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Additive-Free Formic Acid Dehydrogenation Catalyzed by a Cobalt Complex

Nicolas Lentz 1 Alicia Aloisi 1 Pierre Thuéry 1 Emmanuel Nicolas 1 Thibault Cantat 1
1 LCMCE - Laboratoire de Chimie Moléculaire et de Catalyse pour l'Energie (ex LCCEF)
NIMBE UMR 3685 - Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M)
Abstract : 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 67 min–1 measured in the first minute and a turnover number (TON) of 454, without the need for bases or additives. A mechanistic study reveals the existence of ligand–metal cooperativity with intermolecular hydrogen bonding, also influenced by the concentration of formic acid.
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https://hal-cea.archives-ouvertes.fr/cea-03190418
Contributor : Serge Palacin <>
Submitted on : Tuesday, April 6, 2021 - 11:42:13 AM
Last modification on : Thursday, April 8, 2021 - 3:42:46 AM

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Nicolas Lentz, Alicia Aloisi, Pierre Thuéry, Emmanuel Nicolas, Thibault Cantat. Additive-Free Formic Acid Dehydrogenation Catalyzed by a Cobalt Complex. Organometallics, American Chemical Society, 2021, 40 (5), pp.565-569. ⟨10.1021/acs.organomet.0c00777⟩. ⟨cea-03190418⟩

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