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H-beta分子筛催化苯胺缩合制备二苯胺
Synthesis of diphenylamine by condensation of aniline over H-beta zeolite
【摘要】 对苯胺缩合生成二苯胺用H-beta分子筛催化剂进行研究,考察分子筛硅铝比和NH4F改性对H-beta分子筛催化苯胺缩合反应的影响,采用NH3-TPD和Py-IR对催化剂进行表征。结果表明,B酸是催化苯胺缩合的活性中心,低硅铝比与适当卤素处理均可提高B酸含量,有利于缩合反应。反应温度320℃,空速0. 2 h-1,0. 125 mol·L-1的NH4F溶液处理硅铝比为25的H-beta分子筛上,二苯胺的收率达到34. 68%。基于催化活性位点的研究,探讨了苯胺缩合反应机理。
【Abstract】 H-beta zeolite catalyst for the condensation of aniline to diphenylamine was studied. The effect of SiO2/Al2O3 ratio and NH4F modification on the condensation of aniline were investigated. The catalyst was characterized by NH3-TPD and Py-IR. It was found that Brnsted acid was the active center for aniline condensation,and the low ratio of SiO2/Al2O3 and the appropriate treatment by halogen could increase the content of Brnsted acid. The yield of diphenylamine was 34. 68% at the temperature of 320 ℃ and the space velocity of 0. 2 h-1 over H-beta zeolite with SiO2/Al2O3 ratio of 25 and modified by NH4F of 0. 125 mol·L-1. The mechanism of aniline condensation was discussed based on study of catalytic active sites.
【Key words】 fine chemical engineering; H-beta zeolite; aniline; diphenylamine; acid;
- 【文献出处】 工业催化 ,Industrial Catalysis , 编辑部邮箱 ,2020年03期
- 【分类号】TQ246.31
- 【被引频次】3
- 【下载频次】207