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MFI型金属硅酸盐合成、介孔改性与骨架原子脱除行为

韩静宇 张莉 王洪涛 张舒冬 金英杰

硅酸盐通报2017,Vol.36Issue(9):2913-2922,10.
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

韩静宇 1张莉 1王洪涛 1张舒冬 2金英杰1

作者信息

  • 1. 辽宁石油化工大学化学化工与环境学部,抚顺 113001
  • 2. 中国石化抚顺石油化工研究院,抚顺 113001
  • 折叠

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)

硅酸盐通报

OA北大核心CSCDCSTPCD

1001-1625

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