In this paper, we report the investigation of the reaction of adsorbed NH and N with styrene on Ag(110) using temperature-programmed reaction spectroscopy. Using O2 and NH3 as the starting reagents, NH and N species were deposited on a Ag surface. The reaction of styrene on NH- and N-covered Ag surface appears to yield 2-phenylaziridine and benzonitrile, with additional products HCN and NH3. The formation of aziridine, the nitrogenous analogue of styrene epoxide, is proposed to be due to the cycloaddition of adsorbed NH to the carbon-carbon double bond. These results suggest that Ag-based heterogeneous catalysts may be useful for the aziridination of olefins.