Solar fuels research aims to mimic photosynthesis and devise integrated systems that can capture, convert, and store solar energy in the form of high-energy molecular bonds. Molecular hydrogen is generally considered an ideal solar fuel because its combustion is essentially pollution-free. Cobaloximes rank among the most promising earth-abundant catalysts for the reduction of protons to molecular hydrogen. We have used multifrequency EPR spectroscopy at X-band, Q-band, and D-band combined with DFT calculations to reveal electronic structure and establish correlations among the structure, surroundings, and catalytic activity of these complexes. To assess the strength and nature of ligand cobalt interactions, the BF2-capped cobaloxime, Co(dmgBF2)2, was studied in a variety of different solvents with a range of polarities and stoichiometric amounts of potential ligands to the cobalt ion. This allows the differentiation of labile and strongly coordinating axial ligands for the Co(II) complex. Labile, or weakl...

/pdf/the-hydrogen-catalyst-cobaloxime-a-multifrequency-epr-and-2xczfpw14d.pdf

The Hydrogen Catalyst Cobaloxime: A Multifrequency EPR and DFT Study of Cobaloxime’s Electronic Structure

Dihydrogen reduction of nitroaromatics, alkenes, alkynes and aromatic carbonyls by ortho-metalated Pd(II) complexes in homogeneous phase

Transition metals in organic synthesis: hydroformylation, reduction and oxidation

Transition metals in organic synthesis: Hydroformylation, reduction and oxidation: Annual survey covering the year 1983

2 – Hydrogenation and related reactions

Reaction of cobalt dimethylglyoxime dihydrate with amines gives rise to a catalyst for hydrogenation of nitrobenzene. Solutions of this catalyst in acetone are paramagnetic and EPR spectra of these solutions were measured. The presence of nitrobenzene considerably alters the EPR spectra. It was also observed that electron transfer from cobaloximes to TCNE is only possible in the presence of PhNO2. Changes of the EPR spectra during catalytic process were observed and interpreted.

Epr study of the system [diaquocobaloxime + amine] as a catalyst for the hydrogenation of nitrobenzene

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Epr study of the system [diaquocobaloxime + amine] as a catalyst for the hydrogenation of nitrobenzene