Two active species from a single metal halide precursor: a case study of highly productive Mn-catalyzed dehydrogenation of amine-boranes via intermolecular bimetallic cooperation

Gulyaeva, E.S.; Osipova, E.S.; Kovalenko, S.A.; Filippov, O.A.; Belkova, N.V.; Vendier, L.; Canac, Y.; Shubina, E.S.; Valyaev, D.A.

Авторы: Gulyaeva Ekaterina S., Osipova Elena S., Kovalenko Sergey A., Filippov Oleg A., Belkova Natalia V., Vendier Laure, Canac Yves, Shubina Elena S., Valyaev Dmitry A.
Журнал: Chemical science
Год издания: 2023
Издательство: Royal Society of Chemistry
Местоположение издательства: United Kingdom
DOI: 10.1039/D3SC05356C
Аннотация: Metal-metal cooperation for inert bond activation is an ubiquitous concept in coordination chemistry and catalysis. While the great majority of such transformations proceeds via intramolecular mode in binuclear complexes, only few examples of intermolecular small molecules activation are known to date using usually bimetallic frustrated Lewis pairs (Mδ+∙∙∙M’δ−). We introduce herein an alternative approach for the intermolecular bimetallic cooperativity observed in catalytic dehydrogenation of amine-boranes, in which the concomitant activation of N−H and B−H bonds of the substrate proceeds by a synergetic action of Lewis acidic (M+) and basic hydride (M−H) metal species derived from the same mononuclear complex (M−Br). It was also demonstrated that this system generated in situ from air-stable Mn(I) complex fac-[(CO)3(bis(NHC))MnBr] and NaBPh4 shows high activity for H2 production from several substrates (Me2NHBH3, tBuNH2BH3, MeNH2BH3, NH3BH3) at low catalyst loading (0.1% to 50 ppm) providing outstanding efficiency for Me2NHBH3 (TON up to 18200) largely superior to all known 3d, s-, p-, f-block metal derivatives and FLPs. These results permit to take a step forward towards more extensive use of intermolecular bimetallic cooperation concept in a modern homogeneous catalysis.
Добавил в систему: Гуляева Екатерина Сергеевна

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Two active species from a single metal halide precursor: a case study of highly productive Mn-catalyzed dehydrogenation of amine-boranes via intermolecular bimetallic cooperationстатья

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