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The mode of operation of titania-supported vanadia (VOₓ) catalysts for NOx abatement using ammonia selective catalytic reduction (NH₃-SCR) is still vigorously debated. We introduce a new high surface area VOₓ/TiO₂/SBA-15 model catalyst system based on mesoporous silica SBA-15 making use of atomic layer deposition (ALD) for controlled synthesis of titania and vanadia multilayers. The bulk and surface structure is characterized by X-ray diffraction (XRD), UV-vis and Raman spectroscopy, as well as X-ray photoelectron spectroscopy (XPS), revealing the presence of dispersed surface VOx species on amorphous TiO₂ domains on SBA-15, forming hybrid Si–O–V and Ti–O–V linkages. Temperature-dependent analysis of the ammonia SCR catalytic activity reveals NOx conversion levels of up to ~60%. In situ and operando diffuse reflection IR Fourier transform (DRIFT) spectroscopy shows N–Hstretching modes, representing adsorbed ammonia and -NH₂ and -NH intermediate structures on Bronsted and Lewis acid sites. Partial Lewis acid sites with adjacent redox sites are proposed as the active sites and desorption of product molecules as the rate-determining step at low temperature. The high NOₓ conversion is attributed to the presence of highly dispersed VOₓ species and the moderate acidity of VOₓ supported on TiO₂/SBA-15.