CTABr为介孔模板制备多级孔道ZSM-5:由介孔硅铝酸盐到多级孔道沸石分子筛
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- 英文论文题名：Synthesis of hierarchical ZSM-5 using CTABr as mesoporogen:from the ordered mesoporous silica-alumina species to hierarchical zeolite
- 论文作者：薛腾 ; 吴海虹
- 英文论文作者：Teng Xue ; Haihong Wu ; Shanghai Key Laboratory of Green Chemistry and Chemical Processes ; School of Chemistry and Molecular Engineering ; East China Normal University
- 年：2016
- 作者机构：华东师范大学化学与分子工程学院上海市绿色化学与化工过程绿色化重点实验室;
- 论文关键词：ZSM-5 ; 多级孔道 ; CTABr ; 己二胺 ; 原位转化
- 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：TQ424.25
- 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：119k
- 原文格式：D
- 会议级别：全国
摘要
多级孔道分子筛兼具微孔沸石的良好热稳定性和水热稳定性、强催化活性、优异择形选择性以及介孔分子筛的优良扩散性能,成为分子筛研究的热点~[1]。新颖的双功能模板剂的应用更是将多级孔道分子筛合成研究推向新的高峰,但高昂的成本使得该类方法难以推广;以廉价的常规阳离子表面活性剂做介孔模板制备多级孔道沸石面临的问题是介孔相和沸石相的分离。本文以CTABr做介孔模板,以导向能力相对较弱的己二胺做结构导向剂制备多级孔道ZSM-5分子筛。晶化过程中CTABr首先组装无定形硅铝物种形成介孔相、继而在己二胺作用下介孔相坍塌并原位转化形成多级孔ZSM-5纳米晶粒聚集体。己二胺做结构导向剂有利于ZSM-5分子筛纳米粒子聚集体的形成~[2],且其较弱的结构导向能力避免了与介孔模板CTABr的竞争,从而有效避免了无定形介孔相与沸石相的分离;而原位形成的介孔相包覆的CTABr抑制了ZSM-5分子筛聚集体初级纳米粒子的生长及相互融合,使分子筛聚集体粒间介孔得到更好地保留。所得ZSM-5分子筛纳米粒子聚集体高度晶化,其介孔体积高达0.32 cm~3/g、外比表面积达112.3 m~2/g,具有相对规则、分布范围窄的介孔孔径分布,在催化大分子参与的反应时表现出优异的性能。该方法廉价、简单,适用于各种硅源、铝源,具有很宽的硅铝比适用范围。
Hierarchical ZSM-5 aggregates were fabricated using CTABr as mesoporogen together with 1,6-diaminohexane as structure-directing agent.During the crystallization,mesoporous silica-alumina species formed firstly at the convenience of CTABr and then transformed in-situ to the hierarchical ZSM-5 aggregates with the assistance of 1,6-diaminohexane.1,6-Diaminohexane as the structure-directing agent facilitated the formation of the ZSM-5 aggregates while the encapsulated CTABr inhibited the further growth and fusion of primary nanoparticles,preserving the interparticle mesoporosity as large as possible.The obtained hierarchical ZSM-5aggregates were highly crystallized,with large external surface area,mesopore volume and regular mesopore size distributions.And they exhibited improved catalytic performance in the large-molecule involved reactions due to the improved accessibility of the active sites.
Hierarchical ZSM-5 aggregates were fabricated using CTABr as mesoporogen together with 1,6-diaminohexane as structure-directing agent.During the crystallization,mesoporous silica-alumina species formed firstly at the convenience of CTABr and then transformed in-situ to the hierarchical ZSM-5 aggregates with the assistance of 1,6-diaminohexane.1,6-Diaminohexane as the structure-directing agent facilitated the formation of the ZSM-5 aggregates while the encapsulated CTABr inhibited the further growth and fusion of primary nanoparticles,preserving the interparticle mesoporosity as large as possible.The obtained hierarchical ZSM-5aggregates were highly crystallized,with large external surface area,mesopore volume and regular mesopore size distributions.And they exhibited improved catalytic performance in the large-molecule involved reactions due to the improved accessibility of the active sites.
引文
[1]Zhang,K;M.L.Ostraat.Catal.Today 2016.264:3.
[2]Chen,L.;Zhu,S.;Wang,Y.*;He,M.New J.Chem.2010.34(10):2328.
[2]Chen,L.;Zhu,S.;Wang,Y.*;He,M.New J.Chem.2010.34(10):2328.