Nuclear resonance vibrational spectroscopic and computational study of high-valent diiron complexes relevant to enzyme intermediates

Kiyoung Park, Caleb B. Bell, Lei V. Liu, Dong Wang, Genqiang Xue, Yeonju Kwak, Shaun D. Wong, Kenneth M. Light, Jiyong Zhao, E. Ercan Alp, Yoshitaka Yoda, Makina Saito, Yasuhiro Kobayashi, Takehiro Ohta, Makoto Seto, Lawrence Que, Edward I. Solomon

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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.

Original languageEnglish (US)
Pages (from-to)6275-6280
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume110
Issue number16
DOIs
StatePublished - Apr 16 2013

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    Park, K., Bell, C. B., Liu, L. V., Wang, D., Xue, G., Kwak, Y., Wong, S. D., Light, K. M., Zhao, J., Alp, E. E., Yoda, Y., Saito, M., Kobayashi, Y., Ohta, T., Seto, M., Que, L., & Solomon, E. I. (2013). Nuclear resonance vibrational spectroscopic and computational study of high-valent diiron complexes relevant to enzyme intermediates. Proceedings of the National Academy of Sciences of the United States of America, 110(16), 6275-6280. https://doi.org/10.1073/pnas.1304238110