负载纳米银有机多孔材料的制备及其催化性能研究

发布时间：2018-05-04 07:29

本文选题：有机多孔聚合物 + 银纳米粒子　；参考：《湘潭大学》2017年硕士论文

【摘要】：作为金属纳米粒子的理想载体,有机多孔聚合物(Porous Organic Polymers,POPs)骨架密度低、比表面积高、物化性质稳定、制备方法简单多样。银纳米粒子因其在催化、抗菌、相分离、表面增强拉曼散射等方面的潜在应用,已经受到广泛的关注,而具有高比表面积和多级孔道的POPs负载的银纳米粒子复合物作为非均相催化剂,更受瞩目。本文通过糖基或咔唑基单体的超交联聚合制备高比表面积(含醛基)多孔聚合物,利用银离子在聚合物表面的原位还原,得到负载纳米银的复合材料。以单糖为起始原料经过苄基化、交联反应得到三种多孔聚合物,它们具有类似的孔径分布,表现为微/介孔特征,其比表面积(SBET)达970-1220 m~2g~( 1),对CO2的吸附量达10.5 wt%-14.4 wt%。以含醛基的SugPOP-1为起始原料进行氧化还原反应原位合成银纳米粒子负载的SugPOP-1复合材料AgNPs/SugPOP-1。通过紫外吸收曲线监测AgNPs/SugPOP-1复合物对4-硝基苯酚的催化性能,结果表明AgNPs/SugPOP-1复合物在870 s时已经基本完成了催化反应,体现出具有良好的催化性能,活性因子高达51.4 s 1 g~( 1)。以3,5-二咔唑苯甲醛为单体通过氧化偶联反应得到多孔聚合物,它的BET比表面积高达580 m~2g~( 1),孔径分布图表明其具有微介孔的特征。含有醛基的DPOP-1通过氧化还原反应得到AgNPs/DPOP-1复合物,AgNPs/DPOP-1复合物对4-硝基苯酚的催化活性因子为37.8 s 1g~( 1)。设计一种含有咔唑基团的富勒烯基单体,将交联位点引入到富勒烯表面,通过氧化偶联反应得到具有比表面积为594 m~2g~( 1)的多孔聚合物FuPOP-1,它对CO2和CH4的吸附量分别为9.6 wt%、1.3 wt%。利用富勒烯上碳球的反应性,对FuPOP-1进一步后修饰得到比表面积为200 m~2g~( 1)-380 m~2g~( 1)的含钯、铑和氟的FuPOP-1取代物。
[Abstract]:As an ideal carrier of metal nanoparticles, organic porous polymer (Porous Organic Polymer) has low skeleton density, high specific surface area, stable physicochemical properties and simple and varied preparation methods. Silver nanoparticles have attracted wide attention for their potential applications in catalysis, antibacterial, phase separation, surface enhanced Raman scattering and so on. Silver nanoparticles with high specific surface area and multilevel pores supported on silver nanoparticles are more attractive as heterogeneous catalysts. In this paper, high specific surface area (Aldol) porous polymers were prepared by hypercrosslinking polymerization of glycosyl or carbazolyl monomers. The composite materials loaded with nano-silver were obtained by in-situ reduction of silver ions on the surface of the polymers. Three kinds of porous polymers were obtained by benzylation of monosaccharide and crosslinking reaction. They have similar pore size distribution and show microporous / mesoporous characteristics. The specific surface area of SBETs is 970 ~ 1220 mt-1 路g ~ (-1), and the adsorption capacity of CO2 is 10.5 wt%-14.4 / wt. Silver nanoparticles supported SugPOP-1 composites AgNPs / SugPOP-1 were synthesized in situ by redox reaction using SugPOP-1 containing aldehyde group as the starting material. The catalytic activity of AgNPs/SugPOP-1 complex for 4-nitrophenol was monitored by UV absorption curve. The results showed that the catalytic reaction of AgNPs/SugPOP-1 complex was basically completed at 870 s, which showed good catalytic activity, and the activity factor was up to 51.4 s / 1 g / g. The porous polymer was prepared by oxidative coupling reaction with 3 / 5-dicarbazolbenzaldehyde as monomer. The specific surface area of the polymer was as high as 580mm2 / 2g / g. The pore size distribution showed that the polymer had the characteristics of micromesoporous. The catalytic activity factor of DPOP-1 containing aldehyde group for 4-nitrophenol was obtained by redox reaction. The catalytic activity factor of Ag-NPs / DPOP-1 complex for 4-nitrophenol was 37.8 s ~ (-1) g ~ (-1) 路g ~ (-1) ~ (-1) 路g ~ (-1) ~ (-1) ~ (-1). A kind of fullerenyl monomer containing carbazole group was designed. The crosslinking site was introduced to the surface of fullerene, and the porous polymer FuPOP-1 with a specific surface area of 594 mm2 2gN (1) was obtained by oxidative coupling reaction. The adsorption amount of CO2 and CH4 was 9.6 wttand 1.3 wt, respectively. Based on the reactivity of carbon spheres on fullerene, FuPOP-1 was further modified to obtain FuPOP-1 substituents containing palladium, rhodium and fluorine with a specific surface area of 200mg ~ 380mg ~ 2g ~ (-1).
【学位授予单位】：湘潭大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TB383.4;O643.36

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