Hydrogen abstraction reactions of the ferryl [FeO](2+) moiety are investigated theoretically using a simple molecular model (OH)(2)FeO by DFT methods. Obtained thermochemical and structural data are compared with high-level electron-correlated methods: CCSD(T), BD and MCQDPT2. Two bonding patterns are observed: triple oxo-iron bond Fe*equivalent to 0* and single Fe-O-center dot bond with radical oxygen. Predicted thermochemistry and reactivity with H-2 and CH4 molecules for the later one fits well with available experimental data on the N2O + FeZSM5 catalytic system. (c) 2015 Elsevier B.V. All rights