About: Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes

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About: Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes Goto Sponge NotDistinct Permalink

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rdf:type	skos:Concept http://linked.opendata.cz/ontology/domain/vavai/Vysledek
Description	Ruthenium and osmium complexes 2a,b and 3a,b featuring the N-4,6-dioxo-5,5-dibutyl- or the N-4,6-dioxo-5,5-di-(2-propenyl)-1,4,5,6-tetrahydropyrimidin-2-yl-N'(4-ethenylphenyl)-urea ligand dimerize by a self-complementary quadruply hydrogen-bonding donor/donor/acceptor/acceptor (DDAA) motif. We provide evidence that the dimeric structures are maintained in nonpolar solvents and in 0.1 M NBu4PF6/CH2Cl2 supporting electrolyte solution. All complexes are reversibly oxidized in two consecutive two-electron oxidations (Delta E-1/2 approximate to 500 mV) without any discernible potential splitting for the oxidation of the individual hydrogen-bridged redox active moieties. IR and UV/vis/NIR spectroelectrochemistry show a one-step conversion of the neutral to the dication without any discernible features of an intermediate monooxidized radical cation. Oxidation-induced IR changes of the NH and CO groups that are involved in hydrogen bonding are restricted to the styryl-bonded urea NH function. Ruthenium and osmium complexes 2a,b and 3a,b featuring the N-4,6-dioxo-5,5-dibutyl- or the N-4,6-dioxo-5,5-di-(2-propenyl)-1,4,5,6-tetrahydropyrimidin-2-yl-N'(4-ethenylphenyl)-urea ligand dimerize by a self-complementary quadruply hydrogen-bonding donor/donor/acceptor/acceptor (DDAA) motif. We provide evidence that the dimeric structures are maintained in nonpolar solvents and in 0.1 M NBu4PF6/CH2Cl2 supporting electrolyte solution. All complexes are reversibly oxidized in two consecutive two-electron oxidations (Delta E-1/2 approximate to 500 mV) without any discernible potential splitting for the oxidation of the individual hydrogen-bridged redox active moieties. IR and UV/vis/NIR spectroelectrochemistry show a one-step conversion of the neutral to the dication without any discernible features of an intermediate monooxidized radical cation. Oxidation-induced IR changes of the NH and CO groups that are involved in hydrogen bonding are restricted to the styryl-bonded urea NH function. (en)
Title	Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes (en)
skos:prefLabel	Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes (en)
skos:notation	RIV/61388955:_____/09:00335789!RIV10-MSM-61388955
http://linked.open...avai/riv/aktivita	P Z
http://linked.open...avai/riv/aktivity	P(KAN100400702), P(OC 139), Z(AV0Z40400503)
http://linked.open...iv/cisloPeriodika	13
http://linked.open...vai/riv/dodaniDat	2010
http://linked.open...aciTvurceVysledku	Záliš, Stanislav
http://linked.open.../riv/druhVysledku	J - Článek v odborném periodiku
http://linked.open...iv/duvernostUdaju	S - Úplné a pravdivé údaje nepodléhající ochraně podle zvláštních právních předpisů
http://linked.open...titaPredkladatele	Ústav fyzikální chemie J. Heyrovského AV ČR, v.v.i.
http://linked.open...dnocenehoVysledku	312862
http://linked.open...ai/riv/idVysledku	RIV/61388955:_____/09:00335789
http://linked.open...riv/jazykVysledku	eng - angličtina
http://linked.open.../riv/klicovaSlova	bridget diruthenium complexes; supramolecular polymers; distance dependence (en)
http://linked.open.../riv/klicoveSlovo	bridget diruthenium complexes distance dependence supramolecular polymers
http://linked.open...odStatuVydavatele	US - Spojené státy americké
http://linked.open...ontrolniKodProRIV	[A34ACB8CBCD1]
http://linked.open...i/riv/nazevZdroje	Journal of the American Chemical Society
http://linked.open...in/vavai/riv/obor	CG
http://linked.open...ichTvurcuVysledku	1 (xsd:int)
http://linked.open...cetTvurcuVysledku	4 (xsd:int)
http://linked.open...vavai/riv/projekt	Nanostructured materials for catalytic, electrocatalytic and sorption applications http://linked.opendata.cz/resource/domain/vavai/projekt/OC%20139
http://linked.open...UplatneniVysledku	2009
http://linked.open...v/svazekPeriodika	131
http://linked.open...iv/tvurceVysledku	Záliš, Stanislav Winter, R. F. Zabel, M. Pichlmaier, M.
http://linked.open...ain/vavai/riv/wos	000264806300065
http://linked.open...n/vavai/riv/zamer	Struktura, reaktivita a dynamika molekulárních a biomolekulárních systémů: teorie, experiment, aplikace
issn	0002-7863
number of pages	12 (xsd:int)
is http://linked.open...avai/riv/vysledek of	Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes Electron Transfer Across Multiple Hydrogen Bonds: The Case of Ureapyrimidinedione-Substituted Vinyl Ruthenium and Osmium Complexes

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