Cu/TiO_2和Cu/ZrO_2催化甲醇脱氢反应的对比研究(英文)

考察了ＴｉＯ_２和ＺｒＯ_２担载的铜基催化剂的结构及其催化甲醇脱氢的反应性能。氮吸附和ＥＸＡＦＳ结果显示，两个催化剂的结构性质以及铜所处的配位环境比较接近。但Ｘ-射线光电子能谱测试结果显示，催化剂Ｃｕ／ＴｉＯ_２中铜周围的电子密度较催化剂Ｃｕ／ＺｉＯ_２中的高。ＴｉＯ_２结果表明，ＴｉＯ_２能够降低与之接触的较大ＣｕＯ的还原温度。催化剂电子结构的不同导致反应性能的差异，在Ｃｕ／ＴｉＯ_２催化剂上甲酸甲酯是主要产物，而Ｃｕ／ＺｒＯ_２催化剂则催化甲醇深度脱氢生成ＣＯ。此外，Ｃｕ／ＺｒＯ_２催化剂失活较Ｃｕ／ＴｉＯ_２催化剂慢得多。

COMPARATIVE STUDY OF Cu/TiO2 AND Cu/ZrO2 FOR METHANOL DEHYDROGENATION

The structure and performance of TiO_2 and ZrO_2 supported copper catalysts for methanol dehydrogenation were investigated. The nitrogen physisorption experiment and EXAFS measurement indicated that the textural properties and coordination environment of the two catalysts were similar. While, X-ray photoelectron spectrascopy indicated that the charge density of copper in Cu/TiO_2 was higher than that in Cu/ZrO_2, and TPR results suggested that titania significantly enhanced the reducibility of the large CuO.particles. Therefore, the two catalysts showed different catalytic properties. Methyl formate was the main product over Cu/TiO_2, While the reaction over Cu/ZrO_2 produced CO predominantly. Furthermore, the Cu/ZrO_2 catalyst deactivated more slowly than the Cu/TiO_2 catalyst.