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Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis
dc.contributor.author | Marchi, Miriam | |
dc.contributor.author | Criado, Alejandro | |
dc.contributor.author | Filippini, Giacomo | |
dc.contributor.author | Prato, Maurizio | |
dc.contributor.author | Melchionna, Michele | |
dc.contributor.author | Fornasiero, Paolo | |
dc.date.accessioned | 2024-08-09T07:48:50Z | |
dc.date.available | 2024-08-09T07:48:50Z | |
dc.date.issued | 2023-07-06 | |
dc.identifier.citation | M. Marchi, E. Raciti, S. M. Gali, F. Piccirilli, H. Vondracek, A. Actis, E. Salvadori, C. Rosso, A. Criado, C. D'Agostino, L. Forster, D. Lee, A. C. Foucher, R. K. Rai, D. Beljonne, E. A. Stach, M. Chiesa, R. Lazzaroni, G. Filippini, M. Prato, M. Melchionna, P. Fornasiero, Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis. Adv. Sci. 2023, 10, 2303781. https://doi.org/10.1002/advs.202303781 | es_ES |
dc.identifier.issn | 2198-3844 | |
dc.identifier.uri | http://hdl.handle.net/2183/38498 | |
dc.description.abstract | [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 CX (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. | es_ES |
dc.description.sponsorship | The authors gratefully acknowledge the support from the European Union's Horizon 2020 project SAN4Fuel (Grant No. HORIZON-WIDERA-2021-ACCESS-03-01: 101079384). The UK High-Field Solid-State NMR Facility used in this research was funded by the EPSRC and the BBSRC (Grant No. EP/T015063/1), as well as the University of Warwick including via part funding through Birmingham Science City Advanced Materials Projects 1 and 2 supported by Advantage West Midlands (AWM) and the European Regional Development Fund (ERDF). Collaborative assistance from the Facility Manager Team (Dinu Iuga, University of Warwick) is acknowledged. C.D. and L.F. would like to acknowledge the EPSRC (Grant No. EP/V026089/1) for supporting their research activities. This electron microscopy was carried out in part at the Singh Center for Nanotechnology, which is supported by the NSF National Nanotechnology Coordinated Infrastructure Program under Grant No. NNCI-2025608. Additional support to the Nanoscale Characterization Facility at the Singh Center was provided by the Laboratory for Research on the Structure of Matter (MRSEC) supported by the National Science Foundation (Grant No. DMR-1720530). A.C. thanks Ministerio de Ciencia e Innovación (MCIN) for his research grant Ramón y Cajal (Grant No. RYC2020-030183-I). The modeling activities in Mons were supported by the Energy Transition Fund of the Belgian Federal Government (FPS Economy) within the T-REX project, the Belgian National Fund for Scientific Research (FRS-FNRS) within the Consortium des Équipements de Calcul Intensif – CÉCI, under Grant No. 2.5020.11, and by the Walloon Region (ZENOBE Tier-1 supercomputer, under Grant No. 1117545). E.R. is grateful to the University of Trieste and the University of Mons for a joint doctoral fellowship. S.M.G. is FNRS Postdoctoral Researcher. D.B. is FNRS Research Director. E.S. and M.C. acknowledge support through the Project CH4.0 under the MUR program “Dipartimenti di Eccellenza 2023-2027” (CUP: D13C22003520001). P.F. acknowledges PRIN 2022 Project funded by the Italian Ministry MUR Italy (project acronym: SYSSY-CAT). | es_ES |
dc.description.sponsorship | EPSRC/BBSRC; EP/T015063/1 | es_ES |
dc.description.sponsorship | EPSRC; EP/V026089/1 | es_ES |
dc.description.sponsorship | National Science Foundation; NNCI-2025608 | es_ES |
dc.description.sponsorship | National Science Foundation; DMR-1720530 | es_ES |
dc.description.sponsorship | Walloon Region (ZENOBE Tier-1 supercomputer); 1117545 | es_ES |
dc.description.sponsorship | Belgian National Fund for Scientific Research (FRS-FNRS); 2.5020.11 | es_ES |
dc.language.iso | eng | es_ES |
dc.publisher | Wiley-VCH | es_ES |
dc.relation | info:eu-repo/grantAgreement/EC/HE/101079384 | es_ES |
dc.relation | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RYC2020-030183-I/ES/ | es_ES |
dc.relation | info:eu-repo/grantAgreement/MUR/Progetti di Ricerca di Rilevante Interesse Nazionale 2022/ 20224P9ABM/IT/ | es_ES |
dc.relation | info:eu-repo/grantAgreement/MUR/D13C22003520001/CH4.0/IT/ | es_ES |
dc.relation.uri | https://doi.org/10.1002/advs.202303781 | es_ES |
dc.rights | © 2023 The Authors. Advanced Science published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License (https://creativecommons.org/licenses/by/4.0/), which permits use, distribution and reproduction in any medium, provided the original work is properly cited. | es_ES |
dc.subject | Carbon nitride | es_ES |
dc.subject | Dual photocatalysis | es_ES |
dc.subject | Nickel | es_ES |
dc.subject | Organic synthesis | es_ES |
dc.title | Carbon Vacancies Steer the Activity in Dual Ni Carbon Nitride Photocatalysis | es_ES |
dc.type | info:eu-repo/semantics/article | es_ES |
dc.rights.access | info:eu-repo/semantics/openAccess | es_ES |
UDC.journalTitle | Advanced Science | es_ES |
UDC.volume | 10 | es_ES |
UDC.issue | 26 | es_ES |
UDC.startPage | Article 2303781 | es_ES |
dc.identifier.doi | 10.1002/advs.202303781 |
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