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An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation

The different activity of a 1% Pd/carbon catalyst towards aromatic and aliphatic aldehydes hydrogenation has been explored by (13)C NMR relaxation. The ratio between T1 relaxation times of adsorbed (ads) and free diffusing (bulk) molecules (T1(ads)/T1(bulk)) can be used as an indicator of the relati...

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Autores principales: Stucchi, Marta, Vasile, Francesca, Cattaneo, Stefano, Villa, Alberto, Chieregato, Alessandro, Vandegehuchte, Bart D., Prati, Laura
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8955477/
https://www.ncbi.nlm.nih.gov/pubmed/35335722
http://dx.doi.org/10.3390/nano12060908
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author Stucchi, Marta
Vasile, Francesca
Cattaneo, Stefano
Villa, Alberto
Chieregato, Alessandro
Vandegehuchte, Bart D.
Prati, Laura
author_facet Stucchi, Marta
Vasile, Francesca
Cattaneo, Stefano
Villa, Alberto
Chieregato, Alessandro
Vandegehuchte, Bart D.
Prati, Laura
author_sort Stucchi, Marta
collection PubMed
description The different activity of a 1% Pd/carbon catalyst towards aromatic and aliphatic aldehydes hydrogenation has been explored by (13)C NMR relaxation. The ratio between T1 relaxation times of adsorbed (ads) and free diffusing (bulk) molecules (T1(ads)/T1(bulk)) can be used as an indicator of the relative strength of interaction between the reactant and the catalytic surface, where the lower the T1(ads)/T1(bulk), the higher the adsorption strength. It can be seen that 1% Pd/carbon showed a reverse catalytic behaviour towards benzaldehyde and octanal hydrogenation, which can be explained by analysing the T1 relaxation times related to each substrate in the presence of the catalyst. Comparing and correlating the different T1(ads)/T1(bulk) values, we were able to prove that the different catalytic results mainly depend on the contrasting adsorption behaviour of substrates on the catalyst. Moreover, the role of the solvent has been disclosed, as NMR results revealed that the adsorption of the reactants was strongly affected by the choice of solvent, which is revealed to be critical in modulating catalytic activity. As a consequence, T1(ads)/T1(bulk) measurements can provide a guide to the selection of appropriate reaction conditions for improving catalytic activity.
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spelling pubmed-89554772022-03-26 An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation Stucchi, Marta Vasile, Francesca Cattaneo, Stefano Villa, Alberto Chieregato, Alessandro Vandegehuchte, Bart D. Prati, Laura Nanomaterials (Basel) Article The different activity of a 1% Pd/carbon catalyst towards aromatic and aliphatic aldehydes hydrogenation has been explored by (13)C NMR relaxation. The ratio between T1 relaxation times of adsorbed (ads) and free diffusing (bulk) molecules (T1(ads)/T1(bulk)) can be used as an indicator of the relative strength of interaction between the reactant and the catalytic surface, where the lower the T1(ads)/T1(bulk), the higher the adsorption strength. It can be seen that 1% Pd/carbon showed a reverse catalytic behaviour towards benzaldehyde and octanal hydrogenation, which can be explained by analysing the T1 relaxation times related to each substrate in the presence of the catalyst. Comparing and correlating the different T1(ads)/T1(bulk) values, we were able to prove that the different catalytic results mainly depend on the contrasting adsorption behaviour of substrates on the catalyst. Moreover, the role of the solvent has been disclosed, as NMR results revealed that the adsorption of the reactants was strongly affected by the choice of solvent, which is revealed to be critical in modulating catalytic activity. As a consequence, T1(ads)/T1(bulk) measurements can provide a guide to the selection of appropriate reaction conditions for improving catalytic activity. MDPI 2022-03-09 /pmc/articles/PMC8955477/ /pubmed/35335722 http://dx.doi.org/10.3390/nano12060908 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Stucchi, Marta
Vasile, Francesca
Cattaneo, Stefano
Villa, Alberto
Chieregato, Alessandro
Vandegehuchte, Bart D.
Prati, Laura
An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation
title An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation
title_full An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation
title_fullStr An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation
title_full_unstemmed An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation
title_short An Insight into the Role of Reactant Structure Effect in Pd/C Catalysed Aldehyde Hydrogenation
title_sort insight into the role of reactant structure effect in pd/c catalysed aldehyde hydrogenation
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8955477/
https://www.ncbi.nlm.nih.gov/pubmed/35335722
http://dx.doi.org/10.3390/nano12060908
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