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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 被引量:2

Synthesis of ethylidene diacetate by carbonylation of methyl acetate catalyzed by mesoporous materials supported RhCl(TPP)_3 complexes
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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, N2 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℃, 6.0MPa, CO/H2 volume ratio of 2 and reaction time of 6h, the catalysts were applied in the presence of CH3I to investigate their catalytic performance. Among the catalysts, RhCl(TPP)3/SBA-16 exhibited optimal catalytic performance, and had better stability and reusability.
作者 荣俊 韩武刚 孙玥 陈树伟 李瑞丰 RONG Jun;HAN Wu-gang;SUN Yue;CHE Shu-wei;LI Rui-feng(College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology of Ministry Education, Taiyuan 030024, China)
出处 《天然气化工—C1化学与化工》 CAS CSCD 北大核心 2019年第2期34-39,55,共7页 Natural Gas Chemical Industry
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)
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 mesoporous molecular sieves RhCl(TPP)3 methyl acetate carbonylation ethylidene diacetate acetic anhydride
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