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Not Limited to Iron: A Cobalt Heme–NO Model Facilitates N–N Coupling with External NO in the Presence of a Lewis Acid to Generate N ₂ O

https://doi.org/10.1002/anie.201909137

Abucayon, Erwin G.; Khade, Rahul L.; Powell, Douglas R.; Zhang, Yong; Richter‐Addo, George B. (October 2019, Angewandte Chemie International Edition)

Abstract Some bacterial heme proteins catalyze the coupling of two NO molecules to generate N₂O. We previously reported that a heme Fe–NO model engages in this N−N bond‐forming reaction with NO. We now demonstrate that (OEP)Co^II(NO) similarly reacts with 1 equiv of NO in the presence of the Lewis acids BX₃(X=F, C₆F₅) to generate N₂O. DFT calculations support retention of the Co^IIoxidation state for the experimentally observed adduct (OEP)Co^II(NO⋅BF₃), the presumed hyponitrite intermediate (P^.+)Co^II(ONNO⋅BF₃), and the porphyrin π‐radical cation by‐product of this reaction, and that the π‐radical cation formation likely occurs at the hyponitrite stage. In contrast, the Fe analogue undergoes a ferrous‐to‐ferric oxidation state conversion during this reaction. Our work shows that cobalt hemes are chemically competent to engage in the NO‐to‐N₂O conversion reaction.
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Unusual monodentate binding of a C-NONOate ligand in the nitrosyl complex (OEP)Ru(NO)(η1-ONN(t-Bu)O)

https://doi.org/10.1016/j.ica.2020.119567

Xu, Nan; Bevak, Alexander; Roesch, Joseph; Armstrong, Bernadette; Abucayon, Erwin; Bell, Zachary; Powell, Douglas R.; Richter-Addo, George B. (July 2020, Inorganica Chimica Acta)

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Interactions of acetamide and acrylamide with heme models: Synthesis, infrared spectra, and solid state molecular structures of five- and six-coordinate ferric porphyrin derivatives

https://doi.org/10.1016/j.jinorgbio.2019.03.003

Xu, Nan; Guan, Ye; Nguyen, Nhi; Lingafelt, Colin; Powell, Douglas R.; Richter-Addo, George B. (May 2019, Journal of Inorganic Biochemistry)

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