摘要
研发缓和反应条件下异丁烯胺化生产叔丁胺(原子经济型绿色化工过程)高性能催化剂对于该反应具有重要意义,采用氢氧化钠(NaOH)与十六烷基三甲基溴化铵(CTAB)混合液处理不同模板剂六亚甲基亚胺(HMI)含量的MCM-49分子筛,制备了一系列不同物化性质的MCM-49样品,考察了其在异丁烯胺化过程中的反应性能。结果表明,随着初始样品中模板剂含量的降低(模板剂对分子筛骨架保护作用减弱),经处理后,催化剂样品的比表面积、外表面积及介孔孔容显著增大,结晶度有所降低,而中强酸量先增大后降低。C150-NaOH/CTAB和C250-NaOH/CTAB样品,在保持较高结晶度的同时,其酸量比H型样品有显著升高,并在异丁烯胺化过程呈现出较佳的反应活性;异丁烯转化率与催化剂中强酸量呈线性正相关,而与样品的织构性质及多级孔结构无明显关联性。
Developing highly efficient catalyst under mild reaction conditions（relative lower pressure and temperature）is of great significance for the isobutylene amination process,which is an atom economic and green chemical process.A series of modified hierarchical MCM-49 catalysts,prepared by NaOH and cetyltrimethylammonium bromide（CTAB）alkaline treatment of MCM-49 zeolite with different hexamethyleneimine（HMI）template agent contents, with different texture properties and acidity were tested in isobutylene amination process under mild conditions.The results indicate that,after treatment,the specific surface,the external surface and the mesopore volume become remarkably increased,while the crystallinity is slightly declined.But the mid-strong acid becomes firstly increased and then decreased.The C150-NaOH/CTAB and C250-NaOH/CTAB samples,with higher crystallinity and amount of acidity,show much better reactive activity than MCM-49 in isobutylene amination process.The reaction activity of the samples is closely related to the amount of acid sites with mid-strong acidity,rather than the textural properties and hierarchical porosity.
作者
高尚耀
江南
朱向学
陈福存
谢素娟
魏会娟
李秀杰
王玉忠
安杰
刘盛林
徐龙伢
GAO Shangyao;JIANG Nan;ZHU Xiangxue;CHEN Fucun;XIE Sujuan;WEI Huijuan;LI Xiujie;WANG Yuzhong;AN Jie;LIU Shenglin;XU Longya(Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;Shandong NHU Amino Acid Co.,Ltd.,Weifang 261041,China;Nanjing Rongxin Chemical Co.,Ltd.,Nanjing 210047,China;Yanshan Branch,Beijing Research Institute of Chemical Industry,SINOPEC,Beijing 102500,China)
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
2018年第4期811-816,共6页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
中国科学院王宽诚率先人才计划
大连市高层次人才创新支持计划项目(2015R009)资助
关键词
异丁烯
胺化
叔丁胺
MCM-49分子筛
碱处理
isobutylene
amination
tert -butylamine
MCM-49 zeolite
alkaline treatment
