The Influence of Au Loading and TiO2 Support on the Catalytic Wet Air Oxidation of Glyphosate over TiO2+Au Catalysts

Abstract

This study aimed to explore the impact of varying amounts of added Au (0.5 to 2 wt.%) and the structural characteristics of anatase TiO2 supports (nanoparticles (TP, SBET = 88m2/g) and nanorods (TR, SBET = 105 m2/g)) on the catalytic efficiency of TiO2+Au catalysts in eliminating the herbicide glyphosate from aqueous solutions via the catalytic wet air oxidation (CWAO) process. The investigation was conducted using a continuous-flow trickle-bed reactor. Regardless of the TiO2 support and the amount of Au added, the addition of Au has a positive effect on the glyphosate degradation rate. Regarding the amount of Au added, the highest catalytic activity was observed with the TP + 1% Au catalyst, which had a higher Schottky barrier (SB) than the TP + 2% Au catalyst, which helped the charge carriers in the TiO2 conduction band to increase their reduction potential by preventing them from returning to the Au. The role of glyphosate degradation product adsorption on the catalyst surface is crucial for sustaining the long-term catalytic activity of the investigated TiO2+Au materials. This was particularly evident in the case of the TR + 1% Au catalyst, which had the highest glyphosate degradation rate at the beginning of the CWAO experiment, but its catalytic activity then decreased over time due to the adsorption of glyphosate degradation products, which was favoured by the presence of strong acidic sites. In addition, the TR + 1% Au solid had the smallest average Au particle size of all analyzed materials, which were more easily deactivated by the adsorption of glyphosate degradation products. The analysis of the degradation products of glyphosate shows that the oxidation of glyphosate in the liquid phase involves the rupture of C–P and C–N bonds, as amino-methyl-phosphonic acid (AMPA), glyoxylic acid and sarcosine were detected.