论文总字数：18054字

摘 要

采用水热法并通过控制前驱体溶液的浓度合成了不同形貌的盘状和柱状ZnO晶体，并通过 X射线衍射(XRD)、扫描电镜(SEM)、透射电子显微镜(TEM)、选区电子衍射(SAED)、拉曼光谱(Raman)及氢气程序升温还原(H2-TPR)等表征其形貌结构、生长习性及其与Cu之间的相互作用。发现随着前驱体溶液浓度的减小，ZnO晶体结构逐渐延长，六边形极性面直径减小，形状由盘状向柱状转变。然后分别将这些ZnO晶体作为助剂制备了不同形貌的Cu/ZnO催化剂，并用于醋酸异丙酯(IA)加氢合成乙醇和异丙醇的反应。结果发现：ZnO晶体的形貌结构对IA加氢催化性能有明显的影响，盘状Cu/ZnO催化剂具有最高的IA转化率和产物选择性；对催化活性与ZnO极性面所占比例进行了关联，得到了较好的线性关系，极性面比例越高，IA转化率越高。这归因于极性面比例较高的ZnO与Cu之间的相互作用更强，活性组分铜的分散更均匀、更容易还原，从而使催化加氢活性更高。

关键词：ZnO形貌 极性面 醋酸异丙酯 加氢 乙醇 异丙醇

The synergy of Cu and ZnO with different morphology and influence on hydrogenation of isopropyl acetate to ethanol and isopropanol

Abstract

Plate and rod-like hexagonal ZnO crystals were synthesized via a facile solution by adjusting the precursor concentration. The crystals’ structures, growth habits and the synergy between Cu and ZnO with different morphology were characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectra and H2 temperature-programmed reduction (H2-TPR). It was found that with the decrease of the precursor concentration, the ZnO crystals were elongated along the length axis, and the diameter of the planes were reduced, leading to the shape evolution from hexagonal plate to prismatic rod. The resulted ZnO crystals were used as cocatalyst of copper based catalysts for hydrogenation of isopropyl acetate to ethanol and isopropanol. The morphology of ZnO crystals had a significant impact on the catalytic performance of IA hydrogenation; the Plate-like Cu/ZnO catalyst had the highest conversion of isopropyl acetate and the selectivity of ethanol and isopropanol. A linear relationship between the percentage of the polar planes surface area and the conversion of isopropyl acetate was identified. IA conversion increases with increasing proportion of the polar surface. This was attributed to that the higher polar surface ratio of ZnO led to stronger interaction of ZnO and Cu. And the active component, copper, was better dispersed, thus easier to be reduced, so that the catalytic hydrogenation activity was higher.

Key words: ZnO morphology，polar planes，isopropyl acetate，hydrogenation， ethanol，isopropanol

目 录

摘 要 I

Abstract II

第一章 前言 1

1.1 课题背景 1

1.2 乙醇简介 1

1.3 异丙醇简介 4

1.4 醋酸异丙酯简介 5

1.5酯加氢催化剂研究进展 6

第二章 实验部分 9

2.1试剂及药品 9

2.2催化剂的制备 9

2.2.1不同形貌ZnO晶体的合成 9

2.2.2不同形貌Cu/ZnO催化剂的制备 9

2.3催化剂性能评价 10

2.3.1实验装置 10

2.3.2反应产物的分析方法 11

2.4催化剂的表征 11

第三章 结果与讨论 13

3.1催化剂形貌表征 13

3.1.1 X射线衍射（XRD） 13

3.1.2扫描电镜（SEM） 14

3.1.3透射电镜（TEM） 15

3.1.4拉曼光谱（Raman） 16

3.1.5程序升温还原（H2-TPR） 17

3.2催化剂性能及构效关系 18

第四章 结论及展望 21

参考文献 22

致谢 24

第一章 前言

1.1 课题背景

近年来，越来越多的研究者致力于乙醇的多途径生产研究，由于乙醇作为汽车发动机的可替代燃料比传统的汽油燃料拥有更多的优势^[1-2]，它不仅拥有良好的抗爆震性能^[3-4]，而且还可以减少温室气体的排放，是理想的清洁能源。

当前由于醋酸行业的产能过剩，由醋酸和丙烯直接酯化生成醋酸异丙酯，再由醋酸异丙酯加氢生成乙醇的研究也越来越多^[5-8]。

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