Light-induced electron transfer in simple and supramolecular Ru-polypyridine complexes

mann, Stefan Bo; Heppe, Gisela; Schwarz, Ralph; Thiery, Urs; Trierweiler, H.-P.

doi:10.1007/bf03040816

Cited by 5 publications

(9 citation statements)

References 26 publications

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“…Natural as well as artificial photosynthesis possesses, − as primordial characteristics, efficient light-harvesting units for the conversion of solar energy. The basic reaction to be realized is light-induced charge separation leading to the cleavage of water.…”

Section: Introductionmentioning

confidence: 99%

“…The basic component for such systems is a good sensitizer (S = D) for electron transfer, such as porphins, ruthenium polypyridines, dyes, and semiconductors. In this Account we will treat first and exclusively functionalized ruthenium polypyridines and then more complex RuL 3 (D)−viologen (A) polyads, especially the ones developed in our group. With suitable acceptors such as viologens, electron transfer occurs in these systems.…”

Section: Introductionmentioning

confidence: 99%

“…A second route uses halopyridines and Cu(0) or Ni(0), and the third access employs Pd(0), halopyridines, and pyridyl-boric acids (Suzuki reaction). A complete construction of the second ring of 2,2‘-bipyridines is possible with the Kröhnke reaction. , …”

Section: Introductionmentioning

confidence: 99%

“…More complex D−A-linked ligands 6 will be treated below. From these ligands RuL 3 or RuL 2 L complexes were prepared …”

Section: Introductionmentioning

confidence: 99%

“…The synthetic strategy we employed for ruthenium polypyridines 6 is shown in Scheme , ,− which shows a general method for the synthesis of trishomoleptic (such as A) and bisheteroleptic Ru(II) complexes (such as B) (DMSO = dimethyl sulfoxide, λ−λ = bpz = 1,4-bipyridazine, or μ−μ = bpy = 2,2‘-bipyridine).

2 …”

Section: Introductionmentioning

confidence: 99%

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Ruthenium Polypyridine Complexes. On the Route to Biomimetic Assemblies as Models for the Photosynthetic Reaction Center

2001

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We describe in this Account the preparation of RuL(3) complexes and their significance as biomimetic models for the photosynthetic reation center. Their preparation from simple or more complicated bypyridine ligands L and their photophysical data, especially their stability, are reported. Biomimetic models involving three concepts of the interaction of RuL(3) with acceptors in coordinatively, mechanically, or covalently linked supramolecular assemblies are also presented. The electron transfer (ET) of the noncovalently linked assemblies of RuL(3) complexes carrying polyether chains with one or two anisyl binding sites (4 or 5) with the cyclic bisviologen was studied. Molecular modeling and NMR titration clearly show the formation of supramolecular assemblies. Time-resolved spectroscopy demonstrated that ET and charge separation in the RuL(3) complexes with two binding sites are more efficient. The more constrained RuL(3)-bisviologen-catenane (6) possesses two conformations which exhibit different efficiency in ET, creating a charge-separated state in the microsecond domain. The covalently linked Ru(bpy)(3)(2+)-viologen assemblies having one (7, diad) or two bisviologen arms (8, diad) result in efficient ET. Addition of linear polyethers, cyclic polyethers, or crowns generates new triads and tetrads of the pseudorotaxane type. Molecular modeling and NMR titration clearly indicate the formation of supramolecular assemblies. The analysis of time-resolved studies proves fast ET and especially long-lived charge-separated states in these pseudorotaxanes. These data, compared with the findings for the photosynthetic reation center, show conclusive results. The lifetimes of the charge-separated states increase clearly in the sequence for noncovalently < mechanically < and covalently linked assemblies.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

“…More complex D−A-linked ligands 6 will be treated below. From these ligands RuL 3 or RuL 2 L complexes were prepared …”

Section: Introductionmentioning

confidence: 99%

2 …”

Section: Introductionmentioning

confidence: 99%

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Ruthenium Polypyridine Complexes. On the Route to Biomimetic Assemblies as Models for the Photosynthetic Reaction Center

2001

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Effektive Ladungstrennung in einem intermolekularen Komplex aus Elektronendonor und doppelarmiger Triade: ein Modellsystem für die Kontrolle des Elektronentransfers durch Umgebungseffekte

et al. 1995

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Effective Charge Separation in Intermolecular Complexes of an Electron Donor and a Doubly Branched Triad Assembly: A Model System for Environmental Effects Controlling Electron Transfer

Zahavy

Seiler

Marx–Tibbon

et al. 1995

Angew. Chem. Int. Ed. Engl.

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It is too early to say whether Al, Ti avoidance is a general phenomenon in titanoaluminosilicates; however, it seems logical that, when possible, aluminum and titanium will not be neighbors. This has implications for aluminum incorporation in ETS-4.r31 Although a full structural study has not been performed on ETS-4, the structure is believed to be related to that of zorite.l*I All silicon sites in the structure of zorite neighbor titanium. and consequently aluminum atoms cannot avoid being adjacent to titanium atoms. We have been unsuccessful in our attempts to incorporate aluminum into ETS-4, possibly because the AI,Ti avoidance principle holds.In conclusion ETAS-I 0 displays Al, Ti avoidance when low to medium concentrations of aluminum are incorporated. This preference of certain sites for aluminum is maintained at higher aluminum concentrations, although the avoidance rule does not hold strictly. . The Sill Al. 1 Ti) and Si(0AI. 1 Ti) sites are crystallographically distinct. MAS NMR spectra were recorded on a Bruker MSL400 spectrometer. For "Si NMR spectra a 3.5 bs 45" pulse was used with an interpulse delay of35 s. For the "A1 NMR spectrum a 0.6 ps x/18 pulse was used with an intcrpulse delay oT0.5 s. Expcrimcwttrl Procedure ETAS-I0 with

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Light-induced electron transfer in simple and supramolecular Ru-polypyridine complexes

Cited by 5 publications

References 26 publications

Ruthenium Polypyridine Complexes. On the Route to Biomimetic Assemblies as Models for the Photosynthetic Reaction Center

Ruthenium Polypyridine Complexes. On the Route to Biomimetic Assemblies as Models for the Photosynthetic Reaction Center

Effektive Ladungstrennung in einem intermolekularen Komplex aus Elektronendonor und doppelarmiger Triade: ein Modellsystem für die Kontrolle des Elektronentransfers durch Umgebungseffekte

Effective Charge Separation in Intermolecular Complexes of an Electron Donor and a Doubly Branched Triad Assembly: A Model System for Environmental Effects Controlling Electron Transfer

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