具有MFI拓补结构的中空沸石的设计合成及应用
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- 英文论文题名：Design synthesis of hollow zeolite with MFI topology
- 论文作者：郭新闻 ; 代成义 ; 张安峰 ; 刘民 ; 宋春山
- 英文论文作者：Xinwen Guo ; Chengyi Dai ; Anfeng Zhang ; Min Liu ; Chunshan Song ; State Key Lab of Fine Chemicals ; PSU-DUT Joint Center for Energy Research School of Chemical Engineering ; Dalian University of Technology ; Energy Institute ; Department of Energy & Mineral Engineering ; Penn State University
- 年：2016
- 作者机构：大连理工大学精细化工国家重点实验室大工-宾州联合能源研究中心;美国宾州州立大学能源与矿物系能源研究所;
- 论文关键词：中空沸石 ; ZSM-5 ; 碱处理 ; 表面富硅 ; 封装
- 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：225k
- 原文格式：D
- 会议级别：全国
摘要
近年来,由于纳米中空材料在微反应器、储能及药物缓释等方面的广泛应用,引起了研究者们越来越广泛的关注。其中,由于中空沸石具有良好的水热稳定性和狭窄的微孔孔径分布,使其成为封装金属、制备微反应器的优良载体。然而,沸石材料固有的刚性骨架,使得合成形貌规则的中空沸石成为挑战。通过实验结果结合理论计算,确定了中空S-1沸石的形成机理,制备了"碗状"及三维大孔沸石。以得到的中空S-1为母体,使用"瓶中造船"技术成功的将磷钨酸(HPW)封装到了空腔内部。在不影响催化剂活性的情况下,极大的抑制了HPW在反应过程中的流失。随后,将Au,Ag,Pd,Pt等贵金属以及Fe,Cu,Ni,Co等过渡金属封装到了中空沸石内部。其中封装Pd的催化剂(Pd@Hol S-1)在Suzuki偶联反应中表现出良好的底物选择性;封装Ni-Pt双金属的催化剂(Ni-Pt@Hol S-1)在甲烷二氧化碳重整反应中表现出优异的抗积碳能力。最近,成功合成了表面富硅的中空ZSM-5沸石,在联苯的烷基化反应中,同时提高了反应物的转化率和目标产物的选择性;在此基础上,合成了具有双层结构的中空ZSM-5沸石;还将多种单一金属或双金属以及碳纳米管封装到了中空ZSM-5空腔内部。
In this paper,hollow S-1 zeolite nanocubes could be easily controlled from about 150 to 600 nm by simply adjusting the size of parent silicalite-1.Use hollow S-l nanocubes as host material,HPW@Hollow S-l,a novel solid catalyst which can be reused in the synthesis of ethyl acetate,was successfully prepared by the ship-in-bottle approach.Using "impregnation-dissolution-recrystallization" method,Au,Ag,Pd,Pt,Fe,Cu,Ni metal nanoparticles have been successfully encapsulated in hollow silicalite-1 single crystals.The synthesized hollow ZSM-5 exhibits both higher shape selectivity and higher activity in biphenyl methylation with methanol than that of the solid ZSM-5.Furthermore,hollow ZSM-5 single crystals with double layer shells were successfully prepared with a layer-by-layer technique followed with dissolution-recrystallization strategy.Hollow ZSM-5 nano-sized crystals with encapsulated Fe_2O_3,carbon nanotubes(CNTs),and hollow ZSM-5 encapsulating bimetallic(oxide)nanoparticles such as CuO-Pd,and CuO-Pt as well as Fe_2O_3-Au have also been successfully synthesized.
In this paper,hollow S-1 zeolite nanocubes could be easily controlled from about 150 to 600 nm by simply adjusting the size of parent silicalite-1.Use hollow S-l nanocubes as host material,HPW@Hollow S-l,a novel solid catalyst which can be reused in the synthesis of ethyl acetate,was successfully prepared by the ship-in-bottle approach.Using "impregnation-dissolution-recrystallization" method,Au,Ag,Pd,Pt,Fe,Cu,Ni metal nanoparticles have been successfully encapsulated in hollow silicalite-1 single crystals.The synthesized hollow ZSM-5 exhibits both higher shape selectivity and higher activity in biphenyl methylation with methanol than that of the solid ZSM-5.Furthermore,hollow ZSM-5 single crystals with double layer shells were successfully prepared with a layer-by-layer technique followed with dissolution-recrystallization strategy.Hollow ZSM-5 nano-sized crystals with encapsulated Fe_2O_3,carbon nanotubes(CNTs),and hollow ZSM-5 encapsulating bimetallic(oxide)nanoparticles such as CuO-Pd,and CuO-Pt as well as Fe_2O_3-Au have also been successfully synthesized.
引文
1.Dai C.,Zhang A.;Liu M.,Guo X.;Song C.Adv.Funct.Mater.,DOI:10.1002/adfm.201502980.
2 .Dai C.;Zhang A.;Li L.;Hou K.;Ding F.;Li J.;Mu D.;Song C.;Liu M.;Guo X.Chem.Mater.2013,25:4197.
2 .Dai C.;Zhang A.;Li L.;Hou K.;Ding F.;Li J.;Mu D.;Song C.;Liu M.;Guo X.Chem.Mater.2013,25:4197.