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[en] Highlights: • N2-adsorption on copper cluster cations was studied by mass spectrometry. • A pulsed magnetron sputtering in aggregation cell was used to form Cun+. • The N2-adsorption reactivity of Cun+ decreased rapidly with n = 6–10. • A correlation between observed reactivity and calculated binding energy was found. We have observed gas-phase reactions between N2 molecules and copper cluster cations, Cun+ (n = 2–17), formed by a modulated pulsed power magnetron sputtering cluster ion source. By introducing N2 gas effusively between the source and an acceleration region of a time-of-flight mass spectrometer in the vacuum chamber, N2-adsorbed copper cluster cations, CunN2+, were observed in mass spectra. The N2-adsorption reactivity of Cun+ was found to be relatively lower at n ≥ 10 than at the smaller n. The cluster-size dependence of N2-adsorption on Cun+ has a correlation with binding energies between Cun+ and N2 calculated by density functional theory.