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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,...
Autores principales: | , , , , , , , , , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
John Wiley and Sons Inc.
2023
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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. |
format | Online Article Text |
id | pubmed-10502671 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | John Wiley and Sons Inc. |
record_format | MEDLINE/PubMed |
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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