无介孔模板制备多级结构ZSM-5沸石分子筛
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- 英文论文题名：On the mesoporogen-free synthesis of single-crystalline hierarchically structured ZSM-5 zeolites in a dry gel system
- 论文作者：葛同广 ; 贺晓耘 ; 华子乐 ; 施剑林
- 英文论文作者：Tonguang Ge ; Xiaoyun He ; Zile Hua ; Jianlin Shi ; Shanghai Institute of Ceramics ; Chinese Academy of Sciences
- 年：2016
- 作者机构：中国科学院上海硅酸盐研究所;
- 论文关键词：多级结构沸石 ; 无介孔模板 ; 三维贯穿介孔 ; 准固相转化
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十二分会： 多孔功能材料
- 语种：中文
- 分类号：O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十二分会 ; 多孔功能材料
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：314k
- 原文格式：D
- 会议级别：全国
摘要
多级结构沸石同时具备高度晶化的微孔沸石骨架和介孔材料的高扩散通道,很好地解决了较大分子在微孔孔道的扩散结焦问题,在学术界和工业应用领域引起了广泛的关注。近年来虽然报道了很多关于制备多级结构沸石的工作,但是以往的合成方法主要集中在模板法(软模板、硬模板和自模板)和后处理的方法,在产生多级结构的过程当中不可避免地使用到介孔模板剂或者破坏沸石完整结构(牺牲活性中心,并受限于硅铝比),介孔孔道的三维贯通性也一直是一个亟待解决的问题和挑战。为此,我们开发出一种准固相转化的方法,在不添加介孔模板剂的条件下,通过调整前驱体凝胶的状态制备出介孔孔道三维贯穿于单晶沸石颗粒,并提出一种动力学控制沸石成核与生长的多级结构形成机理。并成功应用于不同Si/Al体系多级结构沸石的制备。相比于传统沸石,在模型反应中表现出更加优异的催化性能。
Herein,based on a steam-assisted crystallization(SAC) method,we first report a facile and scalable strategy for the synthesis of single-crystalline hierarchically structured ZSM-5 zeolites(HSZs) by only using small amount of micropore structure-directing agents(i.e.tetrapropylammonium hydroxide).Further,a kinetic-controlled nucleation-growth mechanism is proposed for the synthesis of single-crystalline HSZs with this novel process,and HSZs with variable Si/Al ratios(30-150) have also been successfully synthesized.Compared with the conventional microporous ZSM-5,the synthesized HSZs exhibited significantly enhanced activity and stability and prolonged lifetime in model reactions,especially when bulky molecules were involved.
Herein,based on a steam-assisted crystallization(SAC) method,we first report a facile and scalable strategy for the synthesis of single-crystalline hierarchically structured ZSM-5 zeolites(HSZs) by only using small amount of micropore structure-directing agents(i.e.tetrapropylammonium hydroxide).Further,a kinetic-controlled nucleation-growth mechanism is proposed for the synthesis of single-crystalline HSZs with this novel process,and HSZs with variable Si/Al ratios(30-150) have also been successfully synthesized.Compared with the conventional microporous ZSM-5,the synthesized HSZs exhibited significantly enhanced activity and stability and prolonged lifetime in model reactions,especially when bulky molecules were involved.
引文
[1]Ge,T.;Hua,Z.;He,X.;Lv,J.;Chen,H.;Zhang,L.;Yao,H.;Liu,Z.;Lin C.;Shi,J.Chem.-Eur.J.Received
[2]He,X.;Ge,T.;Hua,Z.;Zhou,J.;Lv,J.;Zhou,J.;Liu,Z.;Shi,J.ACS Appl.Mater.Interfaces DOI:10.1021/acsami.6b00141
[2]He,X.;Ge,T.;Hua,Z.;Zhou,J.;Lv,J.;Zhou,J.;Liu,Z.;Shi,J.ACS Appl.Mater.Interfaces DOI:10.1021/acsami.6b00141