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Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis

The manipulation of carbon nitride (CN) structures is one main avenue to enhance the activity of CN‐based photocatalysts. Increasing the efficiency of photocatalytic heterogeneous materials is a critical step toward the realistic implementation of sustainable schemes for organic synthesis. However,...

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Autores principales: Marchi, Miriam, Raciti, Edoardo, Gali, Sai Manoj, Piccirilli, Federica, Vondracek, Hendrik, Actis, Arianna, Salvadori, Enrico, Rosso, Cristian, Criado, Alejandro, D'Agostino, Carmine, Forster, Luke, Lee, Daniel, Foucher, Alexandre C., Rai, Rajeev Kumar, Beljonne, David, Stach, Eric A., Chiesa, Mario, Lazzaroni, Roberto, Filippini, Giacomo, Prato, Maurizio, Melchionna, Michele, Fornasiero, Paolo
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10502671/
https://www.ncbi.nlm.nih.gov/pubmed/37409444
http://dx.doi.org/10.1002/advs.202303781
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author Marchi, Miriam
Raciti, Edoardo
Gali, Sai Manoj
Piccirilli, Federica
Vondracek, Hendrik
Actis, Arianna
Salvadori, Enrico
Rosso, Cristian
Criado, Alejandro
D'Agostino, Carmine
Forster, Luke
Lee, Daniel
Foucher, Alexandre C.
Rai, Rajeev Kumar
Beljonne, David
Stach, Eric A.
Chiesa, Mario
Lazzaroni, Roberto
Filippini, Giacomo
Prato, Maurizio
Melchionna, Michele
Fornasiero, Paolo
author_facet Marchi, Miriam
Raciti, Edoardo
Gali, Sai Manoj
Piccirilli, Federica
Vondracek, Hendrik
Actis, Arianna
Salvadori, Enrico
Rosso, Cristian
Criado, Alejandro
D'Agostino, Carmine
Forster, Luke
Lee, Daniel
Foucher, Alexandre C.
Rai, Rajeev Kumar
Beljonne, David
Stach, Eric A.
Chiesa, Mario
Lazzaroni, Roberto
Filippini, Giacomo
Prato, Maurizio
Melchionna, Michele
Fornasiero, Paolo
author_sort Marchi, Miriam
collection PubMed
description The manipulation of carbon nitride (CN) structures is one main avenue to enhance the activity of CN‐based photocatalysts. Increasing the efficiency of photocatalytic heterogeneous materials is a critical step toward the realistic implementation of sustainable schemes for organic synthesis. However, limited knowledge of the structure/activity relationship in relation to subtle structural variations prevents a fully rational design of new photocatalytic materials, limiting practical applications. Here, the CN structure is engineered by means of a microwave treatment, and the structure of the material is shaped around its suitable functionality for Ni dual photocatalysis, with a resulting boosting of the reaction efficiency toward many C—X (X = N, S, O) couplings. The combination of advanced characterization techniques and first‐principle simulations reveals that this enhanced reactivity is due to the formation of carbon vacancies that evolve into triazole and imine N species able to suitably bind Ni complexes and harness highly efficient dual catalysis. The cost‐effective microwave treatment proposed here appears as a versatile and sustainable approach to the design of CN‐based photocatalysts for a wide range of industrially relevant organic synthetic reactions.
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spelling pubmed-105026712023-09-16 Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis Marchi, Miriam Raciti, Edoardo Gali, Sai Manoj Piccirilli, Federica Vondracek, Hendrik Actis, Arianna Salvadori, Enrico Rosso, Cristian Criado, Alejandro D'Agostino, Carmine Forster, Luke Lee, Daniel Foucher, Alexandre C. Rai, Rajeev Kumar Beljonne, David Stach, Eric A. Chiesa, Mario Lazzaroni, Roberto Filippini, Giacomo Prato, Maurizio Melchionna, Michele Fornasiero, Paolo Adv Sci (Weinh) Research Articles The manipulation of carbon nitride (CN) structures is one main avenue to enhance the activity of CN‐based photocatalysts. Increasing the efficiency of photocatalytic heterogeneous materials is a critical step toward the realistic implementation of sustainable schemes for organic synthesis. However, limited knowledge of the structure/activity relationship in relation to subtle structural variations prevents a fully rational design of new photocatalytic materials, limiting practical applications. Here, the CN structure is engineered by means of a microwave treatment, and the structure of the material is shaped around its suitable functionality for Ni dual photocatalysis, with a resulting boosting of the reaction efficiency toward many C—X (X = N, S, O) couplings. The combination of advanced characterization techniques and first‐principle simulations reveals that this enhanced reactivity is due to the formation of carbon vacancies that evolve into triazole and imine N species able to suitably bind Ni complexes and harness highly efficient dual catalysis. The cost‐effective microwave treatment proposed here appears as a versatile and sustainable approach to the design of CN‐based photocatalysts for a wide range of industrially relevant organic synthetic reactions. John Wiley and Sons Inc. 2023-07-06 /pmc/articles/PMC10502671/ /pubmed/37409444 http://dx.doi.org/10.1002/advs.202303781 Text en © 2023 The Authors. Advanced Science published by Wiley‐VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
Marchi, Miriam
Raciti, Edoardo
Gali, Sai Manoj
Piccirilli, Federica
Vondracek, Hendrik
Actis, Arianna
Salvadori, Enrico
Rosso, Cristian
Criado, Alejandro
D'Agostino, Carmine
Forster, Luke
Lee, Daniel
Foucher, Alexandre C.
Rai, Rajeev Kumar
Beljonne, David
Stach, Eric A.
Chiesa, Mario
Lazzaroni, Roberto
Filippini, Giacomo
Prato, Maurizio
Melchionna, Michele
Fornasiero, Paolo
Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
title Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
title_full Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
title_fullStr Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
title_full_unstemmed Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
title_short Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
title_sort carbon vacancies steer the activity in dual ni carbon nitride photocatalysis
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10502671/
https://www.ncbi.nlm.nih.gov/pubmed/37409444
http://dx.doi.org/10.1002/advs.202303781
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