Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis.

Autor: Marchi M; Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport 'Giacomo Ciamician', INSTM UdR Trieste, University of Trieste, Via Licio Giorgieri 1, Trieste, 34127, Italy., Raciti E; Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons-UMONS, Mons, 7000, Belgium., Gali SM; Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons-UMONS, Mons, 7000, Belgium., Piccirilli F; Elettra Sincrotrone Trieste, Strada Statale 14 km 163.5 in Area Science Park Basovizza, Trieste, 34149, Italy., Vondracek H; Elettra Sincrotrone Trieste, Strada Statale 14 km 163.5 in Area Science Park Basovizza, Trieste, 34149, Italy., Actis A; Department of Chemistry and NIS Centre, University of Torino, Via Pietro Giuria 7, Torino, 10125, Italy., Salvadori E; Department of Chemistry and NIS Centre, University of Torino, Via Pietro Giuria 7, Torino, 10125, Italy., Rosso C; Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport 'Giacomo Ciamician', INSTM UdR Trieste, University of Trieste, Via Licio Giorgieri 1, Trieste, 34127, Italy., Criado A; Centro Interdisciplinar de Química e Bioloxía-CICA, Universidade da Coruña, Rúa As Carballeiras, A Coruña, 15071, Spain., D'Agostino C; Department of Chemical Engineering, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK.; Department of Civil, Chemical, Environmental and Material Engineering (DICAM), Alma Mater Studiorum, University of Bologna, Via Terracini, 28, Bologna, 40131, Italy., Forster L; Department of Chemical Engineering, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK., Lee D; Department of Chemical Engineering, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK., Foucher AC; Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA, 19104-6272, USA., Rai RK; Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA, 19104-6272, USA., Beljonne D; Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons-UMONS, Mons, 7000, Belgium., Stach EA; Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, PA, 19104-6272, USA., Chiesa M; Department of Chemistry and NIS Centre, University of Torino, Via Pietro Giuria 7, Torino, 10125, Italy., Lazzaroni R; Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons-UMONS, Mons, 7000, Belgium., Filippini G; Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport 'Giacomo Ciamician', INSTM UdR Trieste, University of Trieste, Via Licio Giorgieri 1, Trieste, 34127, Italy., Prato M; Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport 'Giacomo Ciamician', INSTM UdR Trieste, University of Trieste, Via Licio Giorgieri 1, Trieste, 34127, Italy.; Center for Cooperative Research in Biomaterials (CIC biomaGUNE), Basque Research and Technology Alliance (BRTA), Paseo de Miramón 194, Donostia-San Sebastián, 20014, Spain.; Ikerbasque, Basque Foundation for Science, Bilbao, 48013, Spain., Melchionna M; Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport 'Giacomo Ciamician', INSTM UdR Trieste, University of Trieste, Via Licio Giorgieri 1, Trieste, 34127, Italy., Fornasiero P; Department of Chemical and Pharmaceutical Sciences, Center for Energy, Environment and Transport 'Giacomo Ciamician', INSTM UdR Trieste, University of Trieste, Via Licio Giorgieri 1, Trieste, 34127, Italy.; ICCOM-CNR, Unit of Trieste, via L. Giorgieri 1, Trieste, 34127, Italy.
Jazyk: angličtina
Zdroj: Advanced science (Weinheim, Baden-Wurttemberg, Germany) [Adv Sci (Weinh)] 2023 Sep; Vol. 10 (26), pp. e2303781. Date of Electronic Publication: 2023 Jul 06.
DOI: 10.1002/advs.202303781
Abstrakt: 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.
(© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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