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Photooxidative Generation of Dodecaborate-Based Weakly Coordinating Anions.
Axtell, Jonathan C; Messina, Marco S; Liu, Ji-Yuan; Galaktionova, Daria; Schwan, Josef; Porter, Tyler M; Savage, Miles D; Wixtrom, Alex I; Rheingold, Arnold L; Kubiak, Clifford P; Winkler, Jay R; Gray, Harry B; Král, Petr; Alexandrova, Anastassia N; Spokoyny, Alexander M.
Afiliação
  • Axtell JC; Department of Chemistry and Biochemistry , University of California, Los Angeles , 607 Charles E. Young Drive East , Los Angeles , California 90095-1569 , United States.
  • Messina MS; Department of Chemistry and Biochemistry , University of California, Los Angeles , 607 Charles E. Young Drive East , Los Angeles , California 90095-1569 , United States.
  • Liu JY; California NanoSystems Institute , University of California, Los Angeles , 570 Westwood Plaza , Los Angeles , California 90095-1569 , United States.
  • Galaktionova D; Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysts, School of Molecular Science and Engineering , East China University of Science and Technology , Shanghai 200237 , P. R. China.
  • Porter TM; Beckman Institute , California Institute of Technology , Pasadena , California 91115 , United States.
  • Savage MD; Department of Chemistry and Biochemistry , University of California, San Diego , 9500 Gilman Drive , La Jolla , California 92093 , United States.
  • Wixtrom AI; Department of Chemistry and Biochemistry , University of California, Los Angeles , 607 Charles E. Young Drive East , Los Angeles , California 90095-1569 , United States.
  • Rheingold AL; Department of Chemistry and Biochemistry , University of California, Los Angeles , 607 Charles E. Young Drive East , Los Angeles , California 90095-1569 , United States.
  • Kubiak CP; Department of Chemistry and Biochemistry , University of California, San Diego , 9500 Gilman Drive , La Jolla , California 92093 , United States.
  • Winkler JR; Department of Chemistry and Biochemistry , University of California, San Diego , 9500 Gilman Drive , La Jolla , California 92093 , United States.
  • Gray HB; Beckman Institute , California Institute of Technology , Pasadena , California 91115 , United States.
  • Král P; Beckman Institute , California Institute of Technology , Pasadena , California 91115 , United States.
  • Spokoyny AM; Department of Chemistry and Biochemistry , University of California, Los Angeles , 607 Charles E. Young Drive East , Los Angeles , California 90095-1569 , United States.
Inorg Chem ; 58(16): 10516-10526, 2019 Aug 19.
Article em En | MEDLINE | ID: mdl-31247818
ABSTRACT
Redox-active proanions of the type B12(OCH2Ar)12 [Ar = C6F5 (1), 4-CF3C6H4 (2), 3,5-(CF3)2C6H3 (3)] are introduced in the context of an experimental and computational study of the visible-light-initiated polymerization of a family of styrenes. Neutral, air-stable proanions 1-3 were found to initiate styrene polymerization through single-electron oxidation under blue-light irradiation, resulting in polymers with number-average molecular weights (Mn) ranging from ∼6 to 100 kDa. Shorter polymer products were observed in the majority of experiments, except in the case of monomers containing 4-X (X = F, Cl, Br) substituents on the styrene monomer when polymerized in the presence of 1 in CH2Cl2. Only under these specific conditions are longer polymers (>100 kDa) observed, strongly supporting the formulation that reaction conditions significantly modulate the degree of ion pairing between the dodecaborate anion and cationic chain end. This also suggests that 1-3 behave as weakly coordinating anions (WCA) upon one-electron reduction because no incorporation of the cluster-based photoinitiators is observed in the polymeric products analyzed. Overall, this work is a conceptual realization of a single reagent that can serve as a strong photooxidant, subsequently forming a WCA.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Inorg Chem Ano de publicação: 2019 Tipo de documento: Article País de afiliação: Estados Unidos
Texto completo
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Inorg Chem Ano de publicação: 2019 Tipo de documento: Article País de afiliação: Estados Unidos