碱脱硅改性的ZSM-12分子筛择形催化合成2,6-二甲基萘的研究  被引量:4

Shape-selective synthesis of 2,6-dimethylnaphthalene over ZSM-12 zeolite modified by desilication in alkaline medium

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作  者:吴伟[1] 李凌飞[1] 武光[1] 吴维果[1] 杨巍[1] 托克塔列夫A.V. 基赫佳宁0.V. 伊切夫斯基G.V. 

机构地区:[1]黑龙江大学化学化工与材料学院功能无机材料化学省部共建教育部重点实验室,中俄联合催化实验室,黑龙江哈尔滨150080 [2]俄罗斯科学院西伯利亚分院鲍列斯科夫催化研究院,俄罗斯新西伯利亚市630090

出  处:《现代化工》2009年第6期40-43,45,共5页Modern Chemical Industry

基  金:中俄政府间合作项目(CR11-24);黑龙江省自然科学基金重点项目(ZD200820-02);黑龙江省科学技术计划项目(国际合作)(WC05A10)

摘  要:用NaOH水溶液处理ZSM-12分子筛制备了脱硅程度不同的改性ZSM-12分子筛,对样品进行了表征,并考察了改性前后分子筛对萘和甲醇烷基化反应的择形催化反应性能。结果表明用适宜浓度的NaOH溶液处理ZSM-12分子筛,在一定温度下通过改变碱处理时间能方便地调节分子筛晶体中产生的二次介孔结构的比例,并改变分子筛的酸性能。改性ZSM-12分子筛同时提高了对萘和甲醇烷基化反应的催化活性和目标产物2,6-二甲基萘的选择性,以0.8 mol/L的NaOH水溶液在65℃下处理1 h制备的改性ZSM-12分子筛为催化剂,在优化的反应条件下萘和甲醇烷基化反应4 h后的萘的转化率为58.3%,2,6-二甲基萘的选择性达到27.3%。The ZSM-12 zeolite with different degrees of desilication are prepared in NaOH solutions and characterized, and its catalytic performance in synthesis of 2, 6-dimethylnaphthalene by the methylation of naphthalene with methanol is also investigated. The results show that the proportion of mesopores framework in the zeolite crystal can be turned expediently by controlling time of desilicatiou at certain temperature in solutions with optimal concentration of NaOH, and the acidity also can be changed.The increase of activity of methylation of naphthalene with methanol and selectivity up to 2,6-DMN are observed over the ZSM-12 catalysts modified by the desilication process in alkaline medium because of diffusivity of products improved in the generated additional mesopores. The conversion of naphthalene and the selectivity to 2,6-DMN are 58.3% and 27.3%, respectively,over the HZSM-12 treated in 0.8 mol/L of NaOH at 65℃ for 1 hour under the optimum alkylation condition of naphthalene with mathano] after 4 hours of reaction.

关 键 词:ZSM-12分子筛 碱脱硅 二次介孔 烷基化 2 6-二甲基萘 

分 类 号:TQ426.61[化学工程]

 

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