无粘结剂ZSM-5催化剂改性及其甲苯与乙烯择形烷基化反应的催化性能  

Modified Binder-free ZSM-5 and Its Catalytic Performance in Shape Selective Alkylation of Toluene with Ethylene

作　　者：沈震浩[1] 马翀玮 孙洪敏[1] 杨为民[1] SHEN Zhenhao;MA Chongwei;SUN Hongmin;YANG Weimin(Sinopec Shanghai Research Institute of Petrochemical Technology,State Key Laboratory of Green Chemical Engineering and Industrial Catalysis,Shanghai 201208,China)

机构地区：[1]中国石油化工股份有限公司上海石油化工研究院,绿色化工与工业催化国家重点实验室,上海201208

出　　处：《化学反应工程与工艺》2020年第6期491-497,共7页Chemical Reaction Engineering and Technology

基　　金：国家重点研发计划(2017YFB0702800)。

摘　　要：利用甲苯与乙烯的烷基化反应制备对甲乙苯,是一条具有技术经济性的合成工艺路线。本工作对无粘结剂ZSM-5分子筛催化剂颗粒进行了聚苯甲基硅氧烷(PPMS)修饰剂化学液相沉积(CLD)改性处理研究,考察了其对催化剂物化性质与择形烷基化反应性能的影响。在CLD改性过程中形成的SiO_(2)使ZSM-5孔口收窄、外表面酸性位点钝化,这可以有效阻止对甲乙苯异构化为间甲乙苯或邻甲乙苯。经过重复3次改性的无粘结剂ZSM-5可将对甲乙苯的择形选择性提高至97%以上,与改性的常规含粘结剂ZSM-5催化剂颗粒相比,CLD改性的无粘结剂ZSM-5催化剂颗粒具有更好的烷基化活性和反应稳定性。Production of Para-ethyltoluene(p-ET)via alkylation of toluene and ethylene is considered to be an economical pathway.In this work,binder-free ZSM-5 catalysts modified by chemical liquid deposition(CLD)of polyphenylmethylsiloxane(PPMS)were studied on the physicochemical properties and the shape selective catalytic performance.Through CLD modification,the open mouth of zeolitic channel was narrowed down by SiO_(2) formed,and the acid sites on external surface was passivated.As a result,the non-shape-selective isomerization of p-ET to m-ET or o-ET was suppressed.And the shape selectivity of p-ET was enhanced to more than 97%over binder-free ZSM-5 with three cycles of CLD modification.Compared with modified conventionally shaped ZSM-5 with alumina,CLD modified binder-free ZSM-5 catalysts showed better alkylation activity and stability.

关 键 词：对甲乙苯 择形烷基化 无粘结剂ZSM-5 催化剂 化学液相沉积 表面钝化 

分 类 号：O643.38[理学—物理化学]