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Ion mobility mass spectrometry uncovers regioselectivity in the carboxylate-assisted C–H activation of palladium N-heterocyclic carbene complexes
dc.contributor.author | Ibañez-Ibañez, Laura | |
dc.contributor.author | Mollar Cuni, Andrés | |
dc.contributor.author | Apaloo-Messan , Edmond | |
dc.contributor.author | Sharma, Akhilesh Kumar | |
dc.contributor.author | Mata Martínez, Jose A | |
dc.contributor.author | Maseras, Feliu | |
dc.contributor.author | Vicent Barrera, Cristian | |
dc.date.accessioned | 2024-02-12T10:44:39Z | |
dc.date.available | 2024-02-12T10:44:39Z | |
dc.date.issued | 2023-11-27 | |
dc.identifier.citation | IBÁÑEZ-IBÁÑEZ, Laura, et al. Ion mobility mass spectrometry uncovers regioselectivity in the carboxylate-assisted C–H activation of palladium N-heterocyclic carbene complexes. Dalton Transactions, 2024, vol. 53, no 2, p. 656-665. | ca_CA |
dc.identifier.uri | http://hdl.handle.net/10234/205810 | |
dc.description.abstract | Carboxylate-assisted Pd-catalyzed C–H bond activation constitutes a mild and versatile synthetic tool to efficiently and selectively cleave inert C–H bonds. Herein, we demonstrate a simple method to experimentally evaluate both reactivity and selectivity in such systems using mass spectrometry (MS) methods. The N-heterocyclic carbene (NHC) cations [(NHC)PdX]+, bearing as X− ligand bases commonly used to promote the C–H activation (carboxylates and bicarbonate), are generated in the gas-phase by ESI-MS. Their C–H bond activation at the N-bound groups of the NHC is then studied using Collision Induced Dissociation (CID) experiments. Ion Mobility Spectrometry (IM)-MS is exploited to identify a number of regioisomers associated with the distinctive site selective C–H activations. It is demonstrated that such C–H activation concomitant with acetic acid release occurs from a mixture of activated [(NHC-H)Pd(CH3CO2H)]+ and non-activated [(NHC)Pd(CH3CO2)]+ complexes. The identity of the X-type ligands (X = Cl−, carboxylates and bicarbonate) has a significant impact on the regioisomer branching ratio upon CID conditions. IM-MS in conjunction with a DFT mechanistic study is presented for the acetate-assisted C–H activation of the [(NHC)Pd(CH3CO2)]+ cation featuring butyl and aryl as N-donor groups. | ca_CA |
dc.format.extent | 9 p. | ca_CA |
dc.format.mimetype | application/pdf | ca_CA |
dc.language.iso | eng | ca_CA |
dc.publisher | Royal Society of Chemistry | ca_CA |
dc.relation | Una manera de hacer Europa | ca_CA |
dc.rights | © 2024 The Royal Society of Chemistry | ca_CA |
dc.rights.uri | http://rightsstatements.org/vocab/InC/1.0/ | ca_CA |
dc.subject | activation analysis | ca_CA |
dc.subject | carboxylation | ca_CA |
dc.subject | chemical activation | ca_CA |
dc.subject | palladium compounds | ca_CA |
dc.subject | positive ions | ca_CA |
dc.subject | ligands | ca_CA |
dc.subject | organic compounds | ca_CA |
dc.title | Ion mobility mass spectrometry uncovers regioselectivity in the carboxylate-assisted C–H activation of palladium N-heterocyclic carbene complexes | ca_CA |
dc.type | info:eu-repo/semantics/article | ca_CA |
dc.identifier.doi | https://doi.org/10.1039/D3DT02793G | |
dc.rights.accessRights | info:eu-repo/semantics/embargoedAccess | ca_CA |
dc.type.version | info:eu-repo/semantics/acceptedVersion | ca_CA |
project.funder.name | Ministerio de Ciencia, Innovación y Universidades (Spain) | ca_CA |
project.funder.name | Universitat Jaume I | ca_CA |
project.funder.name | MCIN/AEI/10.13039/501100011033 | ca_CA |
project.funder.name | FEDER | ca_CA |
project.funder.name | AGAUR | ca_CA |
oaire.awardNumber | PID2021-126071OB-C22 | ca_CA |
oaire.awardNumber | CEX2019-000925-S | ca_CA |
oaire.awardNumber | PID2020-112825RB-I00 | ca_CA |
oaire.awardNumber | RED2022-134074-T | ca_CA |
oaire.awardNumber | UJI-B2022-23 | ca_CA |
oaire.awardNumber | FPU20/04385 | ca_CA |
oaire.awardNumber | 2019-BP-00190 | ca_CA |
dc.subject.ods | 3. Salud y bienestar | ca_CA |
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