羰基合成碳酸二甲酯pdnay催化剂的表面酸性和作用机制研究-surface acidity and mechanism of pd nay catalyst for carbonyl synthesis of dimethyl carbonate.docx

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2018-08-07 发布于上海
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羰基合成碳酸二甲酯pdnay催化剂的表面酸性和作用机制研究-surface acidity and mechanism of pd nay catalyst for carbonyl synthesis of dimethyl carbonate.docx

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羰基合成碳酸二甲酯pdnay催化剂的表面酸性和作用机制研究-surface acidity and mechanism of pd nay catalyst for carbonyl synthesis of dimethyl carbonate

In order to further increase the amount of Lewis acid sites and consequently im- prove catalytic activity, alkali metal additives (Li, K, Rb and Cs) were selected to decorate Pd/NaY catalyst. MN carbonylation activity test showed that the potassi- um-doped catalyst performed best. The influences of potassium precursor, doping se- quence and method on the carbonylation performances of MN were investigated. The results indicated that the improvement in activity was closely related to the precursor and doping method of potassium, but was independent on the doping sequence. The observations of experimental characterization and density functional theory (DFT) proved that the potassium enhanced the electron density of Pd species resulting in a stronger interaction between Pd species and CO molecule, meanwhile the potassium ions as Lewis acid sites interacted with O atom of CO. The synergy between Pd active species and Lewis acid sites (Pd-CO···Lewis acid) make CO molecule a more active participant role in carbonylation reaction, further facilitating the synthesis of DMC. KEY WORDS： Carbonylation of methyl nitrite, Dimethyl carbonate, Pd clusters, Lewis acids, Alkaline metal 目录 HYPERLINK \l _bookmark0 第一章文献综述1 HYPERLINK \l _bookmark1 1.1 引言 1 HYPERLINK \l _bookmark2 1.2 碳酸二甲酯 2 HYPERLINK \l _bookmark3 1.2.1 碳酸二甲酯的理化性质2 HYPERLINK \l _bookmark4 1.2.2 碳酸二甲酯的用途2 HYPERLINK \l _bookmark5 1.2.3 碳酸二甲酯的生产工艺3 HYPERLINK \l _bookmark6 1.3 亚硝酸烷基酯羰基化法合成烷基碳酸酯 8 HYPERLINK \l _bookmark7 1.3.1 工艺概述9 HYPERLINK \l _bookmark8 1.3.2 催化剂活性物种的研究12 HYPERLINK \l _bookmark9 1.3.3 含氯体系14 HYPERLINK \l _bookmark10 1.3.4 无氯分子筛体系18 HYPERLINK \l _bookmark11 1.3.5 反应机理研究21 HYPERLINK \l _bookmark12 1.4 论文工作的提出 23 HYPERLINK \l _bookmark13 1.4.1 论文工作的背景23 HYPERLINK \l _bookmark14 1.4.2 研究内容25 HYPERLINK \l _bookmark15 第二章实验部分26 HYPERLINK \l _bookmark16 2.1 化学试剂 26 HYPERLINK \l _bookmark17 2.2 实验装置及工艺流程 27 HYPERLINK \