臺灣博碩士論文加值系統

摘要
在生物無機化學的研究發展中，多核銅金屬蛋白質系列一向被廣為討論，因其結構的複雜及多樣性，深受許多無機化學家注意，模型的研究有助於我們對於這些酵素及金屬蛋白質有更進一步的瞭解，使我們能夠控制某一些變因，並且評估模型的改變及其對生物體的功能的影響。許許多多的模擬銅蛋白結構的研究中，又以三核銅金屬蛋白結構在文獻中少有發表，使得我們對於合成出具有模擬此類型金屬蛋白之結構，並探討其光譜性質將其結構上之特殊性更進一步應用於材料、有機合成、醫藥、環境、化工等方面的研究。本篇論文中所介紹的Cu3I3分子，具有上述的重要特殊性質，並且也利用其結構上的特殊性，應用於一些簡單的反應中。
在我們的實驗中，利用水熱合成法，成功的合成出具有模擬銅金屬蛋白質結構的分子，我們簡稱為Cu3I3。Cu3I3分子其中心金屬所組成的三核銅金屬簇，為一個金字塔形狀，在結構上具有一個C3V的點群，以頂端的Cu原子為正二價，以其為軸心旋轉，有一個C2軸使得底部的兩個Cu原子為等價非整數（+0.5價）的價數分布，整個分子具有混價（Mixed-Valence）的特性，可以進行氧化還原反應及電子傳遞的功能，這在生物學上具有重要的意義。此外，經由光譜的鑑定我們發現許多特異性及熱穩定性，可以提供我們做更進一步的探討及應用。
由於Cu3I3分子具有上述之特性，利用其電子傳遞特性應用於高分子自由基聚合反應上，Cu3I3分子當作反應的催化劑，合成出具有高分子量的聚苯乙烯聚合物，並且分子量分布度控制於1.2以下。這透露了一個訊息，Cu3I3分子傳遞電子的特性，不僅可以應用於高分子的催化方面，提供一個良好的聚合方式，未來將應用其傳遞電子及混價特性，嘗試應用於烷類氧化及DNA切割試劑等方面。
而在NO氣體吸附實驗中，我們得到的結果雖非預期所要吸附的NO氣體，但是所吸附到的NO2氣體亦為空氣污染的來源之一，Cu3I3分子上的二價銅所具有的活性，證明了可以與某些氣體分子作用，未來只要在修正整個反應的環境，在環境化學上，將可作為氮氧化物的氣體感測器。

目錄
中文摘要…………………………………………………………….Ⅰ
圖目錄……………………………………………………………….Ⅴ
表目錄……………………………………………………………….Ⅶ
第一章 序論
第一節 前言………………………………………………….1
第二節 金屬離子在金屬酵素中所扮演的角色…………….2
第三節 銅金屬蛋白質的介紹……………………………….6
第四節 現今對於銅金屬蛋白質結構的模型研究回顧…….12
第二章 實驗部分
第一節 儀器與藥品………………………………………….32
第二節 水熱合成法簡介…………………………………….36
第三節 Cu3I3分子的合成與鑑定……………………………38
第四節 苯乙烯之聚合反應
第五節 NO氣體吸附實驗…………………………………44
第三章 結果與討論
第一節 Cu3I3分子
3-1.1 實驗目…………………………………………….45
3-1.2 實驗結果…………………………………………45
3.1-3 C24H16Cu3I3N4晶體結構探討……………………46
3.1-3-1 光譜探討………………………………………...48
3.1-4 苯乙烯聚合反應…………………………………59
3.1-5 NO氣體吸附實驗……………………………….63
第二節 C24H16Cu4I5N4晶體結構探討………………………71
第四章 結論………………………………………………………72
參考文獻……………………………………………………………74
附錄………………………………………………………

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