Enhanced adsorption and degradation of methylene blue over mixed niobium-cerium oxide – Unraveling the synergy between Nb and Ce in advanced oxidation processes

Abstract

Formation of reactive oxygen species (ROS) via H₂O₂ activation is of vital importance in catalytic environmental chemistry, especially in degradation of organic pollutants. A new mixed niobium-cerium oxide (NbCeO_x) was tailored for this purpose. A thorough structural and chemical characterization of NbCeO_x along with CeO₂ and Nb₂O₅ reference materials was carried out using TEM/STEM/EDS, SEM, XRD, XPS, EPR, UV-vis and N₂ physisorption. The ability of the catalysts to activate H₂O₂ towards ROS formation was assessed on the basis of EPR and Raman measurements. Catalytic activity of the oxides was evaluated in degradation of methylene blue (MB) as a model pollutant. Very high activity of NbCeO_x was attributed to the mixed redox-acidic nature of its surface, which originated from the synergy between Nb and Ce species. These two properties (redox activity and acidity) ensured convenient conditions for efficient activation of H₂O₂ and degradation of MB. The activity of NbCeO_x in MB degradation was found 3 times higher than that of the commercial Nb₂O₅ CBMM catalyst and 240 times higher than that of CeO₂. The mechanism of the degradation reaction was found to be an adsorption-triggered process initiated by hydroxyl radicals, generated on the surface via the transformation of O₂^-•/O₂^2-.