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首页> 外文期刊>Mikrochimica Acta: An International Journal for Physical and Chemical Methods of Analysis >Fabrication and characterisation of gold nano-particle modified polymer monoliths for flow-through catalytic reactions and their application in the reduction of hexacyanoferrate
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Fabrication and characterisation of gold nano-particle modified polymer monoliths for flow-through catalytic reactions and their application in the reduction of hexacyanoferrate

机译:流通式催化反应的金纳米粒子改性聚合物整料的制备,表征及其在还原铁氰化物中的应用

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摘要

Polymer monoliths in capillary (100 μm i.d.) and polypropylene pipette tip formats (vol: 20 μL) were modified with gold nano-particles (AuNP) and subsequently used for flow-through catalytic reactions. Specifically, methacrylate monoliths were modified with amine-reactive monomers using a two-step photografting method and then reacted with ethylenediamine to provide amine attachment sites for the subsequent immobilisation of 4 nm, 7 nm or 16 rnn AuNP. This was achieved by flushing colloidal suspensions of gold nano-particles through each aminated polymer monolith which resulted in a multi-point covalent attachment of gold via the lone pair of electrons on the nitrogen of the free amine groups. Field emission scanning electron microscopy and scanning capacitively coupled conductivity detection was used to characterise the surface coverage of AuNP on the monoliths. The catalytic activity of AuNP immobilised on the polymer monoliths in both formats was then demonstrated using the reduction of Fe(III) to Fe(II) by sodium borohydride as a model reaction by monitoring the reduction in absorbance of the hexacyanoferrate (III) complex at 420 nm. Catalytic activity was significantly enhanced on monoliths modified with smaller AuNP with almost complete reduction (95 %) observed when using monoliths agglomerated with 7 nm AuNPs.
机译:用金纳米颗粒(AuNP)改性毛细管(内径100μm)和聚丙烯移液器吸头形式(体积:20μL)的聚合物整体,然后用于流通式催化反应。具体地,使用两步光接枝方法用胺反应性单体修饰甲基丙烯酸酯整料,然后与乙二胺反应以提供胺附着位点,用于随后固定4 nm,7 nm或16 nm AuNP。这是通过将金纳米颗粒的胶态悬浮液冲洗通过每个胺化的聚合物整体而实现的,这导致金通过游离胺基团的氮上的孤对电子对金进行多点共价连接。使用场发射扫描电子显微镜和扫描电容耦合电导率检测来表征AuNP在整料上的表面覆盖率。然后使用硼氢化钠将Fe(III)还原为Fe(II)作为模型反应,通过监测六氰合铁酸盐(III)配合物在吸光度下的降低,证明了固定在两种形式的聚合物整料上的AuNP的催化活性。 420纳米在使用较小的AuNP改性的整体结构上,使用7 nm AuNP团聚的整体结构时,催化活性显着提高,几乎可以完全还原(95%)。

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