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Additive-Free Formic Acid Dehydrogenation Catalyzed by a Cobalt Complex

preprint
submitted on 01.09.2020 and posted on 02.09.2020 by Nicolas Lentz, Alicia Aloisi, Pierre Thuéry, Emmanuel Nicolas, Thibault Cantat
The reversible storage of hydrogen through the intermediate formation of Formic Acid (FA) is a promising solution to its safe transport and distribution. However, the common necessity of using bases or additives in the catalytic dehydrogenation of FA is a limitation. In this context, two new cobalt complexes (1 and 2) were synthesized with a pincer PP(NH)P ligand containing a phosphoramine moiety. Their reaction with an excess FA yields a cobalt(I)-hydride complex (3). We report here the unprecedented catalytic activity of 3 in the dehydrogenation of FA, with a turnover frequency (TOF) of 4000 h-1 and a turnover number (TON) of 454, without the need for bases or additives. A mechanistic study reveals that the ligand has a non-innocent behaviour due to intermolecular hydrogen bonding, which is influenced by the concentration of formic acid

Funding

818260

History

Email Address of Submitting Author

emmanuel.nicolas@cea.fr

Institution

Université Paris-Saclay, CEA, CNRS, NIMBE

Country

France

ORCID For Submitting Author

0000-0002-0017-5500

Declaration of Conflict of Interest

no conflict of interest

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