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Unprecedented Five-Coordinate Iron(IV) Imides Generate Divergent Spin States Based on the Imide R-Groups.

ABSTRACT: Three five-coordinate iron(IV) imide complexes have been synthesized and characterized. These novel structures have disparate spin states on the iron as a function of the R-group attached to the imide, with alkyl groups leading to low-spin diamagnetic (S=0) complexes and an aryl group leading to an intermediate-spin (S=1) complex. The different spin states lead to significant differences in the bonding about the iron center as well as the spectroscopic properties of these complexes. Mössbauer spectroscopy confirmed that all three imide complexes are in the iron(IV) oxidation state. The combination of diamagnetism and 15 N labeling allowed for the first 15 N NMR resonance recorded on an iron imide. Multi-reference calculations corroborate the experimental structural findings and suggest how the bonding is distinctly different on the imide ligand between the two spin states.

SUBMITTER: Anneser MR 

PROVIDER: S-EPMC6546507 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

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Unprecedented Five-Coordinate Iron(IV) Imides Generate Divergent Spin States Based on the Imide R-Groups.

Anneser Markus R MR   Elpitiya Gaya R GR   Townsend Jacob J   Johnson Elizabeth J EJ   Powers Xian B XB   DeJesus Joseph F JF   Vogiatzis Konstantinos D KD   Jenkins David M DM  

Angewandte Chemie (International ed. in English) 20190507 24

Three five-coordinate iron(IV) imide complexes have been synthesized and characterized. These novel structures have disparate spin states on the iron as a function of the R-group attached to the imide, with alkyl groups leading to low-spin diamagnetic (S=0) complexes and an aryl group leading to an intermediate-spin (S=1) complex. The different spin states lead to significant differences in the bonding about the iron center as well as the spectroscopic properties of these complexes. Mössbauer sp  ...[more]

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