利用Cu/ZnO/Al2O3觸媒進行低溫甲醇產氫自熱反應之研究

Characteristics of Autothermal Reforming of Methanol on Hydrogen Production using Cu/ZnO/Al2O3 derivative at Low Temperature

連多尼(Donny Lesmana)

指導教授 ： 吳和生

元智大學/工程學院/化學工程與材料科學學系/碩士(2013年)

https://doi.org/10.6838/YZU.2013.00068

摘要

摘要

使用Cu/ZnO/Al2O3衍生物，進行自熱重整甲醇反應草酸共沉澱法，固定床反應器，微通道反應器運行的實驗方法和洗塗沉澱。所有的操作條件下，在較低的反應溫度下獲得優化的活性催化劑。
本實驗條件下，用蒸汽對甲醇的摩爾比，氧對甲醇的摩爾比，重時空速，草酸共沉澱，pH值對草酸共沉澱析出溫度，草酸乾燥的共沉澱的時間，不同的溫度下在初始狀態下，不同溫度下加熱催化劑和催化劑，未升溫加熱催化劑加熱催化劑和加熱反應，自熱重整甲醇的各種氧氣濃度。
實驗結果表明，當使用Cu/ZnO/Al2O3/Cr2O3/CeO2（15/15/2.5/1.25/1.25摩爾％）催化劑在反應溫度下為低（200℃），甲醇轉化率等於80％，一氧化碳濃度等於900 ppm的壽命100小時。固定床催化劑的溫度是一個函數的x/ L（長度固定床催化劑）。增長的氧氣濃度，催化劑床層溫度增加有關聯。催化劑床層溫度增加有顯著的效果，增加甲醇轉換。微通道反應器上運行時的實驗結果優於固定床反應器。

關鍵字

自熱重整反應 ； Cu/ZnO/Al2O3/Cr2O3/CeO2 ； 氫 ； 甲醇 ； 草酸共沉澱法 ； 大衣

並列摘要

Abstract

The autothermal reforming methanol reaction was carried out using Cu/ZnO/Al2O3 derivative, with oxalic co-precipitation method and wash coat precipitation method for running experiment on fixed bed reactor and microchannel reactor, respectively. All the operation condition that obtained optimized active catalysts at low reaction temperatures.
The experimental conditions were used steam to methanol mol ratio, the mol ratio of oxygen to methanol, weight hourly space velocity, precipitation temperature on oxalic co-precipitation, pH on oxalic co-precipitation, time of drying on oxalic co-precipitation, various temperatures for heating up catalyst at initial condition, various temperatures on heating up catalyst and un-heating up catalyst, un-heating up catalyst and un-heating up reactant, various oxygen concentration on autothermal reforming methanol.
The experiment result shows when use Cu/ZnO/Al2O3/Cr2O3/CeO2 (15/15/2.5/1.25/1.25 mol%) catalyst at the reaction temperature was lower (200 oC), methanol conversion equaled to 80% and carbon monoxide concentration equal to 900 ppm for lifetimes 100 h. Temperature of fixed bed catalyst is a function of x/L (length of fixed bed catalyst). An increased oxygen concentration has a correlation to increased temperature on catalyst bed. Increased temperature on catalyst bed has the significant effect for increased of methanol conversion. The experiment result when running on microchannel reactor was better than fixed bed reactor.

並列關鍵字

Autothermal reforming reaction ； Cu/ZnO/Al2O3/Cr2O3/CeO2 ； hydrogen ； methanol ； oxalic co-precipitation method ； enriched oxygen

參考文獻

Abanades, S., P. Charvin, G. Flamant, P. Neveu, Screening of water-splitting thermochemical cycles potentially attractive for hydrogen production by concentrated solar energy. Energy, 31 : 2805–2822. (2006)

Abanades, S., P. Charvin, F. Lemont, G. Flamant, Novel two-step SnO2/SnO water-splitting cycle for solar thermochemical production of hydrogen. International Journal of Hydrogen Energy, 33 : 6021–6030. (2008)

Agrell, J., H. Birgersson, M. Boutonnet, I.M. Cabrera, R.M. Navaro, J.L.G. Fierro, Production of hydrogen from methanol over Cu/ZnO catalyst promoted by ZrO2 and Al2O3. Journal of Catalysis, 219 : 389-403. (2003)

Agarwal, V., S. Patel, K.K. Pant, H2 Production by steam reforming of methanol over Cu/ZnO/Al2O3 catalyst: transient deactivation kinetics modeling. Applied Catalysis A: General, 279 : 155-164. (2005)

Alla, M.H.A., F.M. Morsy, A.W.E.E. Enany, Hydrogen production from rotten dates by sequential three stages fermentation. International Journal of Hydrogen Energy, 36 : 3518-3527. (2011)