This work demonstrates a two-step gram-scale synthesis of presynthesized silver (Ag) nanoparticles impregnated with mesoporous TiO 2 and evaluates their feasibility for wastewater treatment and hydrogen gas generation under natural sunlight. Paracetamol was chosen as the model pharmaceutical pollutant for evaluating photocatalytic performance. A systematic material analysis (morphology, chemical environment, optical bandgap energy) of the Ag/TiO 2 photocatalyst powder was carried out, and the influence of material properties on the performance is discussed in detail. The experimental results showed that the decoration of anatase TiO 2 nanoparticles (size between 80 and 100 nm) with 5 nm Ag nanoparticles (1 wt %) induced visible-light absorption and enhanced charge carrier separation. As a result, 0.01 g/L Ag/TiO 2 effectively removed 99% of 0.01 g/L paracetamol in 120 min and exhibited 60% higher photocatalytic removal than pristine TiO 2 . Alongside paracetamol degradation, Ag/TiO 2 led to the generation of 1729 μmol H 2 g −1 h −1 . This proof-of-concept approach for tandem pollutant degradation and hydrogen generation was further evaluated with rare earth metal (lanthanum)-and nonmetal (nitrogen)-doped TiO 2 , which also showed a positive response. Using a combination of ab initio calculations and our new theory model, we revealed that the enhanced photocatalytic performance of Ag/TiO 2 was due to the surface Fermi-level change of TiO 2 and lowered surface reaction energy barrier for water pollutant oxidation. This work opens new opportunities for exploiting tandem photocatalytic routes beyond water splitting and understanding the simultaneous reactions in metal-doped metal oxide photocatalyst systems under natural sunlight.
Mesoporous cobalt oxide was investigated for the liquid phase oxidation of cyclohexene using tertiobutylhydroperoxide (TBHP) as an oxidant. The results were compared with several series of supported cobalt catalysts to study the influence of the cobalt loading and solvents on the overall conversion and selectivity. Mesoporous cobalt was synthesized through the nanocasting route using siliceous SBA-15 mesoporous material as a hard template and cobalt nitrate as the cobalt oxide precursor. Supported cobalt oxide catalysts (Co/MxOy) were synthesized by the impregnation method using two loadings (1 and 5 wt.%) and Al2O3, TiO2, and ZrO2 as supports. Samples were characterised by means: elemental analysis, X-ray powder Diffraction (XRD), BET (surface area), UV-Vis DR Spectroscopy, and Transmission Electron Microscopy (TEM). The results obtained showed that the cobalt oxide retains the mesoporous structure of SBA-15, and in all Co/MxOy, crystalline Co3O4, and CoO phases are observed. The mesoporous cobalt oxide is more active than the supported cobalt catalysts in the allylic oxidation of cyclohexene, with a conversion of 78 % of cyclohexene and 43.3 % selectivity toward 2-cyclohexene-1-ol. The highest activity of mesoporous cobalt oxide could be ascribed to its largest surface area. Furthermore, Co3O4 has both Lewis and Brönsted acidic sites whereas Co/MxOy has only Lewis acidic sites, which could also explain its superior catalytic activity. Moreover, mesoporous cobalt oxide was more stable than supported cobalt catalysts. Therefore, this catalyst is promising for allylic oxidation of alkenes.
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