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Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural

[Image: see text] Oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid is an important transformation for the production of bio-based polymers. Carbon-supported gold catalysts hold great promise for this transformation. Here we demonstrate that the activity, selectivity, and stabilit...

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Autores principales: Donoeva, Baira, Masoud, Nazila, de Jongh, Petra E.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2017
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5627991/
https://www.ncbi.nlm.nih.gov/pubmed/28989810
http://dx.doi.org/10.1021/acscatal.7b00829
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author Donoeva, Baira
Masoud, Nazila
de Jongh, Petra E.
author_facet Donoeva, Baira
Masoud, Nazila
de Jongh, Petra E.
author_sort Donoeva, Baira
collection PubMed
description [Image: see text] Oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid is an important transformation for the production of bio-based polymers. Carbon-supported gold catalysts hold great promise for this transformation. Here we demonstrate that the activity, selectivity, and stability of the carbon-supported gold nanoparticles in the oxidation of 5-hydroxymethylfurfural strongly depend on the surface properties of the carbon support. Gold nanoparticles supported on basic carbon materials with a low density of functional groups demonstrate higher activity in 5-hydroxymethylfurfural oxidation (TOF(Au) up to 1195 h(–1)), higher selectivity to 2,5-furandicarboxylic acid, and better stability in comparison to gold nanoparticles supported on carbon materials with acidic surface groups. Surface groups of basic carbon supports that are positively charged under the reaction conditions result in a higher adsorption and local concentration of hydroxyl ions, which act as cocatalysts for gold and enhance gold-catalyzed dehydrogenation. Negatively charged surface groups of acidic carbons repel hydroxyls and the intermediate monoacid anions, which leads to lower reaction rates and a high selectivity toward 2,5-hydroxymethylfurancarboxylic acid. Understanding the role of support surface charge and local hydroxyl anion concentration provides a basis for the rational design of the optimal carbon support surface chemistry for highly active, selective, and stable catalysts for the oxidation of 5-hydroxymethylfurfural and related reactions.
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spelling pubmed-56279912017-10-06 Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural Donoeva, Baira Masoud, Nazila de Jongh, Petra E. ACS Catal [Image: see text] Oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid is an important transformation for the production of bio-based polymers. Carbon-supported gold catalysts hold great promise for this transformation. Here we demonstrate that the activity, selectivity, and stability of the carbon-supported gold nanoparticles in the oxidation of 5-hydroxymethylfurfural strongly depend on the surface properties of the carbon support. Gold nanoparticles supported on basic carbon materials with a low density of functional groups demonstrate higher activity in 5-hydroxymethylfurfural oxidation (TOF(Au) up to 1195 h(–1)), higher selectivity to 2,5-furandicarboxylic acid, and better stability in comparison to gold nanoparticles supported on carbon materials with acidic surface groups. Surface groups of basic carbon supports that are positively charged under the reaction conditions result in a higher adsorption and local concentration of hydroxyl ions, which act as cocatalysts for gold and enhance gold-catalyzed dehydrogenation. Negatively charged surface groups of acidic carbons repel hydroxyls and the intermediate monoacid anions, which leads to lower reaction rates and a high selectivity toward 2,5-hydroxymethylfurancarboxylic acid. Understanding the role of support surface charge and local hydroxyl anion concentration provides a basis for the rational design of the optimal carbon support surface chemistry for highly active, selective, and stable catalysts for the oxidation of 5-hydroxymethylfurfural and related reactions. American Chemical Society 2017-05-31 2017-07-07 /pmc/articles/PMC5627991/ /pubmed/28989810 http://dx.doi.org/10.1021/acscatal.7b00829 Text en Copyright © 2017 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Donoeva, Baira
Masoud, Nazila
de Jongh, Petra E.
Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural
title Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural
title_full Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural
title_fullStr Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural
title_full_unstemmed Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural
title_short Carbon Support Surface Effects in the Gold-Catalyzed Oxidation of 5-Hydroxymethylfurfural
title_sort carbon support surface effects in the gold-catalyzed oxidation of 5-hydroxymethylfurfural
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5627991/
https://www.ncbi.nlm.nih.gov/pubmed/28989810
http://dx.doi.org/10.1021/acscatal.7b00829
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