Mei Yu, Sharma Geeta, Lu Yan, Ballauff Matthias, Drechsler Markus, Irrgang Thorsten, Kempe Rhett
Physikalische Chemie I, University of Bayreuth, 95440 Bayreuth, Germany.
Langmuir. 2005 Dec 20;21(26):12229-34. doi: 10.1021/la052120w.
We present a study on the catalytic activity of platinum nanoparticles immobilized on spherical polyelectrolyte brushes that act as carriers. The spherical polyelectrolyte brushes consist of a solid core of poly(styrene) onto which long chains of poly(2-methylpropenoyloxyethyl) trimethylammonium chloride are grafted. These positively charged chains form a dense layer of polyelectrolytes on the surface of the core particles ("spherical polyelectrolyte brush") that tightly binds divalent PtCl6-(2) ions. The reduction of these ions within the brush layer leads to nearly monodisperse nanoparticles of metallic platinum. The average size of the particles is approximately 2 nm. The composite particles exhibit excellent colloidal stability. The catalytic activity is investigated by photometrically monitoring the reduction of p-nitrophenol by an excess of NaBH4 in the presence of the nanoparticles. The kinetic data could be explained by the assumption of a pseudo-first-order reaction with regard to p-nitrophenol. In all cases, a delay time t0 has been observed, after which the reactions start. This time is shorter when the catalyst has already been used. All data demonstrate that spherical polyelectrolyte brushes present an ideal carrier system for metallic nanoparticles.
我们展示了一项关于固定在作为载体的球形聚电解质刷上的铂纳米颗粒催化活性的研究。球形聚电解质刷由聚苯乙烯固体核组成,在其上面接枝了聚(2 - 甲基丙烯酰氧基乙基)三甲基氯化铵的长链。这些带正电荷的链在核颗粒表面形成一层致密的聚电解质层(“球形聚电解质刷”),该层紧密结合二价的PtCl6-(2)离子。在刷层内这些离子的还原导致形成近乎单分散的金属铂纳米颗粒。颗粒的平均尺寸约为2纳米。复合颗粒表现出优异的胶体稳定性。通过在纳米颗粒存在下用过量的NaBH4光度监测对硝基苯酚的还原反应来研究催化活性。动力学数据可以通过假设对硝基苯酚的准一级反应来解释。在所有情况下,都观察到了一个延迟时间t0,在此之后反应开始。当催化剂已经被使用时,这个时间更短。所有数据表明球形聚电解质刷是金属纳米颗粒的理想载体系统。