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In situ surface-enhanced Raman scattering (SERS) spectroscopy is used to identify the key reaction intermediates during the plasma-based removal of NO and SO2 under dry and wet conditions on Ag nanoparticles. Density functional theory (DFT) calculations are used to confirm the experimental observations by calculating the vibrational modes of the surface-bound intermediate species. Here, we provide spectroscopic evidence that the wet plasma increases the SO2 and the NOx removal through the formation of highly reactive OH radicals, drivin