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Magnetically Induced Binary Ferrocene with Oxidized Iron.

Saif Ullah1, Stephanie Jensen1, Yanyao Liu2

  • 1Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, North Carolina 27109, United States.

Journal of the American Chemical Society
|August 2, 2023
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Summary
This summary is machine-generated.

Chemically oxidizing ferrocene was achieved by using a metal organic framework host. This enabled a novel high-spin Fe(II) state that readily binds and releases O2, altering its electronic and magnetic structure.

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Area of Science:

  • Organometallic Chemistry
  • Materials Science
  • Magnetochemistry

Background:

  • Ferrocene's structure and electronic properties remain largely unchanged for over 70 years.
  • Previous chemical oxidation attempts of ferrocene by direct iron binding were unsuccessful.
  • No significant structural or magnetic changes were previously reported for oxidized ferrocene.

Purpose of the Study:

  • To fundamentally alter the electronic and magnetic structure of ferrocene.
  • To achieve chemical oxidation of ferrocene by modifying its host environment.
  • To investigate the reversible binding of oxygen to ferrocene.

Main Methods:

  • Utilizing a metal-organic framework (MOF) as a host material for ferrocene.
  • Employing a suite of spectroscopic and analytical techniques including Mößbauer spectroscopy, EXAFS, in situ IR, SQUID, TGA, and EDXRF.
  • Conducting ab initio modeling to complement experimental data.

Main Results:

  • A novel, physically stretched/bent high-spin Fe(II) state of ferrocene was observed within the MOF.
  • This high-spin Fe(II) state readily accepted O2 from air, leading to oxidation to Fe(III).
  • Oxygen binding was demonstrated to be reversible using temperature swing experiments.

Conclusions:

  • Metal-organic framework encapsulation enables unprecedented control over ferrocene's electronic and magnetic properties.
  • Reversible oxygen binding and oxidation state changes in ferrocene have been achieved.
  • This work opens new avenues for manipulating organometallic molecules for sensing or catalytic applications.