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Multifunctional Catalysis of Nanosheet Defective Molybdenum Sulfide Basal Planes for Tandem Reactions Involving Alcohols and Molecular Hydrogen
dc.contributor.author | Rodenes, Miriam | |
dc.contributor.author | Dhaeyere, Frederic | |
dc.contributor.author | Martín Solans, Santiago | |
dc.contributor.author | Concepcion, Patricia | |
dc.contributor.author | Corma, Avelino | |
dc.contributor.author | Sorribes, Iván | |
dc.date.accessioned | 2023-10-03T07:47:39Z | |
dc.date.available | 2023-10-03T07:47:39Z | |
dc.date.issued | 2023-08-21 | |
dc.identifier.citation | Rodenes, M.; Dhaeyere, F.; Martín, S.; Concepción, P.; Corma, A.; Sorribes, I.Multisite Multifunctional Catalysis of Nanosheet Defective Molybdenum Sulfide Basal Planes for Tandem Reactions Involving Alcohols and Molecular Hydrogen. ACS Sustainable Chem. Eng. 2023, 11, 33, 12265–12279, DOI: 10.1021/acssuschemeng.3c01489 | ca_CA |
dc.identifier.issn | 2168-0485 | |
dc.identifier.uri | http://hdl.handle.net/10234/204392 | |
dc.description.abstract | Establishing tandem catalytic synthetic strategies based on the use of readily available, stable, and renewable feedstocks is of great significant for the sustainable advancement of chemical-related industries. The key to success largely relies on applying efficient multifunctional catalysts that allow carrying out one-pot single-step synthesis. In this work, we have demonstrated that defect-engineered basal planes of a molybdenum sulfide nanomaterial ({Mo3S4}n) offer a multifunctional catalytic platform for chemical process intensification. By applying this catalyst, besides borrowing hydrogen-type processes, herein exemplified for the thioetherification of alcohols, we have also disclosed novel and rare coupling reactions requiring hydrogen activation and alcohol dehydrogenation processes in a one-pot fashion. More specifically, oxidized nucleophiles, such as o-dinitroarenes and dinitrophenyl disulfides, are reacted with alcohols in the presence of H2 to yield respectively benzimidazoles and benzothiazoles. The uncommon catalytic reactivity of {Mo3S4}n arises from the presence of coordinatively unsaturated molybdenum and sulfide species, which work as Lewis acid and Lewis basic sites, respectively. As suggested by in situ infrared (IR) spectroscopy investigations, the alcohol dehydrogenation involves the participation of both types of active sites while the H2 dissociation takes place on coordinatively unsaturated sulfide species. | ca_CA |
dc.format.extent | 15 p. | ca_CA |
dc.format.mimetype | application/pdf | ca_CA |
dc.language.iso | eng | ca_CA |
dc.publisher | American Chemical Society | ca_CA |
dc.relation.isPartOf | ACS Sustainable Chemistry & Engineering, 2023, vol. 11, no 33 | ca_CA |
dc.rights | Copyright © 2023 American Chemical Society | ca_CA |
dc.rights.uri | http://rightsstatements.org/vocab/CNE/1.0/ | ca_CA |
dc.subject | molybdenum sulfide | ca_CA |
dc.subject | defective basal planes | ca_CA |
dc.subject | alcohols | ca_CA |
dc.subject | borrowing hydrogen | ca_CA |
dc.subject | coupling reactions | ca_CA |
dc.subject | thioethers | ca_CA |
dc.subject | benzimidazoles | ca_CA |
dc.subject | benzothiazoles | ca_CA |
dc.title | Multifunctional Catalysis of Nanosheet Defective Molybdenum Sulfide Basal Planes for Tandem Reactions Involving Alcohols and Molecular Hydrogen | ca_CA |
dc.type | info:eu-repo/semantics/article | ca_CA |
dc.identifier.doi | https://doi.org/10.1021/acssuschemeng.3c01489 | |
dc.rights.accessRights | info:eu-repo/semantics/embargoedAccess | ca_CA |
dc.relation.publisherVersion | https://pubs.acs.org/doi/full/10.1021/acssuschemeng.3c01489 | ca_CA |
dc.description.sponsorship | This work has been supported by the Gen-T Plan of the Generalitat Valenciana through the programs “Subvencions a l’Excel·lència Científica de Júniors Investigadors” (SEJI/2020/018) and “Investigadors Doctors d’Exel·lència” (CIDEXG/2022/22). Financial support by the Severo Ochoa Center of Excellence program (CEX2021-001230-S) is gratefully acknowledged. S.M. thanks DGA/fondos FEDER (construyendo Europa desde Aragón) for funding the research group Platón (E31_20R). M.R. acknowledges the Vice-Rectorate for Research, Innovation and Transfer of the Universitat Politècnica de València (UPV) for a pre-doctoral fellowship. F.D. thanks the ERASMUS+ program. The authors also thank the Electron Microscopy Service of the UPV for TEM and STEM facilities and Dr. G. Antorrena for technical support in XPS studies. | |
dc.type.version | info:eu-repo/semantics/acceptedVersion | ca_CA |
project.funder.name | Generalitat Valenciana | ca_CA |
project.funder.name | Agencia Estatal de Investigación | ca_CA |
project.funder.name | European Regional Development Fund | ca_CA |
project.funder.name | Erasmus+ | ca_CA |
project.funder.name | Universitat Politècnica de València | ca_CA |
oaire.awardNumber | SEJI/2020/018 | ca_CA |
oaire.awardNumber | CIDEXG/2022/22 | ca_CA |
oaire.awardNumber | CEX2021-001230-S | ca_CA |
oaire.awardNumber | E31_20R | ca_CA |
dc.subject.ods | 9. Industria, innovacion e infraestructura | ca_CA |
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