硅酸盐通报2017,Vol.36Issue(9):2913-2922,10.
MFI型金属硅酸盐合成、介孔改性与骨架原子脱除行为
Synthesis,Mesopore Modification and Framework Atoms Removal of Diverse Metallosilicates with MFI Structure
摘要
Abstract
High-silica metallosilicates with MFI structure , viz.ZSM-5, FeMFI, TS-1 and super high-silica ZSM-5 ( SH-ZSM-5 , mloe ratio Si/Al=402 .4 ) , were synthesized using inorganic raw materials . Mesoporous modification was performed on such protonic zeolites by extracting Si and metallic heteroatom ( M =Al, Fe or Ti ) from framework. The crystal structure , metallic incorporation fraction and mesoporosity were investigated by XRD , FT-IR, UV-vis, N2 adsorption-desorption at 77 K, and SEM/EDX to probe the behavior of framework desilication and demetalation .It is concluded that Si/M molar ratios for the modified zeolites appeared to decrease compared with those of individual precursors , whilst the highly selective desilication observed on isomorphous heterosilicates was shown to facilitate the formation of hierarchically micro-and mesoporous structures with significant textural mesoporosity .The introduction of mesopores in zeolite crystals led to dramatic increases both in of BET surface area and in total micro-and mesopore volume .However , the formation of mesostructure in MFI framework could be affected by different factors ,e.g.the charge density in zeolite framework , the variety of incorporated metal atoms, the changes in crystal morphology and size .The removal efficiency of framework T-atoms was observed typically to descend in the sequence of ZSM-5, FeMFI and TS-1, whereas the relative weight yield and T-atoms removal efficiency decreased for TS-1 and SH-ZSM-5 crystals occurring in aggregation state due to their immoderate desilication .关键词
MFI型沸石/同晶取代/碱酸处理/多级孔结构/脱硅选择性/T-原子脱除效率Key words
MFI zeolite/isomorphous substitution/alkali-acid treatment/hierarchical porous structure/desilication selectivity/T-atoms removal efficiency分类
化学化工引用本文复制引用
韩静宇,张莉,王洪涛,张舒冬,金英杰..MFI型金属硅酸盐合成、介孔改性与骨架原子脱除行为[J].硅酸盐通报,2017,36(9):2913-2922,10.基金项目
国家自然科学基金(21171083) (21171083)