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Vanadium-based catalysts play a pivotal role in the emission control of industrial NO x via selective catalytic reduction (SCR) technology. However, little attention has been paid to the potential emission of greenhouse gas N2O under complex working conditions. This work reports that a commercial V2O5/TiO2 catalyst may lead to significant N2O emission without greatly changing the outlet NO x concentration after chromium (Cr) deposition. With a Cr loading of 2 wt %, N2O concentration increased from 27.8 to 199.2 ppm at 350 °C with the value of outlet N2O/(N2O+N2) from 2.5% to 19.4%. Experimental results combined with DFT+U calculations suggest that nonselective catalytic reduction (NSCR) is the main route for N2O formation in a wide temperature range of 250 ∼ 400 °C. It is stemmed from the fact that the covalent interaction between Cr and V species on the V2O5/TiO2 surface accelerates the conversion of V4+ + Cr6+ → V5+ + Cr3+, leading to a larger proportion of surface V5+. More importantly, surface V5+ is highly related to the redox property of the V2O5/TiO2 catalyst, which is beneficial to NSCR reaction rather than the standard SCR process. The work suggests that to better inhibit the emission of greenhouse gases during the NH3–SCR process, monitoring N2O emission should be included along with the NO x concentrations, especially in complex flue gases.