Based on the 2019 report of the European Environment Agency on Air Quality in Europe nitrogen oxides (NOx) were identified as the most harmful air pollutants in terms of damage to ecosystems. Moreover, in Europe, NO2 is pinpointed as one of the most dangerous pollutants for human health. Anthropogenic emissions of NOx are mainly generated by the combustion of fossil fuels. Nitrogen oxides being emitted into the atmosphere cause environmental problems such as acid rain, acidification of soil, lakes and rivers, eutrophication and photochemical smog. The most effective and widely applicable technology to date for the purification of flue gases from NOx is selective catalytic reduction using ammonia (NH3-SCR de-NOx). Nowadays, one of the most significant research fields in NH3-SCR de-NOx is the application of unconventional reduction methods and the preparation of novel catalysts possessing high specific surface area, uniformity, dispersion of active sites, activity and selectivity. Atomic layer deposition (ALD) is an attractive technique for the deposition of uniformly distributed active catalytic layers, or nanoparticles, on highly porous substrates characterized by a complex structure. For this type of materials, conventional catalyst preparation methods (e.g., impregnation or deposition precipitation) can encounter several limitations. The significant advantage of ALD for the preparation of supported catalysts is that the process can be controlled on the atomic scale, providing the required thickness of an active layer, synthesized with a sub-nm accuracy. Moreover, ALD ensures the formation of catalytic sites from the gas phase, which enhances the possibility of active species being deposited inside pores which are very small in size. In this study, ALD was applied to the preparation of VxOy-based NH3-SCR de-NOx catalysts. Highly porous silica gel powder (63–100 μm) with a specific surface area of up to 450 m2·g−1 was used as a substrate for VxOy/SiO2 with different metal loadings (wt.%). In addition (VxOy+TiO2)/SiO2 catalysts were prepared by applying vanadium (V) tri-i-propoxy oxide (VTIP) and titanium tetrachloride (TiCl4) as precursors with deionized water as the co-reactant. Elemental analysis (ICP-OES) revealed that vanadium loadings of the VxOy/SiO2 catalysts were 0.3, 0.7, 1.1 and 1.60 wt.%, while the loadings in the TiO2-promoted VxOy/SiO2 catalyst were 1.0 and 0.2 wt.% for V and Ti, respectively. The obtained XPS spectra indicated the presence of V2O3 and V2O5 species (V2O5/V2O3 ratio was 1.6 and 6.3 for the as-synthesized and calcined samples respectively). Vanadium(V) oxide is known to be a catalytically active compound for NH3-SCR de-NOx. Additionally, TEM, XRD and N2 adsorption (BET) analyses were conducted to provide a comprehensive characterization of the species size, crystalline phase and porosity of the catalysts prepared.
Novel Catalysts for Selective Catalytic Reduction of NOx by NH3 Prepared by Atomic Layer Deposition of V and Ti Oxides on SiO2 Powder