文献类型：期刊文献

中文题名：TS-1后处理改性对其丁酮氨氧化反应的影响

英文题名：Tuning Catalytic Performance of TS-1 Zeolite for Ammoxidation of Methyl Ethyl Ketone by Post-Treatment with Alkaline Solutions

作者：李金霞[1];王丽[1];王筠松[1];郭耘[1];郭杨龙[1];詹望成[1]

机构：[1]华东理工大学工业催化研究所

年份：2018

卷号：42

期号：9

起止页码：943

中文期刊名：稀有金属

外文期刊名：Chinese Journal of Rare Metals

收录：CSTPCD;;EI(收录号：20185206305357);Scopus;北大核心:【北大核心2017】；CSCD:【CSCD2017_2018】；

基金：国家自然科学基金项目(91545103)资助

语种：中文

中文关键词：钛硅分子筛;后处理改性;骨架Ti;锐钛矿TiO2;氨氧化

外文关键词：titanium silicalite;post-treatment;framework Ti;anatase TiO2;ammoxidation

摘要：采用叔丁胺和四丙基氢氧化铵混合碱溶液对TS-1（titanium silicalite-1）分子筛进行后处理改性，以构建介孔结构和调变分子筛中Ti物种的存在状态，从而提高TS-1分子筛的催化活性。通过系列表征手段重点研究了叔丁胺浓度和改性时间对TS-1分子筛物化性质以及丁酮氨氧化反应性能的影响。结果表明，TS-1经过混合碱溶液改性后，TS-1分子筛中产生了一定的介孔结构，同时锐钛矿TiO2几乎完全脱除，从而显著提高了其丁酮氨氧化反应活性。对于不同叔丁胺浓度和时间后处理改性的TS-1分子筛，相对结晶度以及不同Ti物种（骨架Ti、六配位非骨架Ti和锐钛矿TiO2）的含量是决定其活性的关键因素。以0．2mol·L^-1叔丁胺和TPAOH的混合溶液，在170℃下改性24h得到的TS-1具有最好的丁酮氨氧化反应活性，丁酮转化率和丁酮肟选择性分别为100％和98．6％。
Post-treatment of TS-1 （ titanium silicalite-1 ） zeolite with a mixture of tert-butylamine （TB） and terapropyl ammonium hy- droxide （TPAOH） was carried out to fabricate mesoporous structure and adjust the states of Ti species. The effect of TB concentration and treatment time on the physiochemical properties and the catalytic performance for ammoxidation of methyl ethyl ketone （MEK） of TS-1 was seriously noticed. The results showed that mesoporous structure could be produced and anatase TiO2 was completely elimina- ted after modification of TS-1, leading to the improvement of catalytic activity of TS-1. For TS-1 catalysts treated with different TB con- centrations and different time, the relative crystallinity and the contents of different titanium species （ framework Ti, non-framework Ti with six coordination and anatase TiO2 ） were the critical factors to determine its catalytic activity. After the post-treatment with the mixture of 0.2 mol·L^-1 of TB and TPAOH solution at 170 ℃ for 24 h, the TS-1 catalyst exhibited the highest activity with 100% conversion of MEK and 98.6% selectivity to methyl ethyl ketone oxime （MEKO）.