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• W2912293199 abstract "IntroductionN-heterocyclic carbenes (NHC) are strong  donors and weak acceptors. Also, NHC forms strong metal-carbon bonds in metal complexes and hence complexes bearing NHC ligands are in general, thermally stable. Chemistry of NHCs and their transition metal complexes has been explored extensively in catalysis. Metal hydride or dihydrogen complexes are reactive intermediates and also employed as catalysts in several catalytic reactions such as hydrogenation, transfer hydrogenation, and hydroformylation. The binding of H2 to a metal center and its cleavage for the oxidative addition to a metal center are key steps in these catalytic reactions. There has been a substantial development in the field of dihydrogen chemistry. In particular, elongated dihydrogen complexes are of significant interest due to their relevance in hydrogenation reactions. A large number of elongated dihydrogen complexes have been reported. However, there has been no systematic study for the elongation of the H–H bond in dihydrogen complexes employing NHC’s as a co-ligand.ObjectivesThe objectives of this work are as follows:i. Synthesis and characterization of ruthenium dihydrogen complexes bearing an NHC ligand.ii. Systematic variation in the ligand environment around a metal center for the elongation of the H‒H bond in the process of oxidative addition of H2 to a metal center.iii. To synthesize new ruthenium hydride and dihydride complexes and explore their activities in catalysis such as hydrogenation, hydrodehalogenation, and CO2 activation.Significant resultsA series of dihydrogen complexes bearing NHC ligands of the type [RuCl(η2–H2)(CO)(IMes)(PPh3)(L)](OTf) [L = pyridine (Py), 4-methylpyridine (4MePy), acetonitrile (MeCN), pivalonitrile (Me3CCN)] have been prepared by the protonation of hydride complexes [RuHCl(CO)(IMes)(PPh3)(L)] (L = Py, 4MePy, MeCN, Me3CCN) with HOTf. The ligands (Py, 4MePy, MeCN, Me3CCN) trans to the hydride were found to be labile in all the hydride complexes. The H–H bond distances in the η2–H2 ligands of dihydrogen complexes were found to be temperature dependent. The H–H bond distances got slightly elongated (0.98-0.93 A) with an increase in the temperature (183-233 K). Phosphine analogues, [RuCl(η2–H2)(CO)(PPh3)2(L)](OTf) [L = Py, 4MePy) of NHC dihydrogen complexes were also synthesized. The H‒H bond distances were temperature invariant (0.93 A, 223-263 K) in these complexes.A series of homobimetallic ruthenium hydride [{RuHCl(CO)(IMes)(PPh3)}2(NN)] (NN= 4,4′-bpy, 4,4′-dpyen, 4,4′-dpyan) [4,4′-bipyridine (4,4′-bpy); 1,2-bis(4-pyridyl)ethylene (4,4′-dpyen); 1,2-bis(4-pyridyl)ethane) (4,4′-dpyan)] complexes bearing an NHC ligand and their corresponding dihydrogen complexes of the type [{RuCl(η2–H2)(IMes)(PPh3)(CO)}2(NN)][OTf]2 (NN= 4,4′-bpy, 4,4′-dpyen, 4,4′-dpyan) have been synthesized and characterized. They are the first examples of homobimetallic dihydrogen complexes bearing NHC ligands. In addition, hydrogenation of internal and terminal alkenes was carried out using these homobimetallic…" @default.
• W2912293199 created "2019-02-21" @default.
• W2912293199 creator A5013975202 @default.
• W2912293199 date "2018-11-22" @default.
• W2912293199 modified "2023-09-23" @default.
• W2912293199 title "Chemistry of Ru(II) Complexes Bearing N-heterocyclic Carbene, Hydride, and Dihydrogen Ligands : Synthesis, Mechanistic Insights, and Applications" @default.
• W2912293199 hasPublicationYear "2018" @default.
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