NDLI: Influence of nitrosyl coordination on the binding mode of quinaldate in selective ruthenium frameworks. Electronic structure and reactivity aspects

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Influence of nitrosyl coordination on the binding mode of quinaldate in selective ruthenium frameworks. Electronic structure and reactivity aspects

Content Provider	Royal Society of Chemistry (RSC)
Author	Chowdhury, Abhishek Dutta Lahiri, Goutam Kumar De, Prinaka Mobin, Shaikh M.
Copyright Year	2012
Abstract	The nitrosyl complexes, [RuII(trpy)(L)(NO+)Cl]BF4, [1]BF4, and [RuII(trpy)(L)(NO+)](BF4)2, [2](BF4)2, (trpy = 2,2′:6′,2′′-terpyridine, L− = deprotonated form of unsymmetrical quinaldic acid) have been synthesized. Single crystal X-ray structures of [1]BF4 and [2](BF4)2 reveal that in the former L− binds to the ruthenium ion selectively in a monodentate fashion through the O− donor whereas the usual bidentate mode of L− (O−, N donors) has been retained in [2](BF4)2 with the same meridional configuration of trpy being seen in both. The Ru–NO group in [1]BF4 or [2](BF4)2, exhibits almost linear (sp-hybridized form of NO+) geometry. The difference in bonding mode of the unsymmetrical quinaldate in [1]BF4 and [2](BF4)2 has been reflected in their corresponding ν(NO)/ν(CO) frequencies as well as in their NO based two-step reduction processes, {RuII–NO+} → {RuII–NO•} and {RuII–NO•}→{RuII–NO−}. The close to bent geometry (sp2-hybridized form of NO•) of the one-electron reduced 1 or [2]+ is been reflected in their DFT optimized structures. The spin density plot of the reduced species reveals that NO is the primary spin-bearing center with slight delocalization onto the metal ion which has been reflected in its radical EPR spectrum. [1]+ and [2]2+ undergo facile photorelease of NO with significantly different kNO (s−1) and t1/2 (s) values which eventually lead to the concomitant formation of the corresponding solvent species. The photoreleased NO• can be trapped as an Mb–NO adduct. The reduced species 1 selectively reacts with the molecular oxygen (O2) at pH ∼ 1 to yield the corresponding nitro species, [RuII(trpy)(L)(NO2)Cl]−.
Starting Page	3437
Ending Page	3446
Page Count	10
File Format	HTM / HTML PDF
ISSN	20462069
Volume Number	2
Issue Number	8
Journal	RSC Advances
DOI	10.1039/c2ra00953f
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Ruthenium Allotropes of oxygen Ion Single crystal Terpyridine Molecular geometry X-ray crystallography Carboxylic acid Denticity Solvent Adduct Nucleophile
Content Type	Text
Resource Type	Article
Subject	Chemistry Chemical Engineering

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