Implication of oxidant activation on olefin epoxidation catalysed by Molybdenum catalysts with aroylhydrazonato ligands: Experimental and theoretical studies - Archive ouverte HAL Access content directly
Journal Articles Molecular Catalysis Year : 2021

Implication of oxidant activation on olefin epoxidation catalysed by Molybdenum catalysts with aroylhydrazonato ligands: Experimental and theoretical studies

Arijeta Bafti
Marta Razum
  • Function : Author
Edi Topić
Dominique Agustin
Jana Pisk
  • Function : Author
  • PersonId : 1102952
Višnja Vrdoljak
] A Bafti
  • Function : Author
Iut a P Sabatier
  • Function : Author

Abstract

Dinuclear and mononuclear molybdenum(VI) complexes with aroylhydrazonato ligands were studied as catalysts for cyclooctene and oct-1-ene epoxidation. Different isomers of the OH and NH2 functionalised aroylhydrazones led to four specific [MoO2L] units showing different catalytic activity. Three oxidants have been investigated: tert-butylhydroperoxide (TBHP) in water or in decane, and hydrogen peroxide (H2O2). Catalytic processes with TBHP in decane provided outstanding results in the case of cyclooctene epoxidation: TOF2.5 min > 9000 with 0.25 mol % [Mo] loading. DFT calculations confirmed the relationship between the ligand nature and reactivity with TBHP and H2O2 as oxidant agents. In the case of TBHP as oxidant, calculations considered the solvent in which the oxidant is delivered to the olefin. A plausible mechanism with H2O2 has been proposed after considering various pathways.
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hal-03356884 , version 1 (28-09-2021)

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Arijeta Bafti, Marta Razum, Edi Topić, Dominique Agustin, Jana Pisk, et al.. Implication of oxidant activation on olefin epoxidation catalysed by Molybdenum catalysts with aroylhydrazonato ligands: Experimental and theoretical studies. Molecular Catalysis, 2021, 512, pp.111764. ⟨10.1016/j.mcat.2021.111764⟩. ⟨hal-03356884⟩
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