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使用Cu/ZnO/Al₂O₃催化剂的甲醇重整制氢动力学

Kinetics of hydrogen production of methanol reformation using Cu/ZnO/Al2O3 catalyst.

作者信息

Wu Ho-Shing, Chung Shun-Chang

机构信息

Department of Chemical Engineering and Materials Science, Yuan-Ze University, 135 Yuan Tung Road, ChungLi, Taoyuan, 32003, Taiwan.

出版信息

J Comb Chem. 2007 Nov-Dec;9(6):990-7. doi: 10.1021/cc070066r. Epub 2007 Sep 28.

Abstract

The catalytic performance of methanol reformation using Cu/ZnO/Al2O3 was investigated at low temperature. The operation conditions, such as composition of Cu, Zn, and Al, temperature, molar ratio of H2O/CH3OH, weight hourly space velocity, catalyst weight, and kind and flow rate of carrier gas (helium and air), were evaluated to obtain the optimum reaction condition. The catalysts were prepared by oxalic coprecipitation, coprecipitation, and polyol method. The weight composition of Cu, Zn, and Al prepared by oxalic coprecipitation was 15:15:5 by high-throughput screening of combinatorial chemistry method, which was the best Cu/ZnO/Al2O3 catalyst. The prepared catalysts showed high activity and selectivity towards hydrogen formation. The methanol conversion, production rate, and volumetric percentage of hydrogen using this best catalyst were larger than 95%, 0.65 mol/h x g and 59%, respectively, and the CO volumetric percentage was smaller than 0.22% when the reaction temperature was 240 degrees C. The size and dispersity of copper, and the activity and turnover frequency of the catalyst were calculated as well.

摘要

研究了Cu/ZnO/Al₂O₃用于甲醇低温重整的催化性能。对操作条件进行了评估,如Cu、Zn和Al的组成、温度、H₂O/CH₃OH摩尔比、重量时空速、催化剂重量以及载气(氦气和空气)的种类和流速,以获得最佳反应条件。通过草酸共沉淀法、共沉淀法和多元醇法制备了催化剂。通过组合化学方法的高通量筛选,草酸共沉淀法制备的Cu、Zn和Al的重量组成为15:15:5,这是最佳的Cu/ZnO/Al₂O₃催化剂。制备的催化剂对氢气生成表现出高活性和选择性。当反应温度为240℃时,使用这种最佳催化剂的甲醇转化率、产率和氢气的体积百分比分别大于95%、0.65 mol/h·g和59%,CO的体积百分比小于0.22%。还计算了铜的尺寸和分散度以及催化剂的活性和周转频率。

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