研究生: |
王瑞翔 Rui-Xiang Wang |
---|---|
論文名稱: |
鉑催化劑進行甲醇重組反應來製造氫氣 Hydrogen Production by Reforming of Methanol over Pt/Zn Catalysts |
指導教授: |
葉君棣
Chuin-Tih Yeh |
口試委員: | |
學位類別: |
碩士 Master |
系所名稱: |
理學院 - 化學系 Department of Chemistry |
論文出版年: | 2006 |
畢業學年度: | 94 |
語文別: | 中文 |
論文頁數: | 75 |
中文關鍵詞: | 鉑 、製氫 、甲醇重組 |
外文關鍵詞: | hydrogen production, Pt, ZnO, Methanol reforming |
相關次數: | 點閱:2 下載:0 |
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本研究利用沈積沈澱法(deposition precipitation method)製備以氧化鋅為支撐物的鉑催化劑,並使用TPR、XRD、TEM、ICP等方法來鑑定催化劑的物理與化學特性,也以不同的甲醇重組反應,包括部份氧化反應(POM)、蒸氣重組反應(SRM)、氧化性蒸氣重組反應(OSRM)觀察製備鉑催化劑的催化活性。希望催化劑能具備高的甲醇轉化率(CMeOH)、氫氣選擇性(SH2)與二氧化碳選擇性(SCO2)。
研究中發現製備出來的Pt2/Zn催化劑經過Tp = 400 ℃的氫氣還原處理後,甲醇重組催化具有最好的活性。TPR鑑定結果指出,還原處理的溫度太低時(Tp = 200 ℃、300 ℃)無法有效去除催化劑上的氯離子;過高的還原溫度 (Tp = 500 ℃)則會促使金屬顆粒燒結分散度下降,因此都會使得反應活性下降。
Pt2/Zn催化劑不適合用於催化SRM與OSRM反應,但此催化劑有很好的POM反應活性,以高面積氧化鋅當支撐物製備出的鉑催化劑(Pt2/Zn-70)可於室溫之下起燃,並擁有良好的活性[在反應溫度為TR = 120 ℃時CMeOH = 78 %、SH2 = 77 %、SCO2 = 95 %]。在低溫(TR < 250 ℃)下鉑催化劑的SRM與OSRM反應的表現並不理想,顯示鉑催化劑傾向POM反應不利於SRM的進行。
為了改善鉑催化劑氫氣選擇性不佳的問題,實驗中使用混合催化劑(鉑催化劑與銀催化劑)進行POM反應,反應結果證實此方式可有效地提昇氫氣選擇性(SH2 = 86%),並且保有原本鉑催化劑室溫下起燃的特性。
In this study, supported of Pt/Zn samples were prepared by the method of deposition precipitation. All the catalysts were characterized by TPR, XRD, TEM, ICP experiments. The activities were measured for reforming of methanol reactions, including partial oxidation of methanol (POM), steam reforming of methanol (SRM) and oxidative steam reforming of methanol (OSRM). We purpose to prepare catalysts with high MeOH conversion (CMeOH), H2 selectivity (SH2), and CO2 selectivity (SCO2).
Pt2/Zn catalyst shows best activities after reduced by hydrogen at Tp = 400 ℃. TPR examinations indicated Cl ions can not be substantially removed by reduction at low temperatures (Tp = 200, 300 ℃). However, a H2 reduction at Tp = 500 ℃ deceases the activity of Pt2/Zn catalyst due to sintering of Pt particles at this high temperature.
Pt/Zn catalysts were not active for SRM and OSRM reaction but showed good performance (CMeOH = 78 %, SH2 = 77 %, SCO2 = 95 %) at a low reaction temperature of TR = 120 ℃ and the catalysts can ignite at room temperature. To improve the SH2 of Pt/Zn catalyst, we mixed Pt/Zn and Ag/CeZn catalysts for POM reaction. The Pt/Zn-Ag/CeZn catalyst retains the advantage of igniting at room temperature and shows a high SH2 (86 %).
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