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M(La, Ni, Cr)_xO_y/nano-HBeta分子筛催化2-甲萘与甲醇烷基化性能研究
Catalytic Alkylation of 2-naphthalene with Methanol by M(La, Ni, Cr)xOy Modified Nano-HBeta Zeolite
【摘要】 采用低温-高温二步晶化法动态水热合成制备了椭球形貌纳米HBeta分子筛,采用金属盐溶液等体积浸渍制备了La2O3、Cr2O3以及NiO负载HBeta分子筛,采用XRD、N2吸附-脱附、SEM、NH3-TPD及Py-FTIR等手段对样品的结构、酸性进行表征,并对其催化2-甲萘与甲醇烷基化反应的催化性能进行了研究。结果表明,金属氧化物改性降低了HBeta的结晶度、比表面积和平均孔径。Cr2O3和La2O3改性保持了酸强度分布而明显降低了Cr2O3/HBeta的中强酸酸量;NiO/HBeta上Lewis酸量增加且酸强度降低。La2O3和Cr2O3改性样品的三甲基萘副产物选择性增加,2,6-二甲基萘(2,6-DMN)选择性下降。NiO/HBeta上初始催化活性下降,但产物中二甲基萘(DMNs)选择性增加,2,6-DMN收率由2.52%提高至3.31%。随着反应时间延长,样品的催化活性均下降而2,6-DMN选择性提高,La2O3/HBeta在反应5 h获得4.41%的2,6-DMN收率。
【Abstract】 Nano-HBeta molecular sieves with ellipsoid morphology were prepared via two-step crystallization dynamic hydrothermal method.La2O3、Cr2O3 and NiO modified HBeta catalysts were prepared by equal volume impregnation of metal salt solution.The structure and acidity of the samples were characterized by XRD,N2 adsorption-desorption, SEM、NH3-TPD and Py-FTIR,and the catalytic performance of the samples on the alkylation of 2-methylnaphthalene with methanol was studied.The results show that metal oxide modification reduced the crystallinity, specific surface area and average pore size of HBeta.Cr2O3 and La2O3 kept the distribution of acid strength but decreased the amounts of medium strength acid on Cr2O3/HBeta.The acid strength of NiO/HBeta decreased and the Lewis acid amounts increased significantly.The selectivity to trimethyl naphthalene by-products over La2O3 and Cr2O3 modified HBeta increased, while the selectivity to 2,6-dimethylnaphthalene(2,6-DMN)decreased.The initial catalytic activity of NiO/HBeta decreased, however the selectivity to dimethylnaphthalene(DMNs) increased, and the yield of 2,6-DMN increased from 2.52% to 3.31%.With the increase of reaction time, the catalytic activity of the samples decreased while the selectivity to 2,6-DMN increased, and the yield of 2,6-DMN reached to 4.41% over La2O3/HBeta on 5 h.
【Key words】 HBeta zeolite; metal oxide; 2-methylnaphthalene; alkylation;
- 【文献出处】 有色金属工程 ,Nonferrous Metals Engineering , 编辑部邮箱 ,2022年05期
- 【分类号】TQ241.52;TQ426
- 【下载频次】42