无机盐工业
主管:中海油天津化工研究设计院有限公司
主办:中海油天津化工研究设计院有限公司
   中海油炼油化工科学研究院(北京)有限公司
   中国化工学会无机酸碱盐专业委员会
ISSN 1006-4990 CN 12-1069/TQ
催化材料

以酸解正硅酸乙酯为硅源合成ZSM-5分子筛的过程调控

  • 陈彦广 ,
  • 韩彤 ,
  • 张亚男 ,
  • 杨秀琪 ,
  • 韩洪晶 ,
  • 王皓
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  • 1.东北石油大学化学化工学院,黑龙江大庆 163318
    2.黑龙江省石油与天然气化工省重点实验室
陈彦广(1977— ),男,博士,教授,研究方向为催化材料制备过程调控及能源催化转化利用;E-mail: ygchen79310@126.com。

收稿日期: 2020-01-26

  网络出版日期: 2020-07-13

基金资助

国家自然科学基金(51674089);国家自然科学基金(21908021);黑龙江省杰出青年科学基金(JC2018002);黑龙江省博士后科研发展基金(LBH-Q16037);东北石油大学研究生创新计划项目(JYCX-CX03-2018)

Process regulation of ZSM-5 zeolite synthesis from hydrolyzed tetraethyl orthosilicate as silicon source in acidic medium

  • Yanguang Chen ,
  • Tong Han ,
  • Yanan Zhang ,
  • Xiuqi Yang ,
  • Hongjing Han ,
  • Hao Wang
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  • 1.College of Chemistry and Chemical Engineering,Northeast Petroleum University,Daqing 163318,China
    2.Heilongjiang Provincial Key Laboratory of Oil and Gas Chemical Technology

Received date: 2020-01-26

  Online published: 2020-07-13

摘要

正硅酸乙酯(TEOS)作为合成ZSM-5分子筛的常用硅源,其在不同酸碱介质中水解的前驱体聚合状态对ZSM-5分子筛的粒径和孔径分布具有调控作用。以酸性介质TEOS水解缩合的前驱体为硅源,在水热条件下合成ZSM-5分子筛,并利用XRD、SEM、BET、FI-IR等方法对反应不同阶段的样品进行表征分析。主要考察了水解程度、水解时间、合成过程的pH、晶化温度、晶化时间及模板剂用量对ZSM-5分子筛合成过程的调控,结果表明:以乙醇为共溶剂,以TEOS在硫酸介质pH=2.0时水解20 h的前驱体为硅源,水热合成过程中加入模板剂四丙基氢氧化铵(TPAOH),铝源为氢氧化铝,180 ℃晶化30 h合成了粒径约为200 nm的ZSM-5分子筛,其比表面积提高了35.6%,平均孔径降低了48.6%。

本文引用格式

陈彦广 , 韩彤 , 张亚男 , 杨秀琪 , 韩洪晶 , 王皓 . 以酸解正硅酸乙酯为硅源合成ZSM-5分子筛的过程调控[J]. 无机盐工业, 2020 , 52(7) : 88 -93 . DOI: 10.11962/1006-4990.2019-0444

Abstract

Tetraethyl orthosilicate(TEOS) is usually used as the silicon source for the synthesis of ZSM-5 zeolite.The polymerization state of the precursors hydrolyzed in different acid-base media had a regulatory effect on the grain size and pore size distribution of ZSM-5.The precursor of hydrolysis and condensation of TEOS in acidic medium was used as the silicon source.ZSM-5 was synthesized under hydrothermal conditions,and the samples at different stages during the reaction were characterized by XRD,SEM,BET and FI-IR.The effects of hydrolysis degree,hydrolysis time,pH of synthesis process,crystallization temperature,crystallization time and template dosage on the synthesis of ZSM-5 zeolite were investigated.The results showed that when the ethanol was used as co-solvent,the precursor of TEOS hydrolyzed for 20 h in sulfuric acid medium(pH=2.0) was used as silicon source,tetrapropylammonium hydroxide(TPAOH) was added during the hydrothermal synthesis process,and Al(OH)3 was used as aluminum source,the ZSM-5 zeolite with the crystal grain size(about 200 nm) was synthesized that crystallized at 180 ℃ for 30 h.The specific surface area of ZSM-5 zeolite was increased by 35.6% and the average pore size was decreased by 48.6%.

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