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H2 Binding, Splitting, and Net Hydrogen Atom Transfer at a Paramagnetic Iron Complex.

Demyan E Prokopchuk1, Geoffrey M Chambers1, Eric D Walter2

  • 1Center for Molecular Electrocatalysis, Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.

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Summary
This summary is machine-generated.

Paramagnetic iron complexes can bind and split hydrogen (H2). This study details a novel iron complex that cleaves H2 via a unique mechanism involving a paramagnetic dihydride intermediate.

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Area of Science:

  • Organometallic Chemistry
  • Hydrogen Activation
  • Catalysis

Background:

  • Diamagnetic transition metal complexes for H2 binding and splitting are well-researched.
  • Paramagnetic complexes exhibiting similar reactivity are scarce, presenting a gap in understanding.

Purpose of the Study:

  • To investigate the H2 binding and splitting capabilities of a paramagnetic iron complex.
  • To elucidate the mechanism of H2 cleavage by this novel complex.

Main Methods:

  • Solution-phase studies of H2/D2 binding and cleavage kinetics.
  • Electrochemical analysis and Electron Paramagnetic Resonance (EPR) spectroscopy.
  • Density Functional Theory (DFT) calculations for mechanistic insights.

Main Results:

  • The square planar S = 1/2 FeI(P4N2)+ cation (FeI+) reversibly binds H2/D2 with an inverse isotope effect.
  • FeI+ cleaves H2 via a net hydrogen atom transfer, forming trans-FeII(H)(H2)+.
  • A paramagnetic dihydride intermediate, trans-FeIII(H)2+, was identified as key to the H2 splitting mechanism.

Conclusions:

  • The study presents a rare example of a paramagnetic complex activating H2.
  • A novel mechanism involving intra- and intermolecular steps and a paramagnetic dihydride intermediate is proposed for H2 splitting.
  • The findings contribute to the understanding of hydrogen activation by transition metal complexes.