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Can a Nonorganometallic Ruthenium(II) Polypyridylamine Complex Catalyze Hydride Transfer? Mechanistic Insight from Solution Kinetics on the Reduction of Coenzyme NAD+ by Formate

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dc.contributor.author Chrzanowska, Marta
dc.contributor.author Katafias, Anna
dc.contributor.author van Eldik, Rudi
dc.date.accessioned 2022-03-11T13:37:05Z
dc.date.available 2022-03-11T13:37:05Z
dc.date.issued 2020
dc.identifier.citation Inorganic Chemistry vol. 59, 2020, pp.14944−14953.
dc.identifier.issn 0020-1669
dc.identifier.other https://dx.doi.org/10.1021/acs.inorgchem.0c01613
dc.identifier.uri http://repozytorium.umk.pl/handle/item/6717
dc.description.abstract Application of organometallic ruthenium(II) arene complexes has been successful for the modulation of cellular redox processes via their interaction with species such as formate to control the NAD+/NADH balance in cells. Here we present the first evidence that similar effects can be reached with the application of a nonorganometallic ruthenium(II) polypyridyl complex. Kinetic studies performed demonstrate the ability of [RuII(terpy)(en)(H2O/EtOH)]2+ in water/ethanol (1:9, v/v) solution, where terpy = 2,2′:6′,2″-terpyridine and en = ethylenediamine, to catalyze the reduction of the NAD+ coenzyme to NADH in the presence of formate as hydride transfer source. In this case, terpy instead of arene is responsible for the labilization of coordinated solvent. The suggested catalytic cycle begins with the fast anation of the [RuII(terpy)(en)(H2O/EtOH)]2+ complex by formate. This is followed by the rate-determining formate-catalyzed decarboxylation of the generated ruthenium(II) formato complex to form [RuII(terpy)(en)H]+. Rapid hydride transfer to NAD+ from [RuII(terpy)(en)H]+ to form NADH and to regenerate the starting ruthenium(II) solvato complex, closes the overall catalytic cycle.
dc.description.sponsorship This project was supported financially by the National Science Center, Poland (Grant Preludium 2019/33/N/ST4/00700).
dc.language.iso eng
dc.publisher American Chemical Society
dc.relation.ispartofseries Inorganic Chemistry;2020, 59, 14944−14953
dc.rights Attribution-NonCommercial-NoDerivs 3.0 Poland
dc.rights.uri http://creativecommons.org/licenses/by-nc-nd/3.0/pl/
dc.subject Borohydrides
dc.subject Catalysis
dc.subject Coordination Complexes
dc.subject Formates
dc.subject Hydrogen
dc.subject Kinetics
dc.subject Models
dc.subject Chemical
dc.subject NAD
dc.subject Oxidation-Reduction
dc.subject Pyridines
dc.subject Ruthenium
dc.title Can a Nonorganometallic Ruthenium(II) Polypyridylamine Complex Catalyze Hydride Transfer? Mechanistic Insight from Solution Kinetics on the Reduction of Coenzyme NAD+ by Formate
dc.type info:eu-repo/semantics/article
dc.contributor.supervisor Katafias, Anna


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