Homogeneously catalysed conversion of aqueous formaldehyde to H2 and carbonate

M. Trincado (), Vivek Sinha, Rafael E. Rodriguez-Lugo, Bruno Pribanic, Bas de Bruin () and Hansjörg Grützmacher ()
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M. Trincado: Laboratory of Inorganic Chemistry
Vivek Sinha: Supramolecular and Homogeneous Catalysis Group, van ’t Hoff Institute for Molecular Sciences (HIMS), University of Amsterdam
Rafael E. Rodriguez-Lugo: Labotatorio de Química Bioinorgánica, Centro de Química, Instituto Venezolano de Investigaciones Científicas (IVIC)
Bruno Pribanic: Laboratory of Inorganic Chemistry
Bas de Bruin: Supramolecular and Homogeneous Catalysis Group, van ’t Hoff Institute for Molecular Sciences (HIMS), University of Amsterdam
Hansjörg Grützmacher: Laboratory of Inorganic Chemistry

Nature Communications, 2017, vol. 8, issue 1, 1-11

Abstract: 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.

Date: 2017
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DOI: 10.1038/ncomms14990

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