臺灣博碩士論文加值系統

近年來由於抗生素的濫用，導致抗藥性細菌的增加，成為一個對人類健康具潛在威脅的隱憂。本研究以二維過渡金屬鈦碳化物(Ti3C2Tx MXene)與銅離子混合，形成奈米複合材料 (Cu/MXene) 作為新型抗菌劑之應用。Ti3C2Tx MXene為過渡金屬Ti與輕元素C和H所組成的複合原子層二維化合物，易與菌膜表面作用。此外，藉由Ti3C2Tx MXene易與金屬離子鍵結，將銅離子吸附於Ti3C2Tx MXene，可保留銅離子特性，達到協同作用並提升抑菌之功效。此材料抗菌活性對大腸桿菌、金黃色葡萄球菌及耐甲氧西林金黃色葡萄球菌(MRSA)皆具有很好的抑菌效果，且與Ti3C2Tx MXene相比，Cu/MXene所產生的過氧化氫量(H2O2)增加約十倍左右，其能夠造成菌膜表面氧化壓力上升，再協同Ti3C2Tx MXene本身以鋒利邊緣與細菌表面作用特性，增加對細菌的物理壓力，進而增強材料的抗菌能力。同時，由於Ti3C2Tx MXene本身具有良好的光熱轉換效率，透過照射808 nm雷射，能使Cu/MXene溫度上升(58 oC)並增加H2O2產生值，進而增加抗菌之功效。體外細胞毒性結果揭示了Cu/MXene的高生物相容性。為了證明其實際應用，在小鼠 (C57BL/6) 中進行了體外 MRSA 感染的傷口癒合研究，證明當Cu/MXene作敷料，可有效清除傷口上細菌並加速膠原纖維形成，使癒合速度更快，並加速膠原纖維形成。我們的結果證實此具有光熱特性及生物相容性之二維型奈米複合抗菌劑，具有商業價值。

In recent years, the abuse of antibiotics has led to an increase in drug-resistant bacteria, which has become a potential threat to human health. Therefore, it is in urgent need of developing an alternative to traditional antibiotic therapy. In this study, copper ions adsorption to two-dimensional transition metal titanium carbide (Ti3C2Tx MXene) forming a nanocomposite (Cu/MXene) is used as a new antibacterial agent. Ti3C2Tx MXene is a two-dimensional compound and its atomic layers composed with transition metal Ti and light elements C and H, which is easy to interact with bacterial membrane. In addition, Ti3C2Tx MXene is reactive with metal ions, while the adsorption of copper ions with Ti3C2Tx MXene retains the characteristics of copper ions and synergistically enhances antibacterial effects. Our material has good antibacterial effect against non-multidrug resistant Escherichia coli, Staphylococcus aureus, methicillin-resistant Staphylococcus aureus (MRSA) and Gentamicin-resistant Escherichia coli (E. coli GM). Compared with Ti3C2Tx MXene, Cu/MXene produces more than ten times amount of hydrogen peroxide (H2O2), which can cause the enhancement of oxidation pressure on bacterial, and cooperate with the sharp edges from Ti3C2Tx MXene increasing the physical pressure. Meanwhile, Ti3C2Tx MXene has good photothermal conversion efficiency under NIR irradiation. The temperature of Cu/MXene would rise and accelerate the generation of H2O2 in short period, thus further improving the antibacterial effect. In-vitro cytotoxicity and hemolysis results revealed the high biocompatibility of Cu/MXene. An in-vivo MRSA infection wound healing study was conducted in mice (C57BL/6), showing that when Cu/MXene is used as a dressing material, it can effectively remove bacteria on the wound. So far we have developed a new type of nanocomposite antibacterial agent with photothermal properties, and hope to increase the potential of two-dimensional nanomaterials in antibacterial field in the future.

CONTENTS
致謝 I
中文摘要 IV
ABSTRACT V
FIGURE CONTENTS VIII
1. INTRODUCTION 1
1.1 Bacteria resistance 1
1.2 Antibacterial activity of two-dimensional (2D) nanomaterials 2
1.3 Antibacterial activity of MXene 3
1.4 MXene and metal ions 4
1.5 Antibacterial activity of copper ion 5
1.6 Research motives 6
2. EXPERIMENTAL METHODS 7
2.1 Materials 7
2.2 Preparation of delaminated MXene (Ti3C2Tx) nanosheets 7
2.3 Preparation of Cu/MXene 8
2.4 Characterization of MXene and Cu/MXene 8
2.5 Bacterial culture 9
2.6 In-vitro Antibacterial assay 9
2.7 Evalutuion of photothermal performance of Cu25/MXene 10
2.8 SEM and TEM image of bacteria 11
2.9 Hydrogen peroxide produced by Cu/MXene 11
2.10 Reactive Oxygen Species (ROS) assays. 12
2.11 Biocompatibility test 12
2.12 Hemolysis assays 13
2.13 In-vivo wound healing application 14
3. RESULTS AND DISCUSSION 15
3.1 Characterization of the Cu/MXene 15
3.2 Evaluation for antibacterial activity of Cu/MXene 17
3.3 Antibacterial mechanism of Cu/MXene 19
3.4 Biocompatibility of Cu/MXene 22
3.5 Treatment of infected wounds 23
4. CONCLUSIONS 24
REFERENCES 25
FIGURES 33

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