Literature DB >> 33830763

Dinitrogen Insertion and Cleavage by a Metal-Metal Bonded Tricobalt(I) Cluster.

Mary C Eaton1, Vincent J Catalano2, Jason Shearer3, Leslie J Murray1.   

Abstract

Reduction of a tricobalt(II) tri(bromide) cluster supported by a tris(β-diketiminate) cyclophane results in halide loss, ligand compression, and metal-metal bond formation to yield a 48-electron CoI3 cluster, Co3LEt/Me (2). Upon reaction of 2 with dinitrogen, all metal-metal bonds are broken, steric conflicts are relaxed, and dinitrogen is incorporated within the internal cavity to yield a formally (μ3-η1:η2:η1-dinitrogen)tricobalt(I) complex, 3. Broken symmetry DFT calculations (PBE0/def2-tzvp/D3) support an N-N bond order of 2.1 in the bound N2 with the calculated N-N stretching frequency (1743 cm-1) comparable to the experimental value (1752 cm-1). Reduction of 3 under Ar in the presence of Me3SiBr results in N2 scission with tris(trimethylsilyl)amine afforded in good yield.

Entities:  

Year:  2021        PMID： 33830763      PMCID： PMC8247452          DOI： 10.1021/jacs.1c01840

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


  18 in total

1.  Stepwise reduction of dinitrogen bond order by a low-coordinate iron complex.

Authors:  J M Smith; R J Lachicotte; K A Pittard; T R Cundari; G Lukat-Rodgers; K R Rodgers; P L Holland
Journal:  J Am Chem Soc       Date:  2001-09-19       Impact factor: 15.419

2.  Staggered to eclipsed conformational rearrangement of [Co2(CO)6(PPh3)2] in the solid state: an X-ray diffraction study at high pressure and low temperature.

Authors:  Nicola Casati; Piero Macchi; Angelo Sironi
Journal:  Angew Chem Int Ed Engl       Date:  2005-12-02       Impact factor: 15.336

3.  Predicting catalysis: understanding ammonia synthesis from first-principles calculations.

Authors:  A Hellman; E J Baerends; M Biczysko; T Bligaard; C H Christensen; D C Clary; S Dahl; R van Harrevelt; K Honkala; H Jonsson; G J Kroes; M Luppi; U Manthe; J K Nørskov; R A Olsen; J Rossmeisl; E Skúlason; C S Tautermann; A J C Varandas; J K Vincent
Journal:  J Phys Chem B       Date:  2006-09-14       Impact factor: 2.991

4.  Splendid symmetry: crystallization of an unbridged isomer of Co2(CO)8 in Co2(CO)8.C60.

Authors:  Thelma Y Garcia; James C Fettinger; Marilyn M Olmstead; Alan L Balch
Journal:  Chem Commun (Camb)       Date:  2009-10-29       Impact factor: 6.222

5.  Ammonia synthesis from first-principles calculations.

Authors:  K Honkala; A Hellman; I N Remediakis; A Logadottir; A Carlsson; S Dahl; C H Christensen; J K Nørskov
Journal:  Science       Date:  2005-01-28       Impact factor: 47.728

6.  Catalytic silylation of dinitrogen with a dicobalt complex.

Authors:  Randall B Siedschlag; Varinia Bernales; Konstantinos D Vogiatzis; Nora Planas; Laura J Clouston; Eckhard Bill; Laura Gagliardi; Connie C Lu
Journal:  J Am Chem Soc       Date:  2015-04-06       Impact factor: 15.419

7.  Synthesis, crystal structure and hydroformylation activity of triphenylphosphite modified cobalt catalysts.

Authors:  Marco Haumann; Reinout Meijboom; John R Moss; Andreas Roodt
Journal:  Dalton Trans       Date:  2004-05-10       Impact factor: 4.390

8.  Mimicking the Constrained Geometry of a Nitrogen-Fixation Intermediate.

Authors:  Tianchang Liu; Michael R Gau; Neil C Tomson
Journal:  J Am Chem Soc       Date:  2020-04-21       Impact factor: 15.419

9.  Unusual Dinitrogen Binding and Electron Storage in Dinuclear Iron Complexes.

Authors:  Dieter Sorsche; Matthias E Miehlich; Keith Searles; Guillaume Gouget; Eva M Zolnhofer; Skye Fortier; Chun-Hsing Chen; Michael Gau; Patrick J Carroll; Christopher B Murray; Kenneth G Caulton; Marat M Khusniyarov; Karsten Meyer; Daniel J Mindiola
Journal:  J Am Chem Soc       Date:  2020-04-21       Impact factor: 15.419

10.  Heterogeneous Fe3 single-cluster catalyst for ammonia synthesis via an associative mechanism.

Authors:  Jin-Cheng Liu; Xue-Lu Ma; Yong Li; Yang-Gang Wang; Hai Xiao; Jun Li
Journal:  Nat Commun       Date:  2018-04-23       Impact factor: 14.919
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  1 in total

1.  Combining metal-metal cooperativity, metal-ligand cooperativity and chemical non-innocence in diiron carbonyl complexes.

Authors:  Cody B van Beek; Nicolaas P van Leest; Martin Lutz; Sander D de Vos; Robertus J M Klein Gebbink; Bas de Bruin; Daniël L J Broere
Journal:  Chem Sci       Date:  2022-01-18       Impact factor: 9.825
  1 in total

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