Metal-cocatalyst interaction governs the catalytic activity of M II-porphyrazines for chemical fixation of CO2

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dc.creatorJulia Poliana da Silva Caldas Leal
dc.creatorWerberson de Almeida Bezerra
dc.creatorRafael Pavão das Chagas
dc.creatorChris Hebert de Jesus Franco
dc.creatorFelipe Terra Martins
dc.creatorAlexandre Moreira Meireles
dc.creatorFelipe Cesar Torres Antonio
dc.creatorPaula Homem-de-Mello
dc.creatorThiago Teixeira Tasso
dc.creatorJorge Luiz Sônego Milani
dc.date.accessioned2023-10-16T13:50:55Z
dc.date.accessioned2025-09-09T00:51:50Z
dc.date.available2023-10-16T13:50:55Z
dc.date.issued2021
dc.description.sponsorshipCNPq - Conselho Nacional de Desenvolvimento Científico e Tecnológico
dc.identifier.doihttps://doi.org/10.1021/acs.inorgchem.1c01462
dc.identifier.issn1520-510X
dc.identifier.urihttps://hdl.handle.net/1843/59439
dc.languageeng
dc.publisherUniversidade Federal de Minas Gerais
dc.relation.ispartofInorganic Chemistry
dc.rightsAcesso Restrito
dc.subjectAnions
dc.subjectCatalisadores de metal
dc.subjectEteres
dc.subjectCompostos metálicos
dc.subjectQuímica inorgânica
dc.subject.otherAnions
dc.subject.otherCatalysts
dc.subject.otherEthers
dc.subject.otherIons
dc.subject.otherMetals
dc.titleMetal-cocatalyst interaction governs the catalytic activity of M II-porphyrazines for chemical fixation of CO2
dc.typeArtigo de periódico
local.citation.epage12273
local.citation.issue16
local.citation.spage12263
local.citation.volume60
local.description.resumoChemical fixation of CO2 to produce cyclic carbonates can be a green and atomic efficient process. In this work, a series of porphyrazines (Pzs) containing electron-withdrawing groups and central MII ions (where M = Mg, Zn, Cu, and Co) were synthesized and investigated as catalysts for the cycloaddition of CO2 to epoxides. Then, the efficiency of the Pzs was tested by varying cocatalyst type and concentration, epoxide, temperature, and pressure. MgIIPz bearing trifluoromethyl groups (1) showed the best conversion, producing, selectively, 78% of propylene cyclic carbonate (PCC), indicating that a harder and stronger Lewis acid is more effective for epoxide activation. Moreover, cocatalyst variation showed a notable effect on the reaction yields. Spectrophotometric titrations, MALDI-TOF mass spectra, and theoretical calculations suggest poisoning of the catalyst when tetrabutylammonium chloride (TBAC) and large amounts of tetrabutylammonium bromide (TBAB) were used in the system. The same was not observed for tetrabutylammonium iodide (TBAI), indicating that the metal–cocatalyst interaction may govern the reaction rate. In addition, two rare examples of crystalline structures were obtained, proving the distorted square pyramidal geometry with water molecule as axial ligand. This is one of the first studies reporting Pzs as catalysts for the chemical fixation of CO2, and we believe that the intricate balance between cocatalyst concentration and conversion efficiency shown here may aid future studies in the area.
local.identifier.orcidhttps://orcid.org/0000-0002-4671-8697
local.identifier.orcidhttps://orcid.org/0000-0001-6876-3969
local.identifier.orcidhttps://orcid.org/0000-0001-9004-0927
local.identifier.orcidhttps://orcid.org/0000-0002-5422-198X
local.identifier.orcidhttps://orcid.org/0000-0002-9507-1535
local.identifier.orcidhttps://orcid.org/0000-0002-7049-4689
local.identifier.orcidhttps://orcid.org/0000-0001-9362-9227
local.identifier.orcidhttps://orcid.org/0000-0001-5661-3875
local.publisher.countryBrasil
local.publisher.departmentICX - DEPARTAMENTO DE QUÍMICA
local.publisher.initialsUFMG
local.url.externahttps://pubs.acs.org/doi/10.1021/acs.inorgchem.1c01462

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