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Vanadium-based catalysts play a pivotal role in the emission control of industrial NO
via selective catalytic reduction (SCR) technology. However, little attention has been paid to the potential emission of greenhouse gas N
O under complex working conditions. This work reports that a commercial V
O
/TiO
catalyst may lead to significant N
O emission without greatly changing the outlet NO
concentration after chromium (Cr) deposition. With a Cr loading of 2 wt %, N
O concentration increased from 27.8 to 199.2 ppm at 350 °C with the value of outlet N
O/(N
O+N
) from 2.5% to 19.4%. Experimental results combined with DFT+U calculations suggest that nonselective catalytic reduction (NSCR) is the main route for N
O 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 V
O
/TiO
surface accelerates the conversion of V
+ Cr
→ V
+ Cr
, leading to a larger proportion of surface V
. More importantly, surface V
is highly related to the redox property of the V
O
/TiO
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 NH
-SCR process, monitoring N
O emission should be included along with the NO
concentrations, especially in complex flue gases.