Hydrogen production by partial oxidation of methanol over Au/CuO/ZnO catalysts

Hydrogen production by partial oxidation of methanol over Au/CuO/ZnO catalysts
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DOI:
10.1016/j.molcata.2007.07.002
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发表时间:
2007-10
影响因子:
--
通讯作者:
Hsien-Chang Yang;F. Chang;L. S. Roselin
Hsien-Chang Yang;F. Chang;L. S. Roselin
中科院分区:
化学2区
文献类型:
--
作者:
Hsien-Chang Yang;F. Chang;L. S. Roselin

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研究了甲醇(POM)部分氧化(CH_3OH +0.5O_2 → 2 H_2 + CO_2)制氢在Au/CuO/ZnO(Au 3 wt.%,Cu 37wt.%和Zn 60重量%)催化剂,通过共沉淀法制备。比较了Au/CuO/ZnO催化剂和CuO/ZnO(Cu 40 wt.%)催化剂的活性和Zn 60重量%)催化剂的采用XRD、TEM和TPR等手段对催化剂进行了表征。与CuO/ZnO催化剂相比,Au/CuO/ZnO催化剂具有更高的活性,并且在更少量的CO下表现出更高的氢选择性。TPR分析证明,Au/CuO/ZnO催化剂活性的增强是由于Au和CuO物种之间的强相互作用。焙烧温度对Au/CuO/ZnO催化剂活性的影响取决于载体的晶相和催化剂上Au和CuO的粒径。最佳煅烧温度为573 K。在不同温度下的催化性能表明,在448 K时反应开始,O2被完全消耗。在523 K时,甲醇转化率为100%,氢选择性高达97.7%。在整个研究的温度范围内,形成非常少量的不希望的副产物CO。
Hydrogen production by partial oxidation of methanol (POM) (CH3OH+0.5O2→2H2+CO2) was examined over Au/CuO/ZnO (Au 3wt.%, Cu 37wt.% and Zn 60wt.%) catalysts, prepared by the co-precipitation method. The activity of Au/CuO/ZnO catalysts has been compared with that of CuO/ZnO (Cu 40wt.% and Zn 60wt.%) catalysts. The catalysts were characterized by XRD, TEM and TPR analyses. The Au/CuO/ZnO catalysts are more active and exhibit higher hydrogen selectively with smaller amount of CO compared to the CuO/ZnO catalysts. The enhanced activity of Au/CuO/ZnO catalyst is due to the strong interaction between Au and CuO species as evidenced by TPR analysis. The influence of calcination temperature on the catalytic activity of Au/CuO/ZnO catalyst depends on crystalline phases of support and particle size of Au and CuO present on the catalysts. The optimum calcination temperature is 573K. The catalytic performance at various reaction temperatures shows that at 448K the reaction sets on with O2completely consumed. A high hydrogen selectivity of 97.7% is attained at 523K with 100% methanol conversion. The undesired by-product, CO is formed in very small amount throughout the temperature range studied.