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Literature DB >> 22008018

N2 functionalization at iron metallaboratranes.

Abstract

The reactivity of the anionic dinitrogen complex [(TPB)Fe(N(2))](-) (TPB = tris[2-(diisopropylphosphino)phenyl]borane) toward silicon electrophiles has been examined. [(TPB)Fe(N(2))](-) reacts with trimethylsilyl chloride to yield the silyldiazenido complex (TPB)Fe(NNSiMe(3)), which is reduced by Na/Hg in THF to yield the corresponding sodium-bound anion [(TPB)Fe(NNSiMe(3))]Na(THF). The use of 1,2-bis(chlorodimethylsilyl)ethane in the presence of excess Na/Hg results in the disilylation of the bound N(2) molecule to yield the disilylhydrazido(2-) complex (TPB)Fe≡NR (R = 2,2,5,5-tetramethyl-1-aza-2,5-disilacyclopentyl). One of the phosphine arms of TPB in (TPB)Fe≡NR can be substituted by CO or (t)BuNC to yield crystalline adducts (TPB)(L)Fe≡NR (L = CO, (t)BuNC). The N-N bond in (TPB)((t)BuNC)Fe≡NR is cleaved upon standing at room temperature to yield a phosphoraniminato/disilylamido iron(II) complex. The flexibility of the Fe-B linkage is thought to play a key role in these transformations of Fe-bound dinitrogen.

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Year: 2011 PMID： 22008018 PMCID： PMC3212643 DOI： 10.1021/ja208675p

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

25 in total

1. Nitrogenase MoFe-protein at 1.16 A resolution: a central ligand in the FeMo-cofactor.

Authors: Oliver Einsle; F Akif Tezcan; Susana L A Andrade; Benedikt Schmid; Mika Yoshida; James B Howard; Douglas C Rees
Journal: Science Date: 2002-09-06 Impact factor: 47.728

2. Structure and bonding in three-coordinate N-heterocyclic carbene adducts of iron(II) bis(trimethylsilyl)amide.

Authors: Richard A Layfield; Joseph J W McDouall; Manfred Scheer; Christoph Schwarzmaier; Floriana Tuna
Journal: Chem Commun (Camb) Date: 2011-09-01 Impact factor: 6.222

3. Structural and spectroscopic characterization of first-row transition metal(II) substituted blue copper model complexes with hydrotris(pyrazolyl)borate.

Authors: Yuki Matsunaga; Kiyoshi Fujisawa; Naoko Ibi; Yoshitaro Miyashita; Ken-ichi Okamoto
Journal: Inorg Chem Date: 2005-01-24 Impact factor: 5.165

4. Catalytic reduction of dinitrogen to ammonia at a single molybdenum center.

Authors: Richard R Schrock
Journal: Acc Chem Res Date: 2005-12 Impact factor: 22.384

5. Catalytic C-H bond amination from high-spin iron imido complexes.

Authors: Evan R King; Elisabeth T Hennessy; Theodore A Betley
Journal: J Am Chem Soc Date: 2011-03-15 Impact factor: 15.419

6. Reduction of N2 to ammonia and hydrazine utilizing H2 as the reductant.

Authors: John D Gilbertson; Nathaniel K Szymczak; David R Tyler
Journal: J Am Chem Soc Date: 2005-07-27 Impact factor: 15.419

7. On the feasibility of N2 fixation via a single-site FeI/FeIV cycle: Spectroscopic studies of FeI(N2)FeI, FeIV[triple bond]N, and related species.

Authors: Michael P Hendrich; William Gunderson; Rachel K Behan; Michael T Green; Mark P Mehn; Theodore A Betley; Connie C Lu; Jonas C Peters
Journal: Proc Natl Acad Sci U S A Date: 2006-11-07 Impact factor: 11.205

8. Mechanism of the iron-mediated alkene aziridination reaction: experimental and computational investigations.

Authors: Katie L Klotz; Luke M Slominski; Miranda E Riemer; James A Phillips; Jason A Halfen
Journal: Inorg Chem Date: 2009-02-02 Impact factor: 5.165

9. Dinitrogen chemistry from trigonally coordinated iron and cobalt platforms.

Authors: Theodore A Betley; Jonas C Peters
Journal: J Am Chem Soc Date: 2003-09-10 Impact factor: 15.419

10. Terminal FeI-N2 and FeII...H-C interactions supported by tris(phosphino)silyl ligands.

Authors: Neal P Mankad; Matthew T Whited; Jonas C Peters
Journal: Angew Chem Int Ed Engl Date: 2007 Impact factor: 15.336

36 in total

1. Low-temperature N2 binding to two-coordinate L2Fe(0) enables reductive trapping of L2FeN2(-) and NH3 generation.

Authors: Gaël Ung; Jonas C Peters
Journal: Angew Chem Int Ed Engl Date: 2014-11-13 Impact factor: 15.336

Review 2. Catalytic N₂-to-NH₃ (or -N₂H₄) Conversion by Well-Defined Molecular Coordination Complexes.

Authors: Matthew J Chalkley; Marcus W Drover; Jonas C Peters
Journal: Chem Rev Date: 2020-04-30 Impact factor: 60.622

3. Catalytic reduction of N2 to NH3 by an Fe-N2 complex featuring a C-atom anchor.

Authors: Sidney E Creutz; Jonas C Peters
Journal: J Am Chem Soc Date: 2014-01-09 Impact factor: 15.419

Review 4. Biosynthesis of nitrogenase metalloclusters.

Authors: Markus W Ribbe; Yilin Hu; Keith O Hodgson; Britt Hedman
Journal: Chem Rev Date: 2013-12-13 Impact factor: 60.622

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

Authors: Sean F McWilliams; Eckhard Bill; Gudrun Lukat-Rodgers; Kenton R Rodgers; Brandon Q Mercado; Patrick L Holland
Journal: J Am Chem Soc Date: 2018-06-29 Impact factor: 15.419

6. Alkali-Controlled C-H Cleavage or N-C Bond Formation by N2-Derived Iron Nitrides and Imides.

Authors: K Cory MacLeod; Fabian S Menges; Sean F McWilliams; Stephanie M Craig; Brandon Q Mercado; Mark A Johnson; Patrick L Holland
Journal: J Am Chem Soc Date: 2016-08-29 Impact factor: 15.419

Review 7. Nitrogenase and homologs.

Authors: Yilin Hu; Markus W Ribbe
Journal: J Biol Inorg Chem Date: 2014-12-10 Impact factor: 3.358

N2 functionalization at iron metallaboratranes.

1. Nitrogenase MoFe-protein at 1.16 A resolution: a central ligand in the FeMo-cofactor.

2. Structure and bonding in three-coordinate N-heterocyclic carbene adducts of iron(II) bis(trimethylsilyl)amide.

3. Structural and spectroscopic characterization of first-row transition metal(II) substituted blue copper model complexes with hydrotris(pyrazolyl)borate.

4. Catalytic reduction of dinitrogen to ammonia at a single molybdenum center.

5. Catalytic C-H bond amination from high-spin iron imido complexes.

6. Reduction of N2 to ammonia and hydrazine utilizing H2 as the reductant.

7. On the feasibility of N2 fixation via a single-site FeI/FeIV cycle: Spectroscopic studies of FeI(N2)FeI, FeIV[triple bond]N, and related species.

8. Mechanism of the iron-mediated alkene aziridination reaction: experimental and computational investigations.

9. Dinitrogen chemistry from trigonally coordinated iron and cobalt platforms.

10. Terminal FeI-N2 and FeII...H-C interactions supported by tris(phosphino)silyl ligands.

1. Low-temperature N2 binding to two-coordinate L2Fe(0) enables reductive trapping of L2FeN2(-) and NH3 generation.

Review 2. Catalytic N₂-to-NH₃ (or -N₂H₄) Conversion by Well-Defined Molecular Coordination Complexes.

3. Catalytic reduction of N2 to NH3 by an Fe-N2 complex featuring a C-atom anchor.

Review 4. Biosynthesis of nitrogenase metalloclusters.

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

6. Alkali-Controlled C-H Cleavage or N-C Bond Formation by N2-Derived Iron Nitrides and Imides.

Review 7. Nitrogenase and homologs.

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

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

10. A Triad of Highly Reduced, Linear Iron Nitrosyl Complexes: {FeNO}(8-10).

Review 2. Catalytic N2-to-NH3 (or -N2H4) Conversion by Well-Defined Molecular Coordination Complexes.

Review 4. Biosynthesis of nitrogenase metalloclusters.

Review 7. Nitrogenase and homologs.

Review 2. Catalytic N₂-to-NH₃ (or -N₂H₄) Conversion by Well-Defined Molecular Coordination Complexes.