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作 者:任申勇[1] 张敏[1] 陈尧 张宇琪[1] 申宝剑[1] 徐春明[1] REN Shenyong;ZHANG Min;CHEN Yao;ZHANG Yuqi;SHEN Baojian;XU Chunming(State Key Laboratory of Heavy Oil Processing,the Key Laboratory of Catalysis of CNPC,College of Chemical Engineering and Environment,China University of Petroleum,Beijing 102249,China)
机构地区:[1]中国石油大学(北京)化学工程与环境学院,重质油全国重点实验室,CNPC催化重点实验室,北京102249
出 处:《分子催化(中英文)》2025年第2期154-165,I0003,共13页Journal of Molecular Catalysis(China)
基 金:国家自然科学基金创新研究群体科学基金(22021004)。
摘 要:由于受到分子筛催化剂孔道内的扩散限制,高碳烯烃环氧化反应往往活性较低.本文采用预晶化液补水和硅源的方案合成小晶粒TS-1分子筛,同时减少模板剂的用量降低了合成成本.小晶粒TS-1分子筛的催化扩散路径明显缩短,同时其晶粒间形成晶间介孔结构,有利于反应物分子的传质,大大提高了其催化高碳烯烃环氧化的性能.在催化1-己烯与H_(2)O_(2)的环氧化反应中表现出较好的转化率和环氧己烷的选择性.实验发现随着预晶化凝胶中n(H_(2)O)/n(SiO_(2))比值的降低,以及预晶化温度的升高,TS-1沸石的晶粒也随之减小.Due to diffusion limitation in zeolite catalyst pores,epoxidation reaction of high carbon olefins often has lower activity.This article adopted a method to add silicon source and water into a pre-crystallization solution to synthesize small grain TS-1 zeolite,which reduced the amount of template agent and thus lowered the synthesis cost.The catalytic diffusion path of small grain TS-1 zeolite was significantly shortened,and at the same time,an intergranular mesoporous structure was formed between its grains,which was conducive to the mass transfer of reactant molecules and greatly improved its performance in catalyzing the epoxidation of high carbon olefins.The small grain TS-1 zeolite exhibited good conversion rate and selectivity for epoxyhexane in catalyzing epoxidation reaction of 1-hexene with H_(2)O_(2).It was found that with the decrease of n(H_(2)O)/n(SiO_(2)) ratio in the pre-crystallizing gel and the increase of pre-crystallizing temperature,the crystal size of TS-1 zeolite also decreased.
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