介孔分子筛固载RhCl(TPP)_3催化醋酸甲酯羰基化合成双醋酸亚乙酯

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英文篇名：Synthesis of ethylidene diacetate by carbonylation of methyl acetate catalyzed by mesoporous materials supported RhCl(TPP)_3 complexes 作者：荣俊 ; 韩武刚 ; 孙玥 ; 陈树伟 ; 李瑞丰 英文作者：RONG Jun;HAN Wu-gang;SUN Yue;CHEN Shu-wei;LI Rui-feng;College of Chemistry and Chemical Engineering, Taiyuan University of Technology;Key Laboratory of Coal Science and Technology of Ministry Education; 关键词：介孔分子筛 ; RhCl(TPP)_3 ; 醋酸甲酯 ; 羰基化 ; 双醋酸亚乙酯 ; 醋酐 英文关键词：mesoporous molecular sieves;;RhCl(TPP)_3;;methyl acetate;;carbonylation;;ethylidene diacetate;;acetic anhydride 中文刊名：TRQH 英文刊名：Natural Gas Chemical Industry 机构：太原理工大学化学化工学院;煤科学与技术教育部重点实验室; 出版日期：2019-04-25 出版单位：天然气化工(C1化学与化工) 年：2019 期：v.44;No.245 基金：国家自然科学基金(21546009);; 山西三维集团股份有限公司合作项目,横向(校内编号2012228) 语种：中文; 页：TRQH201902008 页数：7 CN：02 ISSN：51-1336/TQ 分类号：38-43+59

摘要

利用自由配体法将RhCl(TPP)_3配合物封装于介孔分子筛的孔道中,制备了RhCl(TPP)_3/SBA-16、RhCl(TPP)_3/SBA-15、RhCl(TPP)_3/MCM-41催化剂。采用元素分析(ICP-AES)、粉末X射线衍射(XRD)、N_2吸附-脱附、扫描电镜(SEM)、红外光谱(FT-IR)等物理化学方法对所制材料进行了表征。结果表明,采用自由配体法可将RhCl(TPP)_3有效固载于介孔分子筛介孔孔道中。在160℃、6.0MPa合成气(V(CO):V(H_2)=2:1)压力下以碘甲烷为助催化剂,反应6.0h,考察不同催化剂应用于醋酸甲酯羰基化生成双醋酸亚乙酯(EDA)的催化效果。结果表明,RhCl(TPP)_3/SBA-16催化剂具有更好的催化效果,以及较好的可重复利用性。
        The catalysts of RhCl(TPP)_3 encapsulated in the pores of SBA-16, SBA-15 and MCM-41 mesoporous molecular sieves were prepared by flexible ligand method, and were characterized by ICP-AES, XRD, N_2 adsorption-desorption, SEM and FT-IR. The results showed that the complex RhCl(TPP)_3 can be entrapped in the pores of those mesoporous materials. In carbonylation of methyl acetate to ethylidene diacetate at 160℃, 6.0 MPa, CO/H_2 volume ratio of 2 and reaction time of 6h, the catalysts were applied in the presence of CH_3I to investigate their catalytic performance. Among the catalysts, RhCl(TPP)_3/SBA-16 exhibited optimal catalytic performance, and had better stability and reusability.

引文

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