35
3.3.3 Heating abilities of synthesized MNPs under OSB field 41
3.3.4 Summary 43
3.4 The effect of ferromagnetic nanoparticles on the heating properties under OSB field 44
3.4.1 The characterization of synthesized MNPs 44
3.4.2 The heating properties of MNPs under traditional single field 47
3.4.3 The heating properties of ferromagnetic MNPs under OSB field 47
3.4.4 Summary 51
3.5 The effect of size distribution on the heating properties under OSB field 52
3.5.1 The characterizations of synthesized MNPs with different size distributions 52
3.5.2 The heating abilities of MNPs with different size distribution under single field 52
3.5.3 The heating abilities of MNPs with different size distribution under OSB field 55
3.5.4 Summary 56
3.6 The effect of magnetic anisotropy on the heating properties under OSB field 60
3.6.1 The characterization of as-synthesized CoFe2O4 MNPs 60
3.6.2 The heating properties of CoFe2O4 MNPs under single field 62
3.6.3 The heating properties of CoFe2O4 under OSB field 62
3.6.4 Summary 65
3.7 The effect of surfactant on the heating properties under OSB field 66
3.7.1 Result and Discussion 66
3.7.2 The heating properties of MNPs under single field 71
3.7.3 The heating abilities of aggregated MNPs under OSB field 71
3.7.4 The influence of surfactant on heating abilities of MNPs 74
3.7.5 The improvement for the influence of surfactant on heating abilities of MNPs 76
3.7.6 Summary 77
3.8 The application of OSB field on the magnetically controlled drug release 80
3.8.1 The characterization of synthesized chitosan coated Fe3O4 MNPs 80
3.8.2 Determination of antiradical activities of gallic acid and caffeic acid by DPPH method 83
3.8.3 The release of gallic acid and caffeic acid under OSB and single field 85
3.8.4 The kinetic rate of releasing gallic acids under OSB and single field 91
3.8.5 The use of other magnetic nano-carrier on the release under OSB field 91
3.8.6 Summary 94
4 Conclusion 96
5 Reference 98

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