摘要:由于二氧化锆是唯一同时拥有酸性和碱性及氧化性和还原性的金属氧化物,而且还是P一型半导体,易于产生氧空穴,作为催化剂栽体,可和活性组分产生相互作用,因此由它负载的催化剂与其他物质负载的催化剂相比较,具有更多的优良性能。本论文系统研究了Cu/ZrO2催化剂中组份间相互作用对甲醇水蒸气重整反应性能的影响。通过选择不同的成分比例和不同制备方法制备了Cu/ZrO2催化剂。并通过N2吸附、N2O吸附、TEM、TPD和拉曼光谱表征催化剂的物理和化学性质。结果表明,制备方法显著影响活性成分分散,微观结构和吸附性能。在铜/氧化锆催化剂的制备中,27.3%氧化锆负载分级沉淀法在铜和氧化锆之间显示出较高的比表面和界面。这不仅加快甲醇的吸附和水的分解,而且还促进形成Cu+和表面氧物种,从而提高催化活性和稳定性。42876
毕业论文关键词:Cu/ZrO2;甲醇水蒸汽;分步沉淀法
Influence of the component interaction over Cu/ZrO2 catalysts induced with fractionated precipitation method on the catalytic performance for methanol steam reforming
Abstract: Zirconia, as the unique metal oxide with both properties of acidic and alkaline, both properties of oxidizability and reducibility, as well as the property of a p-semiconductor, is a superior catalytic supporter to other materials. In the present work, nanostructure Cu/ZrO2 catalysts for the steam reforming of methanol(MSR) were investigated. A series of binary Cu/ZrO2 catalysts by choosing different composition ratios and different precipitation sequences have been prepared for the production of hydrogen by steam reforming of methanol (SRM). A variety of characterization techniques including N2 adsorption, N2O chemisorption, TEM, TPD and Raman are employed to characterize the physical and chemical properties of the catalysts. The results show that the preparation methods significantly affect the component dispersion, microstructure and adsorption properties. The Cu/ZrO2 catalyst with 27.3% ZrO2 loading prepared by fractionated precipitation method displays higher specific surface and interface between copper and zirconia, which not only accelerates decomposition of adsorbed methanol and water, but also promotes formation of Cu+ and surface oxygen species, accordingly enhancing the catalytic activity and stability.
Keyword:Cu/ZrO2; steam reforming of methanol; fractionated precipitation method
目录
1.1一氧化碳低温氧化催化体系的研究进展 1
1.2一氧化碳的来源以及危害 3
1.3甲醇水蒸气重整制氢催化剂 4
1.3.1铜系催化剂的开发研究现状 4
1.3.2铜系催化剂的活性组分 5
1.4甲醇水蒸气重整制氢反应机理 5
1.5 Cu/ZrO2催化剂体系研究进展 6
1.5.1共沉淀法 6
1.5.2浸渍法 7
1.5.3沉淀沉积法 7
1.5.4溶胶/凝胶法 7
1.5.5微乳液法 7
1.6Cu基复合氧化物催化剂...8
2实验部分 …9
2.1催化剂的制备 9
2.1.1氧化铜催化剂的制备 9
2.1.2ZrO2载体的制备 9
2.1.3Cu/ZrO2催化剂的制备 9