ZSM-5薄层沸石协同晶化及其MTP催化性能研究  

Study on cooperative synthesis of nanolayered ZSM-5 and its catalytic performance in methanol-to-propylene reaction

作　　者：朱小春 张腾跃 赵红娟 张磊[1,3] 刘宏海[2] 申宝剑 ZHU Xiao-chun;ZHANG Teng-yue;ZHAO Hong-juan;ZHANG Lei;LIU Hong-hai;SHEN Bao-jian(CNPC Key Laboratory of Catalysis,State Key Laboratory of Heavy Oil Processing,College of Chemical Engineering and Environment,China University of Petroleum-Beijing,Beijing 102249,China;Lanzhou Petrochemical Research Center,PetroChina Petrochemical Research Institute,Lanzhou 730060,China;PetroChina Guangxi Petrochemical Company,Qinzhou 535008,China)

机构地区：[1]中国石油大学(北京),重质油国家重点实验室,中国石油天然气集团(CNPC)催化重点实验室,北京102249 [2]中国石油石油化工研究院兰州化工研究中心,甘肃兰州730060 [3]中国石油广西石化公司,广西钦州535008

出　　处：《现代化工》2024年第10期81-87,共7页Modern Chemical Industry

基　　金：国家自然科学基金(U1862106);中国石油国际合作项目(KYWX-22-006)。

摘　　要：调整双季铵盐表面活性剂与单季铵盐表面活性剂的使用量,通过协同晶化的方式合成了高结晶度、高介孔容的薄层ZSM-5沸石。利用XRD、XRF、SEM、TEM、NH3-TPD、低温氮气物理吸脱附以及27Al MAS NMR对沸石样品进行表征,并评价其甲醇制丙烯反应(MTP)催化性能。结果表明,薄层沸石的b轴厚度随着双季铵盐表面活性剂使用量的减少而增加,适量的单季铵盐表面活性剂的加入可以起到协同晶化的作用,能够有效稳定胶束,从而调控沸石的形貌。优化2种季铵盐表面活性剂的使用量所得薄层ZSM-5沸石的比表面积和介孔孔容都有所增加,在甲醇制丙烯反应中的活性稳定性也得到较大改善。此外,协同晶化的方式减少了双季铵盐表面活性剂的使用,有利于降低薄层ZSM-5沸石的合成成本。Nanolayered ZSM-5 zeolites with high crystallinity and large mesopore volume are prepared through cooperative synthesis mode by adjusting the dosages of bi-quaternary ammonium surfactant and mono-quaternary surfactant,and characterized in detail by means of XRD,XRF,SEM,TEM,NH3-TPD,low-temperature nitrogen physisorption,and 27Al MAS NMR.Furthermore,their catalytic performance for methanol-to-propylene reaction(MTP)is evaluated.It is shown that C16-6-6 is able to synthesize nanolayered ZSM-5 effectively,but the b-axis thickness of nanolayered ZSM-5 zeolite inevitably increases as the dosage of C16-6-6 decreases in the gel.It is found that the addition of an appropriate amount of low-cost C16-3 can play a synergistic role during the crystallization,which can effectively stabilize the micelles and tune the thickness of the nanolayered ZSM-5 zeolites.Through optimizing the dosages of C16-6-6 and C16-3 in the synthesis,the specific surface area and mesopore volume of the nanolayered zeolites prepared increase,and the stability of catalytic activity of the resulting zeolite samples in methanol-to-propylene reaction is also significantly improved.Most importantly,the cooperative synthesis reduces the using amount of expensive C16-6-6,which is beneficial to reduce the synthesis cost of nanolayered ZSM-5 zeolite.

关 键 词：薄层ZSM-5沸石 季铵盐表面活性剂 协同晶化 低成本 甲醇制丙烯 

分 类 号：TQ426[化学工程]