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3D-macroporous chitosan-based scaffolds with in situ formed Pd and Pt nanoparticles for nitrophenol reduction

3D-macroporous chitosan-based scaffolds with in situ formed Pd and Pt nanoparticles for nitrophenol reduction
3D-macroporous chitosan-based scaffolds with in situ formed Pd and Pt nanoparticles for nitrophenol reduction
3D-macroporous chitosan-based scaffolds (cryogels) were produced via growth of metal-polymer coordinated complexes and electrostatic interactions between oppositely charged groups of chitosan and metal ions under subzero temperatures. A mechanism of reduction of noble metal complexes inside the cryogel walls by glutaraldehyde is proposed, which produces discrete and dispersed noble metal nanoparticles. 3D-macroporous scaffolds prepared under different conditions were characterised using TGA, FTIR, nitrogen adsorption, SEM, EDX and TEM, and the distribution of platinum nanoparticles (PtNPs) and palladium nanoparticles (PdNPs) in the material assessed. The catalytic activity of the in situ synthesised PdNPs, at 2.6, 12.5 and 21.0 μg total mass, respectively, was studied utilising a model system of 4-nitrophenol reduction. The kinetics of the reaction under different conditions (temperature, concentration of catalyst) were examined, and a decrease of catalytic activity was not observed over 17 treatment cycles. Increasing the temperature of the catalytic reaction from 10 to 22 and 35 °C by PdNPs supported within the cryogel increased the kinetic rate by 44 and 126%, respectively. Turnover number and turnover frequency of the PdNPs catalysts at room temperature were in the range 0.20–0.53 h−1. The conversion degree of 4-nitrophenol at room temperature reached 98.9% (21.0 μg PdNPs). Significantly less mass of palladium nanoparticles (by 30–40 times) was needed compared to published data to obtain comparable rates of reduction of 4-nitrophenol.
0144-8617
166-175
Berillo, Dmitriy
74baad33-3b75-47bb-8713-f0b321a759d1
Cundy, Andrew
994fdc96-2dce-40f4-b74b-dc638286eb08
Berillo, Dmitriy
74baad33-3b75-47bb-8713-f0b321a759d1
Cundy, Andrew
994fdc96-2dce-40f4-b74b-dc638286eb08

Berillo, Dmitriy and Cundy, Andrew (2018) 3D-macroporous chitosan-based scaffolds with in situ formed Pd and Pt nanoparticles for nitrophenol reduction. Carbohydrate Polymers, 192, 166-175. (doi:10.1016/j.carbpol.2018.03.038).

Record type: Article

Abstract

3D-macroporous chitosan-based scaffolds (cryogels) were produced via growth of metal-polymer coordinated complexes and electrostatic interactions between oppositely charged groups of chitosan and metal ions under subzero temperatures. A mechanism of reduction of noble metal complexes inside the cryogel walls by glutaraldehyde is proposed, which produces discrete and dispersed noble metal nanoparticles. 3D-macroporous scaffolds prepared under different conditions were characterised using TGA, FTIR, nitrogen adsorption, SEM, EDX and TEM, and the distribution of platinum nanoparticles (PtNPs) and palladium nanoparticles (PdNPs) in the material assessed. The catalytic activity of the in situ synthesised PdNPs, at 2.6, 12.5 and 21.0 μg total mass, respectively, was studied utilising a model system of 4-nitrophenol reduction. The kinetics of the reaction under different conditions (temperature, concentration of catalyst) were examined, and a decrease of catalytic activity was not observed over 17 treatment cycles. Increasing the temperature of the catalytic reaction from 10 to 22 and 35 °C by PdNPs supported within the cryogel increased the kinetic rate by 44 and 126%, respectively. Turnover number and turnover frequency of the PdNPs catalysts at room temperature were in the range 0.20–0.53 h−1. The conversion degree of 4-nitrophenol at room temperature reached 98.9% (21.0 μg PdNPs). Significantly less mass of palladium nanoparticles (by 30–40 times) was needed compared to published data to obtain comparable rates of reduction of 4-nitrophenol.

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Accepted/In Press date: 14 March 2018
e-pub ahead of print date: 18 March 2018
Published date: 1 July 2018

Identifiers

Local EPrints ID: 419129
URI: http://eprints.soton.ac.uk/id/eprint/419129
ISSN: 0144-8617
PURE UUID: bd47264b-2652-4007-9b0e-c58c7ba767a5
ORCID for Andrew Cundy: ORCID iD orcid.org/0000-0003-4368-2569

Catalogue record

Date deposited: 06 Apr 2018 16:30
Last modified: 17 Dec 2019 05:30

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Contributors

Author: Dmitriy Berillo
Author: Andrew Cundy ORCID iD

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