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Reactive high-spin iron(IV)-oxo sites through dioxygen activation in a metal-organic framework.
Hou, Kaipeng; Börgel, Jonas; Jiang, Henry Z H; SantaLucia, Daniel J; Kwon, Hyunchul; Zhuang, Hao; Chakarawet, Khetpakorn; Rohde, Rachel C; Taylor, Jordan W; Dun, Chaochao; Paley, Maria V; Turkiewicz, Ari B; Park, Jesse G; Mao, Haiyan; Zhu, Ziting; Alp, E Ercan; Zhao, Jiyong; Hu, Michael Y; Lavina, Barbara; Peredkov, Sergey; Lv, Xudong; Oktawiec, Julia; Meihaus, Katie R; Pantazis, Dimitrios A; Vandone, Marco; Colombo, Valentina; Bill, Eckhard; Urban, Jeffrey J; Britt, R David; Grandjean, Fernande; Long, Gary J; DeBeer, Serena; Neese, Frank; Reimer, Jeffrey A; Long, Jeffrey R.
Afiliação
  • Hou K; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Börgel J; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
  • Jiang HZH; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • SantaLucia DJ; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
  • Kwon H; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Zhuang H; Max Planck Institute for Chemical Energy Conversion, D-45470 Mülheim an der Ruhr, Germany.
  • Chakarawet K; Max-Planck-Institut für Kohlenforschung, D-45470 Mülheim an der Ruhr, Germany.
  • Rohde RC; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Taylor JW; Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA 94720, USA.
  • Dun C; Department of Materials Science and Engineering, University of California, Berkeley, CA 94720, USA.
  • Paley MV; Department of Chemistry, University of California, Davis, CA 95616, USA.
  • Turkiewicz AB; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Park JG; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Mao H; The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
  • Zhu Z; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Alp EE; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
  • Zhao J; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Hu MY; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Lavina B; Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA 94720, USA.
  • Peredkov S; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
  • Lv X; Department of Materials Science and Engineering, University of California, Berkeley, CA 94720, USA.
  • Oktawiec J; Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
  • Meihaus KR; Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
  • Pantazis DA; Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
  • Vandone M; Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.
  • Colombo V; Center for Advanced Radiation Sources, The University of Chicago, Chicago, IL 60637, USA.
  • Bill E; Max Planck Institute for Chemical Energy Conversion, D-45470 Mülheim an der Ruhr, Germany.
  • Urban JJ; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Britt RD; Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.
  • Grandjean F; Department of Chemistry, University of California, Berkeley, CA 94720, USA.
  • Long GJ; Max-Planck-Institut für Kohlenforschung, D-45470 Mülheim an der Ruhr, Germany.
  • DeBeer S; Department of Chemistry, University of Milan, 20133 Milan, Italy.
  • Neese F; Department of Chemistry, University of Milan, 20133 Milan, Italy.
  • Reimer JA; Consorzio Interuniversitario Nazionale per la Scienza e Tecnologia dei Materiali (INSTM), UdR Milano, Via Golgi 19, 20133 Milano, Italy.
  • Long JR; Max Planck Institute for Chemical Energy Conversion, D-45470 Mülheim an der Ruhr, Germany.
Science ; 382(6670): 547-553, 2023 Nov 03.
Article em En | MEDLINE | ID: mdl-37917685
ABSTRACT
In nature, nonheme iron enzymes use dioxygen to generate high-spin iron(IV)=O species for a variety of oxygenation reactions. Although synthetic chemists have long sought to mimic this reactivity, the enzyme-like activation of O2 to form high-spin iron(IV) = O species remains an unrealized goal. Here, we report a metal-organic framework featuring iron(II) sites with a local structure similar to that in α-ketoglutarate-dependent dioxygenases. The framework reacts with O2 at low temperatures to form high-spin iron(IV) = O species that are characterized using in situ diffuse reflectance infrared Fourier transform, in situ and variable-field Mössbauer, Fe Kß x-ray emission, and nuclear resonance vibrational spectroscopies. In the presence of O2, the framework is competent for catalytic oxygenation of cyclohexane and the stoichiometric conversion of ethane to ethanol.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Science Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos
Texto completo
Adicionar na Minha BVS
Imprimir
XML
PubMed Links
Buscar no Google

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Science Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos