| 负载CuCl_2催化剂上甲醇气相氧化羰化制碳酸二甲酯的研究 |
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| 引用本文： | 曹为,祝明霞,袁友珠. 负载CuCl_2催化剂上甲醇气相氧化羰化制碳酸二甲酯的研究[J]. 厦门大学学报(自然科学版), 2004, 0(3) |
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| 作者姓名： | 曹为 祝明霞 袁友珠 |
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| 作者单位： | 固体表面物理化学国家重点实验室厦门大学化学化工学院，固体表面物理化学国家重点实验室厦门大学化学化工学院，固体表面物理化学国家重点实验室厦门大学化学化工学院 福建厦门361005，福建厦门361005，福建厦门361005 |
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| 基金项目： | 教育部骨干教师和国家自然科学基金(20023001和20021002)资助 |
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| 摘 要： | 经胺基官能团化介孔分子筛负载型CuCl2催化剂,表现出较高的甲醇转化率和碳酸二甲酯(DMC)收率以及较好的催化剂寿命.采用XRD、XPS和BET等对催化剂的体相结构和表面物种进行研究表明:(1)所合成介孔分子筛具有2～4nm的规整孔通道,足以容纳胺基官能团和CuCl2物种,同时留下供反应分子扩散和反应的适度空间,产生足够高的反应活性;(2)CuCl2与胺基之间存在的配位作用,有利于稳定活性中心铜离子,并使在甲醇气相氧化羰化制碳酸二甲酯反应条件下Cu(II)/Cu(I)之间的"氧化 还原"过程易于进行.
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| 关 键 词： | 介孔分子筛 胺基官能团化 CuCl2 甲醇 氧化羰化 碳酸二甲酯 |
Supported CuCl_2 Catalysts for Vapor Phase Oxidative Carbonylation of Methanol to Dimethyl Carbonate |
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| CAO Wei,ZHU Ming-xia,YUAN You-zhuollege of Chemistry and Chemical Engineering,Xiamen University,Xiamen ,China). Supported CuCl_2 Catalysts for Vapor Phase Oxidative Carbonylation of Methanol to Dimethyl Carbonate[J]. Journal of Xiamen University(Natural Science), 2004, 0(3) |
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| Authors: | CAO Wei ZHU Ming-xia YUAN You-zhuollege of Chemistry Chemical Engineering Xiamen University Xiamen China) |
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| Affiliation: | CAO Wei,ZHU Ming-xia,YUAN You-zhu~*ollege of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China) |
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| Abstract: | Pure silica mesoporous molecular sieves MCM-41 and MCM-48 organofunctionalized with 3-aminopropyltrimethoxysilane and N-[(3-trimethoxysilyl) propyl]ethylenediamine, respectively, were served as supports to immobilize CuCl_2 with conventional impregnation method. The supported Cu catalysts showed a considerable enhancement in the reaction rate in heterogeneous vapor-phase oxidative carbonylation of methanol to produce dimethyl carbonate in comparison with that obtained by CuCl_2 supported on non-functionalized mesoporous silicas under identical conditions. The electronic donation of the amino-groups, the accessibility and dischargeability of reactants in the regular mesopores probably account for the good catalytic performance as evidenced by the characteristic studies with XRD, BET, TG-DTA and XPS. |
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| Keywords: | MCM-41 MCM-48 amino-functionalization copper catalyst methanol oxidative carbonylation dimethyl carbonate |
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