Homogeneously catalysed conversion of aqueous formaldehyde to H<sub>2</sub> and carbonate.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 28452367.
- Also identified by DOI 10.1038/ncomms14990 and PMC identifier 5414358.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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 trop<sub>2</sub>dad catalyse the production of H<sub>2</sub> 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.