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2. The Adaptative Modulation of the Phosphinito–Phosphinous Acid Ligand: Computational Illustration Through Palladium-Catalyzed Alcohol Oxidation.

Author

Membrat, Romain, Kondo, Tété Etonam, Agostini, Alexis, Vasseur, Alexandre, Nava, Paola, Giordano, Laurent, Martinez, Alexandre, Nuel, Didier, and Humbel, Stéphane

Subjects
*ALCOHOL oxidation, *LIGANDS (Chemistry), *HYDRIDES, *REACTION forces, *PALLADIUM, *CLASS B metals
Abstract

The phosphinito–phosphinous acid ligand (PAP) is a singular bidentate-like self-assembled ligand exhibiting dissymmetric but interchangeable electronic properties. This unusual structure has been used for the generation of active palladium hydride through alcohol oxidation. In this paper, we report the first theoretical highlight of the adaptative modulation ability of this ligand within a direct H-abstraction path for Pd and Pt catalyzed alcohol oxidation. A reaction forces study revealed rearrangements in the ligand self-assembling system triggered by a simple proton shift to promote the metal hydride generation via concerted six-center mechanism. We unveil here the peculiar behavior of the phosphinito–phosphinous acid ligand in this catalysis. [ABSTRACT FROM AUTHOR]

Published
2024
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4. Phosphinous Acid Platinum Complex as Robust Catalyst for Oxidation: Comparison with Palladium and Mechanistic Investigations

Author

Membrat, Romain, Vasseur, Alexandre, Martinez, Alexandre, Giordano, Laurent, Nuel, Didier, Institut des Sciences Moléculaires de Marseille (ISM2), and Aix Marseille Université (AMU)-École Centrale de Marseille (ECM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
inorganic chemicals, [CHIM.ORGA]Chemical Sciences/Organic chemistry, [CHIM.COOR]Chemical Sciences/Coordination chemistry, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract

International audience; Secondary phosphine oxides proved to be effective preligands to stabilise a hydroxy-platinum based catalyst that allows the aerobic/anaerobic oxidation of challenging sub-strates. Kinetic comparisons showed that this system is more efficient and stable than previously reported similar palladium-based catalysts. A neutral platinum dimer bearing bridging hydroxy ligands has been isolated and fully characterised by X-ray diffraction and its involvement in the mechanism has been evidenced by mechanistic studies.

Published
2018

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