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作 者:商永臣[1,2] 张文祥[1] 李彤[3] 吴通好[1]
机构地区:[1]吉林大学化学学院 [2]哈尔滨师范大学化学系,黑龙江哈尔滨150080 [3]哈尔滨师范大学化学系
出 处:《催化学报》2004年第2期158-162,共5页
基 金:国家自然科学基金资助项目 ( 2 0 2 73 0 2 5 ) ;黑龙江省教育厅资助项目 ( 10 5 3 10 83 )
摘 要:采用动态和静态水热合成法合成了不同Si/Al比的MCM 4 9分子筛 ,并考察了合成分子筛对 1 丁烯骨架异构化反应的催化性能 .结果表明 ,除目的产物异丁烯外 ,主要副产物为丙烯和戊烯 ,产物中没有检测到C6以上的副产物 .异丁烯收率随着反应温度的升高、分子筛晶粒的增大和 1 丁烯分压的降低而升高 .NH3 TPD结果表明 ,随着分子筛Si/Al比的增加 ,分子筛的酸中心数减少 ,导致副产物选择性下降 ,异丁烯选择性升高 .根据反应结果讨论了异丁烯及副产物形成的机理 .MCM-49 molecular sieve with different Si/Al ratios was synthesized hydrothermally under static condition and dynamic condition (autoclave rotated at 60 r/min), and its catalytic performance for skeletal isomerization of 1-butene was studied. The reaction results indicated that, besides the aim product isobutene, propylene and pentenes formed by dimerization-cracking reaction or oligomerization-cracking reaction were the main by-products, and the hydrocarbons higher than C 6 were not detected. Moreover, the yield of isobutene increased with the increase of reaction temperature and molecular sieve crystallite as well as the decrease of 1-butene partial pressure. The NH 3-TPD result indicated that the amount of acid sites decreased with the increase of Si/Al ratio in molecular sieve, which resulted in slower secondary reaction rate and higher selectivity for isobutene. On the basis of these results, the formation mechanism of isobutene and other by-products on MCM-49 was discussed.
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