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首页> 外文期刊>Bulletin of the Chemical Society of Japan >The Alkylation of Biphenyl over Fourteen-Membered Ring Zeolites.The Influence of Zeolite Structure and Alkylating Agent on the Selectivity for 4,4'-Dialkylbiphenyl
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The Alkylation of Biphenyl over Fourteen-Membered Ring Zeolites.The Influence of Zeolite Structure and Alkylating Agent on the Selectivity for 4,4'-Dialkylbiphenyl

机译：十四元环沸石中联苯的烷基化。沸石结构和烷基化剂对4,4'-二烷基苯基选择性的影响

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摘要

Alkylation,i.e.isopropylation,s-butylation,and t-butylation,of biphenyl (BP) was examined over fourteen-mem-bered ring (14-MR) zeolites,CIT-5,UTD-1,and SSZ-53,in order to elucidate the relationships between structure of zeolites and bulkiness of alkylating agents on the shape-selective catalysis.CIT-5 zeolite (CFI) yielded 4,4'-diisopropyl-biphenyl (4,4'-DIPB) in the level of 50-60% in the isopropylation in the range of 150-300 °C.2,2'-,2,3'-,and 2,4'-DIPB (2,x'-DIPB) isomers were obtained as the predominant DIPB isomers at lower temperatures,and the formation of 3,4'-and 3,3'-DIPB isomers increased with an increase in the temperature.However,the selectivities were in the level of 10-15% for UTD-1 (DON) and SSZ-53 (SFH) zeolites in the range of 150-350 °C.The s-butylation with 1-butene gave results similar to the isopropylation,although the selectivities for 4,4'-di-s-butylbiphenyl (4,4'-DSBB) were higher than those for 4,4'-DIPB at 250 °C:80-85% for CFI,40-50% for DON,and 30-40% for SFH.High selectivity for 4,4'-di-t-butylbiphenyl (4,4'-DTBB) was observed in the t-butylation at 250 °C:95% for CFI,90% for DON,and 80% for SFH.These differences are due to the spatial difference in their channels,and also due to bulkiness of alkylating agents,propene,1-butene,and 2-methylpropene.The selectivity for 4,4'-dialkylbiphenyl (4,4'-DABP) was governed by the exclusion of the bulky DABP isomers at the transition state by steric restriction in the zeolite channels.
机译：将烷基化，二异丙基化，求叔丁酯和叔丁基化在14- Membered环（14-MR）沸石，CIT-5，UTD-1和SSZ-53上进行检查为了阐明形状选择性催化作用沸石结构与烷基化试剂的大多全的关系。在50-的水平中产生4,4'-二异丙基 - 联烯基（4,4'-DIPB）的Cit-5沸石（CFI）。在150-300℃的异丙中60％，2,3' - 和2,4'-DIPB（2，X'-DIPB）异构体作为主要的DIPB异构体获得在较低的温度下，3,4'-and 3,3'-dipb异构体的形成随着温度的增加而增加。然而，选择性均为UTD-1（DON）和SSZ-53（SFH）沸石在150-350℃的范围内。具有1-丁烯的S-丁基化与异丙基化相似的结果，尽管4,4'-Di-S-丁基苯基的选择性（4,4 '-DSBB）高于4,4'-DIPB，在250°C：80-85％的CFI，唐40-50％，S的40-50％在250℃下的叔丁基化中观察到4,4'-二叔丁基苯基（4,4'-DTBB）的选择性：95％的CFI，90％用于DON，80％用于SFH这些差异是由于其通道的空间差异，并且还原是由于烷基化试剂，丙烯，1-丁烯和2-甲基前丙烯的膨胀。4,4'-二烷基苯苯基的选择性（4,4'-DABP）通过在沸石通道中的空间限制来排除在过渡状态下庞大的DABP异构体排除。

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