請用此 Handle URI 來引用此文件: http://hdl.handle.net/11455/5103
標題: 微波多元醇法製備負載型銅觸媒應用於潔淨發電技術之研究
Studies on the preparation of supported copper catalysts through microwave polyol process for clean power-generation technology
作者: 莊桂鶴
Chuang, Kui-Hao
關鍵字: catalyst
microwave heated polyol process
clean power-generation technology
出版社: 環境工程學系所
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摘要: 觸媒具有降低反應活化能之優點,可於較低溫度環境下將污染物去除,而觸媒之催化活性受分散性與顆粒大小影響,因此本研究期望發展一簡單快速的觸媒製備方法,應用於淨化火力發電廠或焚化廠反應氣體及水氣轉換或重組碳氫化合物產生之合成氣之一氧化碳 (carbon monoxide, CO) 及氮氧化物 (Nitrogen oxides, NOX),發展潔淨發電技術。 本研究以微波多元醇法製備負載型銅觸媒,探討製備操作參數及擔體種類對觸媒形貌及催化活性之影響,亦與含浸法及多元醇法製備之觸媒比較催化活性,並輔以比表面積分析 (BET)、晶相分析 (XRD)、表面型態觀察 (FESEM)、元素成分分析 (EDS)、感應耦合電漿質譜分析 (ICPMS) 特性分析。 在微波多元醇法製備程序中,微波功率700瓦,微波加熱時間60秒,因為加熱時間短,不需另外添加保護劑即可獲得針狀且分散佳之銅顆粒,而使此觸媒具有高催化反應活性。而 pH 值為2及12之銅顆粒均勻分散於活性碳擔體上,反應溫度175 °C 即可達到極佳之催化活性。擔體選用上,活性碳擔體適用於火力發電廠及焚化廠使用過程中之 NO 還原(< 250 °C)及 CO 氧化反應;氧化鈰擔體可用於火力發電廠及焚化廠使用過程中之 NO 還原 (< 225 °C) 及燃料電池系統中富氫環境氧化 CO 反應;鈰鋯複合氧化物,隨鈰添加比例增加熱穩定性,適用於火力發電廠及焚化廠使用過程中之 NO 還原反應 (> 250 °C)。 不同方法製備之觸媒,其反應活性依序為:微波多元醇法觸媒>多元醇法觸媒>含浸法觸媒。微波多元醇法製備之負載型銅觸媒可有效控制活性相大小及形狀,並提升活性相之高分散性。微波多元醇法簡單快速製備負載型銅觸媒並應用於淨化潔淨發電技術之氣狀污染物。
Air pollutions can be removal by the catalysts at lower reaction temperature with lower activation energy. The catalytic activity is strongly depended on the dispersion and morphology (size and shape) of metal particles. The purpose of this study was to develop a simple and rapid method for preparation of supported copper catalysts. The catalyst preparation may be applied for removal of CO and NOx in the flue gas or syngas from power plants, incinerators, and reforming of hydrocarbons for development of clean power-generation technology. This research was mainly focused on the preparation of supported copper catalysts through microwave polyol process. The effects of operation parameter and support type on morphology and performance of catalysts. In addition, the effects of various preparation methods for supported copper catalysts, namely, impregnation, polyol process, and microwave heated polyol process, on the activity of catalytic were compared. Characterization of catalyst was analyzed by using the techniques of Brunauer-Emmett-Teller (BET) surface area, X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), and inductively coupled plasma mass spectroscopy (ICP-MS). The results revealed that the nanoscaled copper particles were well dispersed, and the catalyst had high catalytic activity even without the addition of PVP was unnecessary in the extremely short preparation time of microwave heated polyol process. Experimental results indicated that a microwave power of 700W and a heated time of 60 s were highly effective, and that copper particles dispersed well on the support, even in the absence of the protecting agent poly-vinyl pyrrolidone (PVP). Supported copper catalyst prepared by microwave-assisted polyol process at the pH value of about 2 and 12 exhibits that copper particles dispersed well on the support. The supported copper catalyst shows excellent catalytic performance at 175 °C. Among different supports, activated carbon (AC)-supported catalysts showed the good removal efficiency of NO (< 250 °C) and CO in the flue gases of power plants and incinerators. For application of CeO2 support, CeO2-supported catalysts were successful used for NO removal in power plants and incinerator (< 225 °C) or selective oxidation of CO in excess hydrogen, separately. The thermal stability of CexZr1-XO2 increased with ratio of Zr/Ce. CexZr1-XO2-supported catalysts were suitable for NO removal in power plants and incinerator at high temperature (> 250 °C). Among the preparation methods, the optimum preparation methods was in the order of microwave heated polyol process > polyol process > impregation method. The particle size, shape, and dispersion of supported copper catalysts were effective controlled by microwave heated polyol process. The microwave polyol process could quickly and easily synthesize the nano-metallic catalysts which could effectively remove the air pollutants for clean power-generation technology.
URI: http://hdl.handle.net/11455/5103
其他識別: U0005-3005201113013200
文章連結: http://www.airitilibrary.com/Publication/alDetailedMesh1?DocID=U0005-3005201113013200


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