Influence of relative humidity on the photocatalytic oxidation (PCO) of toluene by TiO2 loaded on activated carbon fibers: PCO rate and intermediates accumulation

摘要

Photocatalytic oxidation (PCO) tests were carried out for toluene adsorbed on the activated carbon fibers (ACFs)-supported TiO2 photocatalyst in an environmental condition controlled chamber TiO2/ACF catalyst was made and characterized by N2 adsorption isotherm for pore structure and scanning electron microscopy (SEM) for morphology, respectively. Through exploring the remnant of toluene and the accumulation of intermediates on the TiO2/ACF catalyst including species, amount and their change processes under different relative humidity (RH), this study aimed to explore the influence of RH on the PCO of toluene and the roles of water vapor in the PCO process: PCO reaction paths and the accumulation of intermediates on the TiO2/ACF catalyst. Results showed that (1) with the increase of RH in the chamber (15%, 30%, 45% and 60%) the PCO conversion rate of toluene was positive correlated and no catalyst deactivation was observed under all RH levels; (2) during the gas-solid PCO process of toluene, byproducts of aromatic ring oxidation including 2-methyl, p-benzoquinone and o(m, p)-cresol were observed on the TiO2/ACF catalyst which had not been reported, together with the intermediates of side chain oxidation including benzyl alcohol, benzaldehyde and benzoic acid which had been reported; (3) although benzaldehyde was the primary intermediate under all RH level, amounts of the byproducts of aromatic ring oxidation were increased with the increase of RH; and (4) elevated RH increased the accumulation of benzyl alcohol but assuredly decreased the accumulation of benzaldehyde. These results suggested that (1) RH affects both the PCO rate and the PCO reaction path of toluene; (2) although methyl group oxidation is the major path, aromatic ring oxidation, which is not the expected path for the PCO of toluene, is enhanced when the RH increases; (3) apart from the role of hydroxyl radical (~·OH) produced from water by TiO2, water molecule also directly takes part in the PCO process. A hypothesis has been suggested: transition species comprised of benzaldehyde, hydroxyl and water molecule exists in the PCO conversion process from benzaldehyde to benzoic acid, though the hypothesis has not been confirmed.