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Comparative electronic structures of nitrogenase FeMoco and FeVco

Comparative electronic structures of nitrogenase FeMoco and FeVco


Titill: Comparative electronic structures of nitrogenase FeMoco and FeVco
Höfundur: Rees, Julian A.
Bjornsson, Ragnar   orcid.org/0000-0003-2167-8374
Kowalska, Joanna K.
Lima, Frederico A.
Schlesier, Julia
Sippel, Daniel
Weyhermüller, Thomas
Einsle, Oliver
Kovacs, Julie A.
DeBeer, Serena
Útgáfa: 2017
Tungumál: Enska
Umfang: 2445-2455
Háskóli/Stofnun: Háskóli Íslands
University of Iceland
Svið: Verkfræði- og náttúruvísindasvið (HÍ)
School of Engineering and Natural Sciences (UI)
Deild: Raunvísindastofnun (HÍ)
Science Institute (UI)
Raunvísindadeild (HÍ)
Faculty of Physical Sciences (UI)
Birtist í: Dalton Transactions;46(8)
DOI: 10.1039/C7DT00128B
Efnisorð: Inorganic Chemistry; Ólífræn efnafræði; Spectroscopy; Litrófsgreining; Efnasambönd
URI: https://hdl.handle.net/20.500.11815/520

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Tilvitnun:

Rees, J. A., Bjornsson, R., Kowalska, J. K., Lima, F. A., Schlesier, J., Sippel, D., . . . DeBeer, S. (2017). Comparative electronic structures of nitrogenase FeMoco and FeVco. Dalton Transactions, 46(8), 2445-2455. doi:10.1039/C7DT00128B

Útdráttur:

An investigation of the active site cofactors of the molybdenum and vanadium nitrogenases (FeMoco and FeVco) was performed using high-resolution X-ray spectroscopy. Synthetic heterometallic iron–sulfur cluster models and density functional theory calculations complement the study of the MoFe and VFe holoproteins using both non-resonant and resonant X-ray emission spectroscopy. Spectroscopic data show the presence of direct iron–heterometal bonds, which are found to be weaker in FeVco. Furthermore, the interstitial carbide is found to perturb the electronic structures of the cofactors through highly covalent Fe–C bonding. The implications of these conclusions are discussed in light of the differential reactivity of the molybdenum and vanadium nitrogenases towards various substrates. Possible functional roles for both the heterometal and the interstitial carbide are detailed.

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