Homogeneously catalysed conversion of aqueous formaldehyde to H2 and carbonate

نویسندگان

  • M. Trincado
  • Vivek Sinha
  • Rafael E. Rodriguez-Lugo
  • Bruno Pribanic
  • Bas de Bruin
  • Hansjörg Grützmacher
چکیده

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.

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عنوان ژورنال:

دوره 8  شماره 

صفحات  -

تاریخ انتشار 2017