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標題: 1.微粒體甲烷單氧化酵素之結構與功能性之模型三核銅簇化合物之研究(II) 2.探討光合作用之光系統二酵素氧化水分子的反應機制(II)
Structural and Functional Models for the Trinuclear Copper Clusters of the Particulate Methane Monooxygenase (Ii) Exploring the Water-Splitting Catalyzed by Oxygen Evolving Complex in Photosystem II (Ii)
作者: 陳炳宇
關鍵字: 化學類;基礎研究
我的研究計畫將延續我們先前與能源研究相關的議題:能源形態的轉換和綠色能源,一、微粒體甲烷單氧化酵素之結構與功能性之模型三核銅簇化合物之研究。二、探討光合作用之光二酵素氧化水分子的反應機制。在過去的一年中,我們第一個研究主題有很大的進展,我們成功的發展出第一個可以對環己烷分子的C-H 鍵(97 kcal mol-1)進行氧化催化反應,在這個計劃中我們將延續這些重要進展繼續發展與研發新的三核銅簇配位基,並同時進行其基礎研究與工業運用的探索。我們將以設計的一系列的三核銅簇化合物並配合相關光譜、理論計算、電化學等研究以做為設計一高效率催化劑的基礎。並將篩選其中在均相反應中對有機受質具有高活性的三核銅簇化合物,將之嵌入合適之沸石以模擬甲烷單氧化酵素活性中心被包圍在一疏水袋的環境中。此外,三核銅簇化合物也非常適合於燃料電池中的電極設計,我將以簡易修改合成方式,將三核銅簇化合物固定於電極表面,從事相關研究。在第二個主題,我將研究的是光系統二酵素的模型化合物。光系統二酵素經由太陽光的照射激發下進行水分子裂解成氧氣分子與氫質子,並且造成四個電子轉移的催化反應機制。這個催化反應為光系統二酵素中活性中心,一個具有(3+1)模式的四核錳簇化合物所主導進行。在這個子計畫中,根據三核銅簇化合物的研究經驗,我們已合成出一系列三核錳簇模型化合物。這些三核錳簇模型化合物將會先進行一系列的基本研究包含磁性與氧化態之間的變換。之後更進一步接上第四個錳離子用以模擬及瞭解光系統二酵素的催化過程,並將以此為基礎進一步設計能進行水分子裂解成氧氣分子與氫質子的高效率催化劑。

My research effort will extend our two primary projects with regard to energy issues:conversion of energy and green energy. 1. Structural and Functional Models for theTrinuclear Copper Clusters of the particulate Methane Monooxygenase 2. Exploring theWater-Splitting Catalyzed by Oxgen Evolving complex in photosystem II.We have a great harvest in this year. In the first component project, we have successfullydeveloped a trinuclear copper catalyst which is able to facilely and catalytically promoteO-atom transfer into C-H bonds of cyclohexane whose C-H BDE is 97 kcal mol-1. In thisproposal, I will extend these achievements to explore a series of our systematical supportingligands in fundamental studies and industrial applications. It will include basicspectroscopic studies, theoretical calculations and electrochemistry to study the details ofthis system. For those some good candidates for methane catalysis, they will be embeddedinto zeolite with suitable size to fully mimic the hydrophobic pocket of the pMMO. Inaddition, these trinuclear copper complexes will be very favorable on the application of fuelcell. We will simply modify the synthesis of the support ligands to anchor these trinuclearcopper complexes on the surface of electrode to be the cathode of fuel cell.In second proposal, I am going to work on the models of photosystem II enzyme, whichis capable of catalyzing the water molecule to form one dioxygen molecule, 2 protons andtransference of 4 electrons under continueous sun light illumination. The reaction center ofphotosystem II enzyme is a tetranuclear manganese complex with a not symmetrical (3+1)cuboidal comformation. With the experiences of tricopper complex, we have developed aseries of trinuclear manganese complexes in this year. On the basis of these results, we willfirst investigate the intrinsic quality of these trimamganese complexes by means of a seriesof spectroscopic studies, theoretical calculations, and further to attempt to attach anexogenous Mn ion to mimic the PS II enzyme.
其他識別: NSC100-2113-M005-009-MY2
Appears in Collections:化學系所

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