| 研究生: |
黃湘琳 Huang, Hsiang-Lin |
|---|---|
| 論文名稱: |
合成金銅修飾的鐵鉑奈米立方體作為癌症化學動力治療 Synthesis of FePt@Au/Cu0 Nanocubes for Chemodynamic Therapy as Cancer Treatment |
| 指導教授: |
葉晨聖
Yeh, Chen-Sheng |
| 學位類別: |
碩士 Master |
| 系所名稱: |
理學院 - 化學系 Department of Chemistry |
| 論文出版年: | 2024 |
| 畢業學年度: | 112 |
| 語文別: | 中文 |
| 論文頁數: | 122 |
| 中文關鍵詞: | 零價銅 、化學動力治療 、晶格應變 、單原子催化劑 、生物可降解性 |
| 外文關鍵詞: | Zero-valent Copper, Chemodynamic therapy, Lattice strain, Single-atom catalysts, Biodegradable material |
| 相關次數: | 點閱:59 下載:0 |
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隨著癌症罹患人數不斷增加,癌症治療一直是熱門的研究領域。化學動力治療是一應用於癌症治療的方法,透過產生對腫瘤細胞有毒性的活性氧物質以治療癌症,然而化學動力治療仍面臨內源性雙氧水不足的問題,無法提供充足的雙氧水以進行芬頓反應。因此,本研究設計了具有晶格應變 (Lattice strain) 與單原子催化 (Single-atom catalyst) 的FePt@Au/Cu,透過晶格應變與單原子催化促進FePt@Au/Cu產生過氧化氫,以增強化學動力治療效果。
首先合成出FePt@Cu為零價銅,透過加凡尼取代反應合成出FePt@Au/Cu,並於其表面修飾硬脂酸合成出FePt@Au/Cu@SA,以避免材料提早與氧氣反應;透過包吞作用進入目標細胞後,硬脂酸可與細胞膜融合釋放出FePt@Au/Cu,降解釋放銅離子與電子 (Cu → Cu+ + e- → Cu2+ + e-),氧氣接受電子還原成過氧化氫 (O2 + 2H+ + 2e- → H2O2),過氧化氫再與銅離子透過類芬頓反應 (Fenton-like reaction) 產生羥基自由基 (Cu+ + H2O2 → Cu2+ + •OH + -OH)。而FePt@Au/Cu之晶格應變、比表面積以及單原子催化,皆進行相關實驗予以佐證上述因素促進了FePt@Au/Cu能產生更多過氧化氫,提升化學動力治療的效果。實驗結果證實,FePt@Au/Cu生成•OH的反應效率最好。DFT計算結果表明,在FePt@Au/Cu上O2兩次被氫化 (O2(a) → OOH, OOH(a) → H2O2) 的活化能 (0.73 eV, 0.65 eV) 均比 Cu (1.02 eV, 0.91 eV)、FePt@Cu (0.97 eV, 0.97 eV) 低,因此FePt@Au/Cu相較於Cu、FePt@Cu具有更快的H2O2生成速率,使FePt@Au/Cu具有更好的化學動力學治療療效。此外,FePt@Au/Cu@SA具有生物可降解特性,可透過尿液代謝方式排出於體外,避免材料累積於生物體內。
Chemodynamic therapy (CDT) is a method used for cancer treatment but limited by insufficient endogenous hydrogen peroxide. Hence, we provide a degradable gold-copper-modified iron-platinum nanocubes (FePt@Au/Cu) with lattice strain and single-atom catalyst, which had excellent cascade oxidase-like and Fenton-like catalytic reactivity. With stearic acid (SA) modification, FePt@Au/Cu@SA can enter cancer cell through endocytosis, SA could fuse with the cell membrane to release FePt@Au/Cu, when FePt@Au/Cu decomposed, it could release Cu+ and e-, reduced O2 to form H2O2, then generated •OH by Fenton-like reaction. FePt@Au/Cu had better catalytic reactivity than Cu or FePt@Cu. Besides, FePt@Au/Cu was a biodegradable material, could be excreted from the body through urine metabolism to avoid accumulation of materials.
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