Luminescent Ce(III) Complexes as Stoichiometric and Catalytic Photoreductants for Halogen Atom Abstraction Reactions.

Luminescent Ce(III) complexes, Ce[N(SiMe)] (1) and [(MeSi)NC(RN)]Ce[N(SiMe)] (R = Pr, Pr; R = Cy, 1-Cy), with C and C solution symmetries display absorptive 4f → 5d electronic transitions in the visible region. Emission bands are observed at 553, 518, and 523 nm for 1, Pr, and 1-Cy with lifetimes of...

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Publicado en:Journal of the American Chemical Society Vol. 137; no. 29; pp. 9234 - 9238
Autores principales: Haolin Yin, Carroll, Patrick J., Anna, Jessica M., Schelter, Eric J.
Formato: Artículo
Publicado: American Chemical Society 7/29/2015
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Acceso en línea:Ver este registro en EBSCOhost
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        atl: Luminescent Ce(III) Complexes as Stoichiometric and Catalytic Photoreductants for Halogen Atom Abstraction Reactions.
      aug:
        au:
          Haolin Yin
          Carroll, Patrick J.
          Anna, Jessica M.
          Schelter, Eric J.
        affil: P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania, 231 South 34 Street, Philadelphia, Pennsylvania 19104, United States
      su:
        Halogens
        Abstraction reactions
        Photosensitizers
        Metathesis reactions
        Density functional theory
        Abstraction process (Catalysis)
      sug:
        subj:
          Halogens
          Abstraction reactions
          Photosensitizers
          Metathesis reactions
          Density functional theory
          Abstraction process (Catalysis)
      ab: Luminescent Ce(III) complexes, Ce[N(SiMe)] (1) and [(MeSi)NC(RN)]Ce[N(SiMe)] (R = Pr, Pr; R = Cy, 1-Cy), with C and C solution symmetries display absorptive 4f → 5d electronic transitions in the visible region. Emission bands are observed at 553, 518, and 523 nm for 1, Pr, and 1-Cy with lifetimes of 24, 67, and 61 ns, respectively. Time-dependent density functional theory (TD-DFT) studies on 1 and Pr revealed the ²A excited states corresponded to singly occupied 5dz2 orbitals. The strongly reducing metalloradical character of 1, Pr, and 1-Cy in their ²A excited states afforded photochemical halogen atom abstraction reactions from sp³ and sp² C-X (X = Cl, Br, I) bonds for the first time with a lanthanide cation. The dehalogenation reactions could be turned over with catalytic amounts of photosensitizers by coupling salt metathesis and reduction to the photopromoted atom abstraction reactions.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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