双亲性Fe_3O_4@PMO磁性复合材料的合成及其吸附催化性能
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- 英文论文题名：Magnetic amphiphilic yolk-shell nanomaterial with amino/thiol-functionalized PMO shell as efficient catalysts and adsorbents
- 论文作者：代金玉 ; 邹后兵 ; 王润伟 ; 张宗弢 ; 裘式纶
- 英文论文作者：Jinyu Dai ; Houbing Zou ; Runwei Wang ; Zongtao Zhang ; Shilun Qiu ; Department of Chemistry ; University of Jilin
- 年：2016
- 作者机构：吉林大学化学学院;
- 论文关键词：双亲性 ; 需氧催化氧化 ; 磁性复合材料
- 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：TB332
- 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：198k
- 原文格式：D
- 会议级别：全国
摘要
这项工作设计了一种具有高催化活性和稳定性的双亲性纳米吸附催化剂,同时,我们把磁性物质引入双亲性的介孔复合材料中,更好的实现快速分离、回收及重复使用的效果,并将其应用于以水为绿色溶剂的醇的需氧氧化反应。首先,我们根据以前所报道的生长诱导腐蚀法~[1],制备了一种以Fe_3O_4@SiO_2纳米粒子为磁性核~[2],以PMO为中空壳的双亲性纳米材料,在催化剂的支持物上引入可以使金属纳米粒子在配位吸附后原位还原的功能基团,进而减少合成催化剂的步骤。例如,我们设计出把氨基、巯基~[3]并入含有有机桥联基团的杂化材料中,然后将Pd2+吸附后原位还原。这样既可以形成非常小的Pd纳米粒子(平均尺寸在2~5nm之间),又可以通过与不反应的氨基、巯基配位来稳固Pd纳米粒子,既防止纳米粒子的聚集又能使纳米粒子不会从材料中浸出。所得到的材料通过扫描电镜(SEM),透射电镜(TEM),粉末X射线衍射(PXRD),红外(FT-IR),固体核磁等进行详细的表征。我们发现所得到的材料在水系醇的需氧氧化反应中表现出非常好的催化活性和稳定性。同时,我们将其应用于吸附水中有机小分子污染物,表现出较好的吸附性能。
This work describes the preparation of multifunctional yolk-shell hybrid materials which was prepared by the immobilization of amino/thiol within the channels of magnetic periodic mesoporous organosilica(PMO) materials.It was clearly demonstrated that in situ reduction of Pd~(2+) by amino/thiol to produce Pd nanoparticles and coordinate the Pd nanoparticles with amino/thiol-ligands.It was also allowed for maximal exposure to reaction substrates while minimizing Pd nanoparticles leaching.Furthermore,the unique amiphiphilic nanostructures enables oxidation of alcohols reactions to proceed efficiently in water under an air atmosphere.This catalyst is completely magnetically recoverable due to the super paramagnetic behavior of Fe_3O_4 and can be reused with sustained selectivity and activity.
This work describes the preparation of multifunctional yolk-shell hybrid materials which was prepared by the immobilization of amino/thiol within the channels of magnetic periodic mesoporous organosilica(PMO) materials.It was clearly demonstrated that in situ reduction of Pd~(2+) by amino/thiol to produce Pd nanoparticles and coordinate the Pd nanoparticles with amino/thiol-ligands.It was also allowed for maximal exposure to reaction substrates while minimizing Pd nanoparticles leaching.Furthermore,the unique amiphiphilic nanostructures enables oxidation of alcohols reactions to proceed efficiently in water under an air atmosphere.This catalyst is completely magnetically recoverable due to the super paramagnetic behavior of Fe_3O_4 and can be reused with sustained selectivity and activity.
引文
[1]Zou,H.;Wang,R.;Li,X.;Qiu,S.J.Mater.Chem.A.2014,2:12403
[2]Yue,Q.;Zhang,Y.;Zhao,D.;Deng,Y.J.Mater.Chem.A.2015,3:4586
[3]Zhu,F.;Wang,W.;Li,H.J.Am.Chem.Soc.2011,133:11632
[2]Yue,Q.;Zhang,Y.;Zhao,D.;Deng,Y.J.Mater.Chem.A.2015,3:4586
[3]Zhu,F.;Wang,W.;Li,H.J.Am.Chem.Soc.2011,133:11632