沸石
催化作用
烷基
化学
结晶度
酮
选择性
水溶液
分子筛
有机化学
化学工程
结晶学
工程类
作者
Xiaozhe Hou,Zhenjiang Yao,Haojie Li,Miao Wang,Ying Wei,Ling Zhang,Yan Liang,Junjun Qiao,Jingbo Jia,Runduo Zhang
标识
DOI:10.1016/j.micromeso.2022.112340
摘要
Extra-large-pore germanosilicate zeolite ITT was prepared with several structure-tailored alkyl-substituted imidazolium templates. The effect of alkyl chain length and substitution number of template on zeolite topology structure was studied with the variation of synthesis Si/Ge ratio. 1-hexyl-3-methyl-imidazaolium (1H3M) exhibited superior templating effect on the formation of ITT structure within the widest range of synthesis Si/Ge molar ratio of about 2–6. 1H→13C CP/MAS NMR, TGA and molecular simulation results revealed that two 1H3M was occluded in the 18-ring channels per unit cell, presenting the lowest interaction energy with framework. With the combination of XRD, SEM, EDS, ICP, 29Si, 19F MAS NMR, FTIR, N2 physisorption results, it was found that the increase of synthesis Si/Ge ratio improved framework Si/Ge ratio within d4r unit to a certain degree, and in the meantime resulted in the decrease of zeolite crystallinity with the formation of some amorphous phase. ITT showed better Lewis-acid catalytic activity and lactone selectivity for B–V oxidation of 2-adamantanone than BEC, the best germanosilicate zeolite ever reported. The excellent catalytic performance was ascribed to the presence of 18-ring channels in ITT, which facilitated the diffusion of bulky ketone substrate and lactone product. The structure stability of ITT during the reaction was evaluated with the use of either aqueous H2O2 or non-aqueous tert-butyl hydroperoxide (TBHP) as oxidant.
科研通智能强力驱动
Strongly Powered by AbleSci AI