“动态模板”法可控构筑多级孔硅氢化合物材料及其作为贵金属催化剂载体的应用研究

批准号:
21501056
项目类别:
青年科学基金项目
资助金额:
20.0 万元
负责人:
李娜
依托单位:
学科分类:
B0502.无机功能材料化学
结题年份:
2018
批准年份:
2015
项目状态:
已结题
项目参与者:
许建雄、杜晶晶、朱清云、张创、刘玮玮
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中文摘要
本项目旨在建立一种多级孔HSQ材料可控构筑的新方法,并研究多级孔HSQ材料作为贵金属催化剂载体的应用。为此,拟采用“动态模板”方法,即以聚环氧乙烷-b-聚4-乙烯苯基-N,N’-二乙基胺盐酸盐嵌段共聚物为阳离子聚电解质,N-十二烷基肌氨酸钠为阴离子表面活性剂,利用m-PEO-b-PVEAH与Sar-Na形成的介晶复合物为模板,制备多级孔HSQ材料。通过系统研究,阐明多级孔HSQ材料的合成机制,探索出一条多级孔HSQ材料可控构筑的新方法。以多级孔HSQ材料为载体和还原剂,研究贵金属纳米催化剂在其孔道内部的固载情况,开发一种简单高效的负载型贵金属纳米催化剂的制备体系。以水相中硝基苯的催化氢化为模型反应,考察负载型贵金属催化剂的催化性能,揭示多级孔HSQ材料在贵金属纳米催化剂负载中载体材料与催化性能之间的构效关系,拓展HSQ材料在催化领域中的应用。
英文摘要
This project aims at the synthesis of hierarchically porous hydridosilsesquioxane (HSQ) materials and their application as scaffold of noble metal nanoparticles. To accomplish our goal, hierarchically porous HSQ materials are firstly synthesized through “dynamic template” of organic mesomorphous complexes formed by polyelectrolyte (poly(ethylene oxide)-b-poly[N-(4-vinylbenzyl)-N,N’-diethylamine hydrochloride] (m-PEO-b-PVEAH)) and cationic surfactant (N-lauroylsarcosine sodium (Sar-Na)). The key of the design involves: 1) the hydrogen bonding between the ether oxygens of m-PEO chain and trialkoxysilane benefits to the stability of the HSQ during the hydrolysis process; 2) the hydrolysis of the trialkoxysilane precursors in acid condition generates positively charged silica oligomers, the inorganic species will disturb the electrostatic interactions between PVEAH chains and the anion surfactants which makes the phase separation of PVEAH chains and therefore forms a dynamic template. In our strategy, the m-PEO chain and the anion surfactants act as the mesoporous template while the phase separated PVEAH domains act as the secondary nanoporous template. The morphologys and meso-structures of the synthesized hierarchically porous HSQ materials originate from the mesomorphous complex of m-PEO-b-PVEAH/Sar-Na. By adjusting the molecular weight, chain length of the polyelectrolyte, the molar ratio of polyelectrolyte and surfactant, and reaction factors such as synthesis temperature, pH value, hierarchically porous HSQ materials with well-defined morphologys and meso-structures and controllable pore size will be prepared and the synthetic mechanism will be revealed.. Ascribe to the inherent Si-H group and the hierarchically porous structure, the synthesized HSQ materials are used as both the scaffolds and mild reducing agent for the immobilization of noble metal nanoparticles. The advantages of the hierarchically porous HSQ materials lie in: first, without using of other reducing agent simplifies the catalyst preparation process; second, the ordered mesopores in HSQ materials can effectively trap and capture the noble metal nanoparticles avoiding the loss of catalyst during the catalytic process; third, the large pores in HSQ materials can act as the warehouse of the reactant which benefit to the concentration of the reactant and therefore enhance the catalytic property. The structure-activity relationship of the morphology, meso-structure and pore size of HSQ materials with the immobilization efficiency and catalytic property of the noble metal nanoparticles will be explored by choosing the catalytic hydrogenation of nitrobenzene in water as a typical example.. This project is anticipated to develop a new strategy for the synthesis of hierarchically porous HSQ materials and offer a potential theoretical guidance for the application HSQ materials in catalysis.
以带相反电荷聚电解质-表面活性剂形成的复合物介晶为模板,“动态模板”方法可控合成多级孔二氧化硅材料。系统研究反应条件如电解质、表面活性剂、硅源种类以及比例对产物形貌及孔结构的影响,系统总结了影响规律,揭示了多级孔二氧化硅合成机制;以合成的多级孔二氧化硅材料为载体,研究其固载贵金属催化剂(Pd、Ti、Ni-Co合金等)以及生物催化剂(生物酶)的能力,并评价相关催化剂的催化性能。研究表明:1)该方法具有较好的普适性,多种聚电解质与表面活性剂复配体系可成功制备多级孔二氧化硅材料,而且该方法可以拓展至多级孔碳微球的合成;2)硅源种类对多级孔二氧化硅材料的形貌影响显著,通过引入带正电荷的氨基硅源,打破体系的电荷平衡及各物种的组装,成功制备出空心结构多级孔二氧化硅材料;3)基于多级孔道结构有利于物质在材料内部的传输,该材料显示出优异的负载性能,而且制备的异相催化剂显示出良好的催化活性。
期刊论文列表
专著列表
科研奖励列表
会议论文列表
专利列表
Preparation of Hierarchical Nanoporous Al-SiO2/Ni-Mo Composite Electrodes and Their Electrocatalytic Hydrogen Evolution
多级纳米孔Al-SiO2/Ni-Mo复合电极的制备及其电催化析氢
DOI:10.1166/jnn.2016.12991
发表时间:2016
期刊:Journal of Nanoscience and Nanotechnology
影响因子:--
作者:Du Jingjing;Xie Shaowen;Li Na;Xu Jianxiong;Xu Lijian
通讯作者:Xu Lijian
Hydrothermal synthesis and inkjet printing of hexagonal-phase NaYF4: Ln3+ upconversion hollow microtubes for smart anti-counterfeiting encryption
用于智能防伪加密的六方相NaYF4:Ln3上转换空心微管的水热合成及喷墨打印
DOI:10.1039/c8qm00278a
发表时间:2018-11-01
期刊:MATERIALS CHEMISTRY FRONTIERS
影响因子:7
作者:Xie, Shaowen;Tong, Chao;Zhang, Changfan
通讯作者:Zhang, Changfan
Facile Synthesis of Hollow Mesoporous Silica Microspheres via Surface Sol-Gel Process on Functional Polymeric Microsphere Template
在功能聚合物微球模板上通过表面溶胶-凝胶法轻松合成中空介孔二氧化硅微球
DOI:10.1166/jnn.2016.12946
发表时间:2016
期刊:Journal of Nanoscience and Nanotechnology
影响因子:--
作者:Liu Weiwei;Zhang Yaoyao;Xu Jianxiong;Xu Lijian;Du Jingjing;Li Na
通讯作者:Li Na
Fabrication and Electrocatalytic Activity of Hierarchically Nanoporous Pd–HSiO1.5/Ni–Co Composite Electrode for Hydrogen Evolution
多级纳米孔Pd-HSiO1.5/Ni-Co复合电极的制备及其析氢电催化活性
DOI:10.1166/nnl.2017.2408
发表时间:2017-06
期刊:Nanoscience and Nanotechnology Letters
影响因子:--
作者:Na Li;Yahui Feng;Jingjing Du;Changyun Li;Shaowen Xie;Jianxiong Xu
通讯作者:Jianxiong Xu
Hydrothermal Synthesis of PAA-Coated NaYF4:Yb3+, Er3+ Nanophosphors with Predicted Morphology, Phase and Enhanced Upconversion Luminescence Properties
水热合成 PAA 涂覆的 NaYF4:Yb3、Er3 纳米磷光体,具有预测的形貌、相位和增强的上转换发光特性
DOI:10.1166/jnn.2018.16384
发表时间:2018
期刊:Journal of Nanoscience and Nanotechnology
影响因子:--
作者:Tong Chao;Xie Shaowen;Zhou Hu;Li Na;Gong Liang;Jian Jian;Zhang Changfan;Xu Lijian;Xu Jianxiong
通讯作者:Xu Jianxiong
天然辉锑矿的资源化利用及高效储能机制研究
- 批准号:--
- 项目类别:面上项目
- 资助金额:58万元
- 批准年份:2021
- 负责人:李娜
- 依托单位:
基于多级孔碳/氢氧化镍复合电极材料构建混合型超级电容器及其储能机理研究
- 批准号:2021JJ30212
- 项目类别:省市级项目
- 资助金额:0.0万元
- 批准年份:2021
- 负责人:李娜
- 依托单位:
多级孔道结构meso-HSiO1.5纳米颗粒的可控构筑及在催化领域中的应用研究
- 批准号:2018JJ3115
- 项目类别:省市级项目
- 资助金额:0.0万元
- 批准年份:2018
- 负责人:李娜
- 依托单位:
国内基金
海外基金
