本研究探討以水泥與矽鋁酸粉體和適量錳鹽調製成固化劑均勻塗佈於氧化鋁載體後，以高溫燒結方式來製備成臭氧催化觸媒並應用於水溶液相中降解酚，研究主要探討塗佈劑之組成及燒結條件對於錳金屬型觸媒之表面特性及催化性能影響，並以填充床批式反應器進行觸媒臭氧催化降解含酚溶液。研究中將以比表面積分析儀(BET)分析觸媒之孔隙特性，並探討在不同的矽鋁酸粉體添加下對於孔隙體積之改變，並以高效液相層析儀(HPLC)與總有機碳分析儀(TOC)測定水中酚的轉化率及水中總有機碳的去除率，及使用感應耦合電漿原子發射光譜儀(ICP)分析實驗過程中金屬溶出及失活情形，研究中氫氧自由基之活性將以螢光分析法探討臭氧催化氧化反應器催化過程中催化活性之大小。
本研究發現，以固化劑粉體中矽鋁酸粉體添加量可高達40%仍可維持相當機械強度並具最佳臭氧催化氧化性能，當矽鋁酸粉體添加量達40%時，固化層觸媒比表面積可以達到160 m2/g最大比表面積並維持中孔範圍孔徑。本研究首先探討臭氧催化觸媒氫氧自由基生成機制，研究結果發現臭氧催化觸媒於鹼性環境下有利於氫氧自由基產生，固化繼承分中加入矽鋁酸粉體含量可促進製備觸媒擁有較高的比表面積並維持其孔隙度。探討臭氧催化氧化分解酚反應過程中，結果臭氧催化氧化反應在pH10時具有最佳的氧化效率，且在最高矽鋁酸粉體添加量(40%)時，酚的轉換率可在50分鐘可達到100%轉換率及總有機碳去除率達到50%，此結果與自由基測試結果相符。本研究發現水泥與矽鋁酸粉體和活性金屬(Mn)離子所調製成固化劑以塗佈法於適當載體上可有效展現出觸媒活性，本研究中觸媒於臭氧催化反應中確實增加催化氧化之活性並獲得高效率之氧化效果。 The purpose of this study is to develop a new coating method with cement, aluminosilicate and active manganese ion coating the alumina support. Which was activated by high temperature sintering, it was used to catalytic ozonation to degradation phenol in aqueous solution. It was found that the coating material and preparing condition strongly affected the surface properties and activity of catalytic ozonation performance. A packing bed reactor was used to monitoring the catalytic ozonation performance of catalyst. The pore and surface properties of catalyst was determined by the BET analysis. The relationship pore and surface properties of catalyst between catalytic ozonation performances was investigated by HPLC and TOC analyzer. The metal release and deactivated properties of catalyst were monitoring by the ICP analysis and the free radical of hydro peroxide were measured by the fluorescence meter.
It was found that the aluminosilicate content can be up to 40% in the coating powder and the products catalyst still showed a good mechanical property and catalytic ozonation performance. It was found that the surface area is up to 160 m2/g and showed the pore size in range of medium pore size (2-100 nm). It was found that the basic condition in ozonation benefit to the free radical generation and showed high conversion of pollutant. The surface area of coating layer on the catalyst increased with increasing aluminosilicate content in coating powder and keep the similar pore size on the surface. With the optimum content, almost 100% phenol can be conversed and 50% TOC removal can be achieved in 50 minutes ozonation. It was concluded that coating material with cement and aluminosilicate can be easy prepared on many support material and active metal ion doping in the coating powder effective enhanced the ozonation performance of catalyst.
