廉价原料制备钛硅沸石  

Preparation of low\|cost titanium silicalites

作　　者：王祥生 郭新闻 

机构地区：[1]大连理工大学碳资源综合利用开放实验室,辽宁大连116012

出　　处：《大连理工大学学报》2000年第2期155-159,共5页Journal of Dalian University of Technology

基　　金：中国石油化工总公司和国家自然科学基金委联合资助项目!(重大项目29792071)

摘　　要：采用Ti4 + 同晶取代Si4 + 的气固相取代法及水热晶化法制备了钛硅沸石 (TS 1) .1H→13CCP/MASNMR谱的研究结果表明 ,水热晶化法合成时 ,可用TPABr(四丙基溴化铵 )代替TPAOH(四丙基氢氧化铵 ) ,并可把n(TPA+ ) /n(SiO2 )降至 0 .0 5 ;在有TPA+ 存在时 ,有机碱只能起调节凝胶碱度的作用 ;模板作用的顺序是TPA+ (四丙基铵离子 ) >TBA+ (四丁基铵离子 )>TEA+ (四乙基铵离子 ) >有机胺 .用丙烯环氧化反应为探针 ,考察了不同碱源合成的TS 1的催化性能 ,发现以正丁胺、二乙胺、己二胺和TBAOH(四丁基氢氧化铵 )为碱源均可得到催化性能较好的TS 1.采用TPABr为模板剂 ,正丁胺为碱源在 10 0L釜中进行了放大 .结果表明 ,10 0L与 2L釜中合成的TS 1的催化性能相当 .以含硼沸石为母体 ,采用“筑窝植钛”的构思 ,用气固相法合成出了Ti ZSM 5沸石 ,考察了以不同n(SiO2 ) /n(B2 O3 )Low\|cost titanium silicalites were prepared by gas solid isomorphous substitution and hydrothermal method. The results show that,when TS\|1 is prepared by hydrothermal method, TPAOH can be replaced by TPABr whose amount can be decreased to 0.05 [ n (TPA +)/ n (SiO 2)]; when n (TPA +)/ n (SiO 2)≥0.05, organic base can not act as the templating agent, but regulating the basicity of the gel; the order of the templating effect is as follows: TPA +>TBA +>TEA +>organic amine. The epoxidation properties of propylene with dilute H 2O 2 on TS\|1 prepared by using different bases were studied. The results show that, TS\|1 prepared by using n \|butylamine, diethylamine, 1,6\|hexanediamine or TBAOH as the base has good catalytic properties. Moreover, TS\|1 was prepared in a 100 L stainless steel autoclave, using TPABr as the template and n \|butylamine as the base. By gas\|solid isomorphous substitution, Ti\|ZSM\|5 was prepared by using B\|ZSM\|5 as the precursor, and the chemical\|physics properties as well as the propylene epoxidation properties of titanium silicalites prepared by using B\|containing zeolites with different n (SiO 2)/ n (B 2O 3) as the precursor were studied.

关 键 词：水热晶化 Ti-ZSM5 钛硅沸石 制备 原料 

分 类 号：TQ424.25[化学工程] O643.36[理学—物理化学]