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Träfflista för sökning "WFRF:(Akermark B) ;pers:(Huang Ping)"

Sökning: WFRF:(Akermark B) > Huang Ping

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1.
  • Huang, Ping, et al. (författare)
  • Photo-induced oxidation of a dinuclear Mn-2(II,II) complex to the Mn-2(III,IV) state by inter- and intramolecular electron transfer to Ru-III tris-bipyridine
  • 2002
  • Ingår i: Journal of Inorganic Biochemistry. - 0162-0134 .- 1873-3344. ; 91:1, s. 159-172
  • Tidskriftsartikel (refereegranskat)abstract
    • To model the structural and functional parts of the water oxidizing complex in Photosystem 11, a dimeric manganese(II,11) complex (1) was linked to a ruthenium(II)tris-bipyridine (Ru-II(bpy)3) complex via a substituted L-tyrosine, to form the trinuclear complex 2 [J. Inorg. Biochem. 78 (2000) 15]. Flash photolysis of 1 and Ru-II(bpy), in aqueous solution, in the presence of an electron acceptor, resulted in the stepwise extraction of three electrons by Ru-III(bpy), from the Mn-2(II,II) dimer, which then attained the Mn-2(III,IV) oxidation state. In a similar experiment with compound 2, the dinuclear Mn complex reduced the photo-oxidized Ru moiety via intramolecular electron transfer on each photochemical event. From EPR it was seen that 2 also reached the Mn-2(III,IV) state. Our data indicate that oxidation from the Mn-2(II,II) state proceeds stepwise via intermediate formation of Mn-2(II,III) and Mn-2(III,III). In the presence of water, cyclic voltammetry showed an additional anodic peak beyond Mn-2(II,III/III,III) oxidation which was significantly lower than in neat acetonitrile. Assuming that this peak is due to oxidation to Mn-2(III,IV), this suggests that water is essential for the formation of the Mn-2(III,IV) oxidation state. Compound 2 is a structural mimic of the water oxidizing complex, in that it links a Mn complex via a tyrosine to a highly oxidizing photosensitizer. Complex 2 also mimics mechanistic aspects of Photosystem 11, in that the electron transfer to the photosensitizer is fast and results in several electron extractions from the Mn moiety.
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2.
  • Johansson, A., et al. (författare)
  • Synthesis and photophysics of one mononuclear Mn(III) and one dinuclear Mn(III,III) complex covalently linked to a ruthenium(II) tris(bipyridyl) complex
  • 2003
  • Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 42, s. 7502-7511
  • Tidskriftsartikel (refereegranskat)abstract
    • The preparation of donor (D)-photosensitizer (S) arrays, consisting of a manganese complex as D and a ruthenium tris(bipyridyl) complex as S has been pursued. Two new ruthenium complexes containing coordinating sites for one (2a) and two manganese ions (3a) were prepared in order to provide models for the donor side of photosystem II in green plants. The manganese coordinating site consists of bridging and terminal phenolate as well as terminal pyridyl ligands. The corresponding ruthenium-manganese complexes, a manganese monomer 2b and dimer 3b, were obtained. For the dimer 3b, our data suggest that intramolecular electron transfer from manganese to photogenerated ruthenium(III) is fast, k(ET) > 5 x 10(7) s(-1).
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3.
  • Lomoth, R., et al. (författare)
  • Synthesis and characterization of a dinuclear manganese(III,III) complex with three phenolate ligands
  • 2002
  • Ingår i: European Journal of Inorganic Chemistry. - 1434-1948 .- 1099-1948. ; 2002:11, s. 2965-2974
  • Tidskriftsartikel (refereegranskat)abstract
    • A dinuclear manganese complex ([Mn2L(mu-OAc)(2)]PF6) has been synthesized, where L is the trianion of 2,6-bis{[(2-hydroxy-3,5-di- tert-butylbenzyl) (2-pyridylmethyl) amino] methyl)-4-methylphenol, a ligand with three phenolate groups. The two pseudo-octahedrally coordinated Mn ions are bridged via the two bidentate acetate ligands and the 4-methylphenolate group of the ligand. We have characterized the complex with electrochemistry, spectroelectrochemistry and EPR spectroscopy. Electrochemically the Mn-2(III,III) complex undergoes two metal-centered quasi-reversible one-electron reduction steps (E-1/2 = 0.04 and -0.32 V vs. SCE). Reduction to the Mn-2(II,III) state results in transformation into a modified complex with slightly different redox properties. One-electron oxidation (E-1/2 = 0.96 V vs. SCE) affords the Mn-2(III,IV) state while further one-electron oxidation (E-1/2 = 1.13 V vs. SCE) presumably involves ligand oxidation. High valent Mn complexes involving Mn-IV or Mn-V centers are of particular interest as intermediates in catalytic water oxidation. The redox potentials of [Mn2L(mu-OAC)(2)](+) show the expected stabilization of higher manganese oxidation states compared with the related complex, [Mn-2(bpmp)(mu-OAc)(2)](+).
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4.
  • Sun, Licheng C., et al. (författare)
  • Towards an artificial model for Photosystem II : a manganese(II,II) dimer covalently linked to ruthenium(II) tris-bipyridine via a tyrosine derivative
  • 2000
  • Ingår i: Journal of Inorganic Biochemistry. - 0162-0134 .- 1873-3344. ; 78:1, s. 15-22
  • Tidskriftsartikel (refereegranskat)abstract
    • In order to model the individual electron transfer steps from the manganese cluster to the photooxidized sensitizer P-680(+) in Photosystem II (PS II) in green plants, the supramolecular complex 4 has been synthesized. In this complex, a ruthenium(II) tris-bipyridine type photosensitizer has been linked to a manganese(II) dimer via a substituted L-tyrosine, which bridges the manganese ions. The trinuclear complex 4 was characterized by electron paramagnetic resonance (EPR) and electrospray ionization mass spectrometry (ESI-MS). The excited state lifetime of the ruthenium tris-bipyridine moiety in 4 was found to be about 110 ns in acetonitrile, Using flash photolysis in the presence of an electron acceptor (methylviologen), it was demonstrated that in the supramolecular complex 4 an electron was transferred from the excited state of the ruthenium tris-bipyridine moiety to methylviologen, forming a methylviologen radical and a ruthenium(III) tris-bipyridine moiety. Next, the Ru(III) species retrieved the electron from the manganese(II/II) dimer in an intramolecular electron transfer reaction with a rate constant k(ET)>1.0X10(7) s(-1), generating a manganese(II/III) oxidation state and regenerating the ruthenium(II) photosensitizer. This is the first example of intramolecular electron transfer in a supramolecular complex, in which a manganese dimer is covalently linked to a photosensitizer via a tyrosine unit, in a process which mimics the electron transfer on the donor side of PS II.
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5.
  • Wolpher, H., et al. (författare)
  • Synthesis of a Ru(bpy)(3)-type complex linked to a free terpyridine ligand and its use for preparation of polynuclear bimetallic complexes
  • 2004
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 98:4, s. 529-536:98, s. 529-536
  • Tidskriftsartikel (refereegranskat)abstract
    • A terpyridine ligand has been covalently linked to a Ru(bpy)(3) complex via an amide bond. By using this functionalized terpyridine ligand, a series of multinuclear bimetallic complexes have been synthesized and characterized. One of these complexes has the structure of di-mu-oxobridged Mn dimer. EPR spectra of this complex showed that, depending on the procedure for the preparation, the oxidation states of the Mn dimer is either a Mn-2(III,IV) dimer or a mixture of this and Mn-2(IV,IV) dimer. Water oxidation catalyzed by this complex has been performed.
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  • Resultat 1-5 av 5

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