Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 41, Pages 17125-17137Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja306526d
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Funding
- U.S. National Science Foundation
- Deutsche Forschungsgemeinschaft
- Department of Chemistry and Chemical Biology at Cornell University
- Max Planck Society
- Sloan Foundation
- ACS Petroleum Research Fund Grant [50270-DN18]
- National Institute of General Medical Sciences [T32GM008500]
- Natural Sciences and Engineering Research Council of Canada
- National Science Foundation and the National Institutes of Health/National Institute of General Medical Sciences under NSF [DMR-0936384]
- DOE
- BER
- NIH
- NCRR
- BMTP
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1026084] Funding Source: National Science Foundation
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Addition of biphenylene to the bis(imino)pyridine iron dinitrogen complexes, ((PDI)-P-iPr)Fe(N-2)(2) and [((PDI)-P-Me)Fe(N-2))(2)(mu(2)-N-2) ((PDI)-P-R = 2,6-(2,6-R-2-C6H3- N=CMe)(2)C5H3N; R = Me, Pr-i), resulted in oxidative addition of a C C bond at ambient temperature to yield the corresponding iron biphenyl compounds, ((PDI)-P-R)Fe(biphenyl). The molecular structures of the resulting bis(imino)pyridine iron metallacycles were established by X-ray diffraction and revealed idealized square pyramidal geometries. The electronic structures of the compounds were studied by Mossbauer spectroscopy, NMR spectroscopy, magnetochemistry, and X-ray absorption and X-ray emission spectroscopies. The experimental data, in combination with broken-symmetry density functional theory calculations, established spin crossover (low to intermediate spin) ferric compounds antiferromagnetically coupled to bis(imino)pyridine radical anions. Thus, the overall oxidation reaction involves cooperative electron loss from both the iron center and the redox-active bis(imino)pyridine ligand.
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