Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction Comparison

In this study, the temperature-dependent activity of Au/AC nanocatalysts in redox catalytic reactions was investigated. To this end, a series of colloidal gold catalysts supported on activated carbon and titania were prepared by the sol immobilization method employing polyvinyl alcohol as a polymeri...

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Main Authors: Stefano Scurti, Alessandro Allegri, Francesca Liuzzi, Elena Rodríguez-Aguado, Juan Antonio Cecilia, Stefania Albonetti, Daniele Caretti, Nikolaos Dimitratos
Format: Article
Language:English
Published: MDPI AG 2022-03-01
Series:Catalysts
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Online Access:https://www.mdpi.com/2073-4344/12/3/323
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author Stefano Scurti
Alessandro Allegri
Francesca Liuzzi
Elena Rodríguez-Aguado
Juan Antonio Cecilia
Stefania Albonetti
Daniele Caretti
Nikolaos Dimitratos
author_facet Stefano Scurti
Alessandro Allegri
Francesca Liuzzi
Elena Rodríguez-Aguado
Juan Antonio Cecilia
Stefania Albonetti
Daniele Caretti
Nikolaos Dimitratos
author_sort Stefano Scurti
collection DOAJ
description In this study, the temperature-dependent activity of Au/AC nanocatalysts in redox catalytic reactions was investigated. To this end, a series of colloidal gold catalysts supported on activated carbon and titania were prepared by the sol immobilization method employing polyvinyl alcohol as a polymeric stabilizer at different hydrolysis degrees. The as-synthesized materials were widely characterized by spectroscopic analysis (XPS, XRD, and ATR-IR) as well as TEM microscopy and DLS/ELS measurements. Furthermore, 5-hydroxymethylfurfural (HMF) oxidation and 4-nitrophenol (4-NP) reduction were chosen to investigate the catalytic activity as a model reaction for biomass valorization and wastewater remediation. In particular, by fitting the hydrolysis degree with the kinetic data, volcano plots were obtained for both reactions, in which the maximum of the curves was represented relative to hydrolysis intermediate values. However, a comparison of the catalytic performance of the sample Au/AC_PVA-99 (hydrolysis degree of the polymer is 99%) in the two reactions showed a different catalytic behavior, probably due to the detachment of polymer derived from the different reaction temperature chosen between the two reactions. For this reason, several tests were carried out to investigate deeper the observed catalytic trend, focusing on studying the effect of the reaction temperature as well as the effect of support (metal–support interaction) by immobilizing Au colloidal nanoparticles on commercial titania. The kinetic data, combined with the characterization carried out on the catalysts, confirmed that changing the reaction conditions, the PVA behavior on the surface of the catalysts, and, therefore, the reaction outcome, is modified.
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spelling doaj.art-7035ac2e79c548b191057c5b3e4564ab2023-11-24T00:42:54ZengMDPI AGCatalysts2073-43442022-03-0112332310.3390/catal12030323Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction ComparisonStefano Scurti0Alessandro Allegri1Francesca Liuzzi2Elena Rodríguez-Aguado3Juan Antonio Cecilia4Stefania Albonetti5Daniele Caretti6Nikolaos Dimitratos7Industrial Chemistry “Toso Montanari” Department, University of Bologna, Viale Risorgimento 4, 40136 Bologna, ItalyIndustrial Chemistry “Toso Montanari” Department, University of Bologna, Viale Risorgimento 4, 40136 Bologna, ItalyIndustrial Chemistry “Toso Montanari” Department, University of Bologna, Viale Risorgimento 4, 40136 Bologna, ItalyDepartamento de Química Inorgánica, Cristalografía y Mineralogía (Unidad Asociada al ICP-CSIC), Facultad de Ciencias, Campus de Teatinos, Universidad de Málaga, 29071 Málaga, SpainDepartamento de Química Inorgánica, Cristalografía y Mineralogía (Unidad Asociada al ICP-CSIC), Facultad de Ciencias, Campus de Teatinos, Universidad de Málaga, 29071 Málaga, SpainIndustrial Chemistry “Toso Montanari” Department, University of Bologna, Viale Risorgimento 4, 40136 Bologna, ItalyIndustrial Chemistry “Toso Montanari” Department, University of Bologna, Viale Risorgimento 4, 40136 Bologna, ItalyIndustrial Chemistry “Toso Montanari” Department, University of Bologna, Viale Risorgimento 4, 40136 Bologna, ItalyIn this study, the temperature-dependent activity of Au/AC nanocatalysts in redox catalytic reactions was investigated. To this end, a series of colloidal gold catalysts supported on activated carbon and titania were prepared by the sol immobilization method employing polyvinyl alcohol as a polymeric stabilizer at different hydrolysis degrees. The as-synthesized materials were widely characterized by spectroscopic analysis (XPS, XRD, and ATR-IR) as well as TEM microscopy and DLS/ELS measurements. Furthermore, 5-hydroxymethylfurfural (HMF) oxidation and 4-nitrophenol (4-NP) reduction were chosen to investigate the catalytic activity as a model reaction for biomass valorization and wastewater remediation. In particular, by fitting the hydrolysis degree with the kinetic data, volcano plots were obtained for both reactions, in which the maximum of the curves was represented relative to hydrolysis intermediate values. However, a comparison of the catalytic performance of the sample Au/AC_PVA-99 (hydrolysis degree of the polymer is 99%) in the two reactions showed a different catalytic behavior, probably due to the detachment of polymer derived from the different reaction temperature chosen between the two reactions. For this reason, several tests were carried out to investigate deeper the observed catalytic trend, focusing on studying the effect of the reaction temperature as well as the effect of support (metal–support interaction) by immobilizing Au colloidal nanoparticles on commercial titania. The kinetic data, combined with the characterization carried out on the catalysts, confirmed that changing the reaction conditions, the PVA behavior on the surface of the catalysts, and, therefore, the reaction outcome, is modified.https://www.mdpi.com/2073-4344/12/3/323gold colloidal nanoparticleshydrogenation of 4-nitrophenolHMF oxidationPVA hydrolysis degree
spellingShingle Stefano Scurti
Alessandro Allegri
Francesca Liuzzi
Elena Rodríguez-Aguado
Juan Antonio Cecilia
Stefania Albonetti
Daniele Caretti
Nikolaos Dimitratos
Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction Comparison
Catalysts
gold colloidal nanoparticles
hydrogenation of 4-nitrophenol
HMF oxidation
PVA hydrolysis degree
title Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction Comparison
title_full Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction Comparison
title_fullStr Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction Comparison
title_full_unstemmed Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction Comparison
title_short Temperature-Dependent Activity of Gold Nanocatalysts Supported on Activated Carbon in Redox Catalytic Reactions: 5-Hydroxymethylfurfural Oxidation and 4-Nitrophenol Reduction Comparison
title_sort temperature dependent activity of gold nanocatalysts supported on activated carbon in redox catalytic reactions 5 hydroxymethylfurfural oxidation and 4 nitrophenol reduction comparison
topic gold colloidal nanoparticles
hydrogenation of 4-nitrophenol
HMF oxidation
PVA hydrolysis degree
url https://www.mdpi.com/2073-4344/12/3/323
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