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Literature DB >> 28414226

Testing the Push-Pull Hypothesis: Lewis Acid Augmented N₂ Activation at Iron.

Jacob B Geri¹, James P Shanahan¹, Nathaniel K Szymczak¹.

Abstract

We present a systematic investigation of the structural and electronic changes that occur in an Fe(0)-N2 unit (Fe(depe)2(N2); depe = 1,2-bis(diethylphosphino)ethane) upon the addition of exogenous Lewis acids. Addition of neutral boranes, alkali metal cations, and an Fe2+ complex increases the N-N bond activation (Δ νNN up to 172 cm-1), decreases the Fe(0)-N2 redox potential, polarizes the N-N bond, and enables -N protonation at uncommonly anodic potentials. These effects were rationalized using combined experimental and theoretical studies.

Entities: Chemical Disease Species

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Year: 2017 PMID： 28414226 PMCID： PMC5965694 DOI： 10.1021/jacs.7b01982

Source DB: PubMed Journal: J Am Chem Soc ISSN： 0002-7863 Impact factor: 15.419

37 in total

10. Tetrahedral iron featuring an appended Lewis acid: distinct pathways for the reduction of hydroxylamine and hydrazine.

Authors: John J Kiernicki; Emily E Norwine; Matthias Zeller; Nathaniel K Szymczak
Journal: Chem Commun (Camb) Date: 2019-10-01 Impact factor: 6.222

Testing the Push-Pull Hypothesis: Lewis Acid Augmented N₂ Activation at Iron.

1. The controlled relay of multiple protons required at the active site of nitrogenase.

2. Selective Catalytic Reduction of N₂ to N₂H₄ by a Simple Fe Complex.

3. Nitrogen fixation revisited on iron(0) dinitrogen phosphine complexes.

4. A Terminal N2 Complex of High-Spin Iron(I) in a Weak, Trigonal Ligand Field.

5. Molybdenum nitrogenase catalyzes the reduction and coupling of CO to form hydrocarbons.

6. Fe-N2/CO complexes that model a possible role for the interstitial C atom of FeMo-cofactor (FeMoco).

7. Ligand binding to the FeMo-cofactor: structures of CO-bound and reactivated nitrogenase.

Review 8. Dinitrogen binding and cleavage by multinuclear iron complexes.

9. Alkali Metal Variation and Twisting of the FeNNFe Core in Bridging Diiron Dinitrogen Complexes.

10. Exploring secondary-sphere interactions in Fe-N _x H _y complexes relevant to N₂ fixation.

Review 1. Catalytic N₂-to-NH₃ (or -N₂H₄) Conversion by Well-Defined Molecular Coordination Complexes.

2. Effects of N₂ Binding Mode on Iron-Based Functionalization of Dinitrogen to Form an Iron(III) Hydrazido Complex.

3. Isolation and characterization of a high-spin mixed-valent iron dinitrogen complex.

Review 4. Activation of Dinitrogen by Polynuclear Metal Complexes.

5. Hydrazine Capture and N-N Bond Cleavage at Iron Enabled by Flexible Appended Lewis Acids.

6. Tridentate Phosphine Ligands Bearing Aza-Crown Ether Lariats.

7. Hydrogen Bonding to a Dinitrogen Complex at Room Temperature: Impacts on N₂ Activation.

8. Dinitrogen binding and activation at a molybdenum-iron-sulfur cluster.

9. Hydrogen Bonds Dictate O₂ Capture and Release within a Zinc Tripod.

10. Tetrahedral iron featuring an appended Lewis acid: distinct pathways for the reduction of hydroxylamine and hydrazine.

Review 8. Dinitrogen binding and cleavage by multinuclear iron complexes.

Review 1. Catalytic N2-to-NH3 (or -N2H4) Conversion by Well-Defined Molecular Coordination Complexes.

Review 4. Activation of Dinitrogen by Polynuclear Metal Complexes.

Review 1. Catalytic N₂-to-NH₃ (or -N₂H₄) Conversion by Well-Defined Molecular Coordination Complexes.