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Homogeneously catalysed conversion of aqueous formaldehyde to H₂ and carbonate.

ABSTRACT: Small organic molecules provide a promising solution for the requirement to store large amounts of hydrogen in a future hydrogen-based energy system. Herein, we report that diolefin-ruthenium complexes containing the chemically and redox non-innocent ligand trop₂dad catalyse the production of H₂ from formaldehyde and water in the presence of a base. The process involves the catalytic conversion to carbonate salt using aqueous solutions and is the fastest reported for acceptorless formalin dehydrogenation to date. A mechanism supported by density functional theory calculations postulates protonation of a ruthenium hydride to form a low-valent active species, the reversible uptake of dihydrogen by the ligand and active participation of both the ligand and the metal in substrate activation and dihydrogen bond formation.

SUBMITTER: Trincado M

PROVIDER: S-EPMC5414358 | biostudies-literature | 2017 Apr

REPOSITORIES: biostudies-literature

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Homogeneously catalysed conversion of aqueous formaldehyde to H2 and carbonate.

Trincado M M Sinha Vivek V Rodriguez-Lugo Rafael E RE Pribanic Bruno B de Bruin Bas B Grützmacher Hansjörg H

Nature communications 20170428

Small organic molecules provide a promising solution for the requirement to store large amounts of hydrogen in a future hydrogen-based energy system. Herein, we report that diolefin-ruthenium complexes containing the chemically and redox non-innocent ligand trop2dad catalyse the production of H2 from formaldehyde and water in the presence of a base. The process involves the catalytic conversion to carbonate salt using aqueous solutions and is the fastest reported for accept ...[more]

PMID: 28452367

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