Kinetic analysis of the reduction of 4-nitrophenol catalyzed by Au/Pd nanoalloys immobilized in spherical polyelectrolyte brushes

Physical Chemistry Chemical Physics : PCCP
Sasa GuMatthias Ballauff

Abstract

We present a detailed study of the catalytic activity of Au/Pd nanoalloys with Au : Pd molar ratio 75 : 25 synthesized using spherical polyelectrolyte brushes (SPB) as carrier system. The reduction of 4-nitrophenol (Nip) by sodium borohydride (BH4(-)) has been used as a model reaction. This reaction proceeds in two steps: 4-nitrophenol is first reduced to 4-hydroxylaminophenol which in a second step is reduced to the final product 4-aminophenol. Both steps of the reaction proceed on the surface of the nanoparticles (Langmuir-Hinshelwood-mechanism). We use this model to analyze the experimental data obtained by catalysis with the Au/Pd-nanoalloys. Good agreements between theory and experiments were found up to 30% conversion of Nip. The kinetic parameters were compared with the data derived from neat Au and Pd nanoparticles immobilized in the same SPB carrier system. The addition of 25% molar ratio of Pd to the nanoalloys increases the reaction rate of the first step nearly 10 times compared with that of SPB-Au and 60 times compared with that of SPB-Pd. Analysis of the nanoalloy by high-resolution transmission electron microscopy suggests that the surface defects of the nanoalloys play an important role for the enhanced catalyti...Continue Reading

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Citations

May 31, 2015·Ultramicroscopy·P W Hawkes
Jul 6, 2016·Langmuir : the ACS Journal of Surfaces and Colloids·Claudia Kästner, Andreas F Thünemann
Dec 13, 2016·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Xiaoxia Guo, Kongshuang Zhao
May 18, 2017·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Xiaoxia Guo, Kongshuang Zhao
Oct 6, 2018·Inorganic Chemistry·Martin KluenkerWolfgang Tremel
Jul 21, 2017·Langmuir : the ACS Journal of Surfaces and Colloids·Yu LiangXiangke Wang

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