Abstract:
:High-valent intermediates of binuclear nonheme iron enzymes are structurally unknown despite their importance for understanding enzyme reactivity. Nuclear resonance vibrational spectroscopy combined with density functional theory calculations has been applied to structurally well-characterized high-valent mono- and di-oxo bridged binuclear Fe model complexes. Low-frequency vibrational modes of these high-valent diiron complexes involving Fe motion have been observed and assigned. These are independent of Fe oxidation state and show a strong dependence on spin state. It is important to note that they are sensitive to the nature of the Fe2 core bridges and provide the basis for interpreting parallel nuclear resonance vibrational spectroscopy data on the high-valent oxo intermediates in the binuclear nonheme iron enzymes.
journal_name
Proc Natl Acad Sci U S Aauthors
Park K,Bell CB 3rd,Liu LV,Wang D,Xue G,Kwak Y,Wong SD,Light KM,Zhao J,Alp EE,Yoda Y,Saito M,Kobayashi Y,Ohta T,Seto M,Que L Jr,Solomon EIdoi
10.1073/pnas.1304238110subject
Has Abstractpub_date
2013-04-16 00:00:00pages
6275-80issue
16eissn
0027-8424issn
1091-6490pii
1304238110journal_volume
110pub_type
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