Reactive high-spin iron(IV)-oxo sites through dioxygen activation in a metal–organic framework-Reference-Cited by-同舟云学术

Reactive high-spin iron(IV)-oxo sites through dioxygen activation in a metal–organic framework

Published:2023-11-03 Issue:6670 Volume:382 Page:547-553
ISSN:0036-8075
Container-title:Science
language:en
Short-container-title:Science

Author:

Hou Kaipeng¹²^ORCID,Börgel Jonas¹²^ORCID,Jiang Henry Z. H.¹^ORCID,SantaLucia Daniel J.³⁴^ORCID,Kwon Hyunchul¹^ORCID,Zhuang Hao⁵⁶,Chakarawet Khetpakorn⁷^ORCID,Rohde Rachel C.¹^ORCID,Taylor Jordan W.¹^ORCID,Dun Chaochao⁸^ORCID,Paley Maria V.¹²^ORCID,Turkiewicz Ari B.¹^ORCID,Park Jesse G.¹^ORCID,Mao Haiyan⁵^ORCID,Zhu Ziting²⁶^ORCID,Alp E. Ercan⁹^ORCID,Zhao Jiyong⁹^ORCID,Hu Michael Y.⁹^ORCID,Lavina Barbara⁹¹⁰^ORCID,Peredkov Sergey³^ORCID,Lv Xudong¹^ORCID,Oktawiec Julia¹¹^ORCID,Meihaus Katie R.¹,Pantazis Dimitrios A.⁴^ORCID,Vandone Marco¹²^ORCID,Colombo Valentina¹²¹³^ORCID,Bill Eckhard³,Urban Jeffrey J.²⁸^ORCID,Britt R. David⁷¹⁴^ORCID,Grandjean Fernande¹⁵^ORCID,Long Gary J.¹⁵^ORCID,DeBeer Serena³^ORCID,Neese Frank⁴^ORCID,Reimer Jeffrey A.²⁵^ORCID,Long Jeffrey R.¹²⁵^ORCID

Affiliation:

1. Department of Chemistry, University of California, Berkeley, CA 94720, USA.

2. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

3. Max Planck Institute for Chemical Energy Conversion, D-45470 Mülheim an der Ruhr, Germany.

4. Max-Planck-Institut für Kohlenforschung, D-45470 Mülheim an der Ruhr, Germany.

5. Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA 94720, USA.

6. Department of Materials Science and Engineering, University of California, Berkeley, CA 94720, USA.

7. Department of Chemistry, University of California, Davis, CA 95616, USA.

8. The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

9. Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439, USA.

10. Center for Advanced Radiation Sources, The University of Chicago, Chicago, IL 60637, USA.

11. Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.

12. Department of Chemistry, University of Milan, 20133 Milan, Italy.

13. Consorzio Interuniversitario Nazionale per la Scienza e Tecnologia dei Materiali (INSTM), UdR Milano, Via Golgi 19, 20133 Milano, Italy.

14. Miller Institute for Basic Research in Science, University of California, Berkeley CA 94720, USA

15. Department of Chemistry, Missouri University of Science and Technology, University of Missouri, Rolla, MO 65409, USA.

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 O 2 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 O 2 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 Kβ x-ray emission, and nuclear resonance vibrational spectroscopies. In the presence of O 2 , the framework is competent for catalytic oxygenation of cyclohexane and the stoichiometric conversion of ethane to ethanol.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

Link

https://www.science.org/doi/pdf/10.1126/science.add7417

Reference106 articles.

1. Main-Group Compounds Selectively Oxidize Mixtures of Methane, Ethane, and Propane to Alcohol Esters

2. Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts

3. Selective anaerobic oxidation of methane enables direct synthesis of methanol

4. Versatility of biological non-heme Fe(II) centers in oxygen activation reactions

5. Non-Heme Fe(IV)–Oxo Intermediates

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