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Thus, the current protocol can be considered as a simpler, reproducible, and environmentally benign approach for N-methylation of amines.This work employs double-hybrid density functionals to re-examine the CO-NO bond dissociation mechanism of nitrite isomer of 1,1-diamino-2,2-dinitro-ethylene (DADNE) into (NH2)2C=C(NO2)O and nitric monoxide (NO). The calculated results confirm that an activated barrier is present in the CO-NO bond dissociation process of (NH2)2C=C(NO2)(ONO). Furthermore, it is proposed that a radical-radical adduct is