3,5-二甲基苯溴化镁修饰的ZSM-5催化剂乙苯歧化反应
Ethylbenzene Disproportionation over ZSM-5 Modified by 3,5-Dimethyl Phenylmagnesium Bromide
作者单位E-mail
张英 贵州电网有限责任公司电力科学研究院, 贵阳 550002  
李军卫 贵州电网有限责任公司电力科学研究院, 贵阳 550002  
武静文 南京大学化学化工学院, 江苏省机动车尾气污染控制重点实验室, 南京 210093  
许波连 南京大学化学化工学院, 江苏省机动车尾气污染控制重点实验室, 南京 210093 xubolian@nju.edu.cn 
摘要: 采用尺寸较大的有机分子格式试剂(3,5-二甲基苯溴化镁)修饰ZSM-5催化剂,用乙苯歧化反应研究了修饰催化剂的择形性,并利用探针分子动力学扩散测试结合探针分子吸附红外等手段研究分子筛孔径和内外表面酸性性质等。结果表明,少量的3,5-二甲基苯溴化镁精确地中和了ZSM-5分子筛外表面的酸性中心,导致乙苯歧化反应中极高的对二乙苯选择性。而探针分子动力学结果表明,这种修饰并未引起分子筛孔道结构的变化。
关键词: ZSM-5分子筛  表面酸性  乙苯歧化  择形催化
基金项目: 中国南方电网公司科技项目(No.GZ2015-2-0048)资助项目
Abstract: A new kind of ZSM-5 surface modification method was developed by using a large organic molecule Grignard reagent (3,5-dimethyl phenylmagnesium bromide). Their shape selective catalytic properties were studied by ethylbenzene (EB) disproportionation reaction test. The pore structure and surface acid properties were also investigated to understand the shape selectivity enhancement mechanism. Most of the MgO was deposited on external surface due to the big molecule size of 3,5-dimethyl phenylmagnesium bromide. The elimination of external surface acid sites by Grignard reagent is the main reason of its high p-diethylbenzene (p-DEB) selectivity in EB disproportionation reaction. The results of probe molecule adsorption kinetics experiment indicate that this modification method does not change the pore size of ZSM-5.
Keywords: ZSM-5  surface acidic site  ethylbenzene disproportionation  shape selective catalysis
投稿时间:2017-07-09 修订日期:2017-09-27
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张英,李军卫,武静文,许波连.3,5-二甲基苯溴化镁修饰的ZSM-5催化剂乙苯歧化反应[J].无机化学学报,2017,33(12):2351-2356.
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