NDLI: Unusually Efficient Pyridine Photodissociation from Ru(II) Complexes with Sterically Bulky Bidentate Ancillary Ligands

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Unusually Efficient Pyridine Photodissociation from Ru(II) Complexes with Sterically Bulky Bidentate Ancillary Ligands

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Unusually Efficient Pyridine Photodissociation from Ru(II) Complexes with Sterically Bulky Bidentate Ancillary Ligands

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Knoll, Jessica D. Turro, Claudia Durr, Christopher B. Albani, Bryan A.
Description	Author Affiliation: Knoll JD ( Department of Chemistry and Biochemistry, The Ohio State University , Columbus, Ohio 43210, United States.)
Abstract	The introduction of steric bulk to the bidentate ligand in $[Ru(tpy)(bpy)(py)]^{2+}$ (1; tpy = 2,2′:2′,6″-terpyridine; bpy = 2,2′-bipyridine; py = pyridine) to provide $[Ru(tpy)(Me_{2}bpy)(py)]^{2+}$ (2; $Me_{2}bpy$ = 6,6′-dimethyl-2,2′-bipyridine) and $[Ru(tpy)(biq)(py)]^{2+}$ (3; biq = 2,2′-biquinoline) facilitates photoinduced dissociation of pyridine with visible light. Upon irradiation of 2 and 3 in $CH_{3}CN$ $(λ_{irr}$ = 500 nm), ligand exchange occurs to produce the corresponding $[Ru(tpy)(NN)(NCCH_{3})]^{2+}$ (NN = $Me_{2}bpy,$ biq) complex with quantum yields, $Φ_{500},$ of 0.16(1) and 0.033(1) for 2 and 3, respectively. These values represent an increase in efficiency of the reaction by 2–3 orders of magnitude as compared to that of 1, $Φ_{500}$ < 0.0001, under similar experimental conditions. The photolysis of 2 and 3 in $H_{2}O$ with low energy light to produce $[Ru(tpy)(NN)(OH_{2})]^{2+}$ (NN = $Me_{2}bpy,$ biq) also proceeds rapidly $(λ_{irr}$ > 590 nm). Complexes 1–3 are stable in the dark in both $CH_{3}CN$ and $H_{2}O$ under similar experimental conditions. X-ray crystal structures and theoretical calculations highlight significant distortion of the planes of the bidentate ligands in 2 and 3 relative to that of 1. The crystallographic dihedral angles defined by the bidentate ligand, $Me_{2}bpy$ in 2 and biq in 3, and the tpy ligand were determined to be 67.87° and 61.89°, respectively, whereas only a small distortion from the octahedral geometry is observed between bpy and tpy in 1, 83.34°. The steric bulk afforded by $Me_{2}bpy$ and biq also result in major distortions of the pyridine ligand in 2 and 3, respectively, relative to 1, which are believed to weaken its σ-bonding and π-back-bonding to the metal and play a crucial role in the efficiency of the photoinduced ligand exchange. The ability of 2 and 3 to undergo ligand exchange with $λ_{irr}$ > 590 nm makes them potential candidates to build photochemotherapeutic agents for the delivery of drugs with pyridine binding groups.
ISSN	10895639
e-ISSN	15205215
Journal	The Journal of Physical Chemistry A
Issue Number	45
Volume Number	118
Language	English
Publisher	American Chemical Society (United States)
Publisher Date	2014-11-13
Publisher Place	United States
Access Restriction	Open
Subject Keyword	Photolysis Pyridines Chemistry Ruthenium Compounds Crystallography, X-Ray Models, Chemical Proton Magnetic Resonance Spectroscopy Spectrum Analysis Research Support, N.I.H., Extramural Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S. Physical chemistry
Content Type	Text
Resource Type	Article
Subject	Medicine Physical and Theoretical Chemistry

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