Lewis Acid Activation of the Ferrous Heme-NO Fragment toward the N-N Coupling Reaction with NO to Generate N2O

Erwin G. Abucayon, Rahul L. Khade, Douglas R. Powell, Yong Zhang, George B. Richter-Addo

Research output: Contribution to journalArticlepeer-review

25 Scopus citations

Abstract

Bacterial NO reductase (bacNOR) enzymes utilize a heme/non-heme active site to couple two NO molecules to N2O. We show that BF3 coordination to the nitrosyl O-atom in (OEP)Fe(NO) activates it toward N-N bond formation with NO to generate N2O. 15N-isotopic labeling reveals a reversible nitrosyl exchange reaction and follow-up N-O bond cleavage in the N2O formation step. Other Lewis acids (B(C6F5)3 and K+) also promote the NO coupling reaction with (OEP)Fe(NO). These results, complemented by DFT calculations, provide experimental support for the cis:b3 pathway in bacNOR.

Original languageEnglish
Pages (from-to)4204-4207
Number of pages4
JournalJournal of the American Chemical Society
Volume140
Issue number12
DOIs
StatePublished - 28 Mar 2018

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