2011-01-012024-05-18https://scholars.lib.ntu.edu.tw/handle/123456789/711463摘要：光觸媒是異相觸媒重要的研究領域之一，有可能可以克服在選擇性氧化反應時，常見產物低選擇率的問題，例如烯類的環氧化。進行選擇性光催化氧化反應時，不僅須要特別的光觸媒，而且須要知曉反應物種結構之間的關係，因此必須從根本了解光催化的機理。但目前光催化的反應基本步驟及反應時的光觸媒狀態尚未被研究清楚，主要原因是這項研究須要結合有互補性專長的團隊才能達成。本計畫將由具有光觸媒研究經驗的台灣大學化工系觸媒實驗室，和具有光譜分析專長的西班牙高等科學委員會所屬觸媒與石油化學研究所，共同進行合作以達成以下目標。 本計畫將設計一個光譜式的光反應器，用原位(in situ)方式探測光催化反應，以揭發光觸媒反應機理，光譜分析包括使用近紅外光(NIR)-拉曼(Raman)光譜。截至目前為止，很少有用此原位方法探測光催化反應的報導，尤其是使用紅外光譜，原因是在光觸媒表面，水的強吸附覆蓋了大部分紅外光譜的信號。而在光照催化反應時，拉曼光譜則受限於原本就有瑩光(fluorescence)的強烈干擾。本計畫提出使用近紅外光雷射的拉曼光譜分析，可以有效避開瑩光的強烈干擾，同時拉曼光譜原本就沒有(或很弱)水的信號，將可順利以原位方式探測光催化反應。為了證實這個方法，初步將用TiO2/SiO2 和V5+/SiO2光觸媒，進行丙烯的光催化環氧化為測試反應。 <br> Abstract: Photocatalytic reactions are an important field in heterogeneous catalysis, which may overcome significant selectivity limitations in selective oxidation reactions, such as olefin epoxidation. Selective photocatalytic oxidations not only needs a unique photocatalysts, but we must also determine structural performance relationships. There is a need to fundamentally understand photocatalysis because the reaction mechanism of photocatalysis and the actual state of the catalyst during reaction remain unclear. This requires a combined effort of complementary talents to foster fundamental understanding. Thus, the expertise on photocatalysis by National Taiwan University (NTU) group and the expertise in spectroscopy during reaction on oxides by Instituto de Catalisis y Petroleoquimica (ICP) group will combine to tackle this objective. The goal of the proposal is to design a spectroscopic reaction cell to investigate and reveal the mechanism of photocatalysis by means of in situ spectroscopy methods, included NIR-Raman. Very few in situ studies have successfully been done so far during photocatalytic reaction; typically by IR, where water absorption of IR signal is significant. Raman studies have been hampered by inherent fluorescence generated. The implementation of NIR-lasers for Raman spectroscopy overcomes fluorescence limitations and has no water interference. As a proof of concept, the reaction of epoxidation of propylene will be investigated on silica-supported photocatalysts, such as TiO2/SiO2 and V5+/SiO2.光催化原位光譜分析近紅外線-拉曼光譜環氧化PhotocatalysisIn-situ spectroscopyNIR-Ramanepoxidation