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Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept

[Image: see text] Hybrid catalysts are attracting much attention, since they combine the versatility and efficiency of homogeneous organic catalysis with the robustness and thermal stability of solid materials, for example, mesoporous silica; in addition, they can be used in cascade reactions, for e...

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Autores principales: Miletto, Ivana, Ivaldi, Chiara, Gianotti, Enrica, Paul, Geo, Travagin, Fabio, Giovenzana, Giovanni Battista, Fraccarollo, Alberto, Marchi, Davide, Marchese, Leonardo, Cossi, Maurizio
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8489525/
https://www.ncbi.nlm.nih.gov/pubmed/34621460
http://dx.doi.org/10.1021/acs.jpcc.1c06150
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author Miletto, Ivana
Ivaldi, Chiara
Gianotti, Enrica
Paul, Geo
Travagin, Fabio
Giovenzana, Giovanni Battista
Fraccarollo, Alberto
Marchi, Davide
Marchese, Leonardo
Cossi, Maurizio
author_facet Miletto, Ivana
Ivaldi, Chiara
Gianotti, Enrica
Paul, Geo
Travagin, Fabio
Giovenzana, Giovanni Battista
Fraccarollo, Alberto
Marchi, Davide
Marchese, Leonardo
Cossi, Maurizio
author_sort Miletto, Ivana
collection PubMed
description [Image: see text] Hybrid catalysts are attracting much attention, since they combine the versatility and efficiency of homogeneous organic catalysis with the robustness and thermal stability of solid materials, for example, mesoporous silica; in addition, they can be used in cascade reactions, for exploring both organic and inorganic catalysis at the same time. Despite the importance of the organic/inorganic interface in these materials, the effect of the grafting architecture on the final conformation of the organic layer (and hence its reactivity) is still largely unexplored. Here, we investigate a series of organosiloxanes comprising a pyridine ring (the catalyst model) and different numbers of alkylsiloxane chains used to anchor it to the MCM-41 surface. The hybrid interfaces are characterized with X-ray powder diffraction, thermogravimetric analyses, Fourier-transform infrared spectroscopy, nuclear magnetic resonance techniques and are modeled theoretically through molecular dynamics (MD) simulations, to determine the relationship between the number of chains and the average position of the pyridine group; MD simulations also provide some insights about temperature and solvent effects.
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spelling pubmed-84895252021-10-05 Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept Miletto, Ivana Ivaldi, Chiara Gianotti, Enrica Paul, Geo Travagin, Fabio Giovenzana, Giovanni Battista Fraccarollo, Alberto Marchi, Davide Marchese, Leonardo Cossi, Maurizio J Phys Chem C Nanomater Interfaces [Image: see text] Hybrid catalysts are attracting much attention, since they combine the versatility and efficiency of homogeneous organic catalysis with the robustness and thermal stability of solid materials, for example, mesoporous silica; in addition, they can be used in cascade reactions, for exploring both organic and inorganic catalysis at the same time. Despite the importance of the organic/inorganic interface in these materials, the effect of the grafting architecture on the final conformation of the organic layer (and hence its reactivity) is still largely unexplored. Here, we investigate a series of organosiloxanes comprising a pyridine ring (the catalyst model) and different numbers of alkylsiloxane chains used to anchor it to the MCM-41 surface. The hybrid interfaces are characterized with X-ray powder diffraction, thermogravimetric analyses, Fourier-transform infrared spectroscopy, nuclear magnetic resonance techniques and are modeled theoretically through molecular dynamics (MD) simulations, to determine the relationship between the number of chains and the average position of the pyridine group; MD simulations also provide some insights about temperature and solvent effects. American Chemical Society 2021-09-17 2021-09-30 /pmc/articles/PMC8489525/ /pubmed/34621460 http://dx.doi.org/10.1021/acs.jpcc.1c06150 Text en © 2021 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Miletto, Ivana
Ivaldi, Chiara
Gianotti, Enrica
Paul, Geo
Travagin, Fabio
Giovenzana, Giovanni Battista
Fraccarollo, Alberto
Marchi, Davide
Marchese, Leonardo
Cossi, Maurizio
Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept
title Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept
title_full Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept
title_fullStr Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept
title_full_unstemmed Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept
title_short Predicting the Conformation of Organic Catalysts Grafted on Silica Surfaces with Different Numbers of Tethering Chains: The Silicopodality Concept
title_sort predicting the conformation of organic catalysts grafted on silica surfaces with different numbers of tethering chains: the silicopodality concept
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8489525/
https://www.ncbi.nlm.nih.gov/pubmed/34621460
http://dx.doi.org/10.1021/acs.jpcc.1c06150
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