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.
Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis / Marchi M.; Raciti E.; Gali S.M.; Piccirilli F.; Vondracek H.; Actis A.; Salvadori E.; Rosso C.; Criado A.; D'Agostino C.; Forster L.; Lee D.; Foucher A.C.; Rai R.K.; Beljonne D.; Stach E.A.; Chiesa M.; Lazzaroni R.; Filippini G.; Prato M.; Melchionna M.; Fornasiero P.. - In: ADVANCED SCIENCE. - ISSN 2198-3844. - ELETTRONICO. - 10:(2023), pp. e2303781.1-e2303781.12. [10.1002/advs.202303781]
Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
D'Agostino C.;
2023
Abstract
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.File | Dimensione | Formato | |
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