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GIANLUCA LI PUMA

Six-flux absorption-scattering models for photocatalysis under wide-spectrum irradiation sources in annular and flat reactors using catalysts with different optical properties

Abstract

The photocatalytic oxidation of 2-hydroxybenzoic acid (2-HBA) in an annular tubular reactor (R1) and a flat rectangular open channel reactor (R2), which were irradiated with light sources emitting in the UVB, UVA and visible range of the solar radiation spectrum, and using two photocatalysts, titanium dioxide (TiO2 P25) and Ag-modified TiO2 P25 (Ag@TiO2) was modeled. The local volumetric rate of photon absorption (LVRPA) in the reactors was evaluated by the six-flux absorption scattering model (SFM). The Langmuir-Hinshelwood kinetic model of the degradation of a model contaminant on irradiated aqueous suspensions of TiO2 P25 and Ag@TiO2 was combined with the SFM radiation model and light emission models to determine local reaction rates, and further integrated with the reactors hydrodynamics and material balances to model the degradation of 2-HBA in the photoreactors. The linear source spherical emission (LSSE) and extensive source superficial diffuse emission (ESSDE) models were compared in terms of incident and transmitted photon fluxes through the reactor. It was shown that both LSSE and ESSDE models could be successfully applied for the modeling of annular and flat reactors, considering the emission from tubular fluorescent light sources. Since current research calls for materials with wide absorption in the solar radiation spectrum, spanning from the UV to the visible, therefore, the SFM model was adapted to consider such wide distribution. The optical properties of the photocatalysts were averaged over narrow wavelength ranges of the solar spectrum, wherein the contributions by the UVA, UVB and visible light irradiation to the LVRPA and contaminant degradation rate were separated. The effects of catalyst concentration, liquid velocity profile and the photon flux from different light sources on the 2-HBA degradation rate were explored. The “intrinsic” reaction kinetic constants of 2-HBA photocatalytic oxidation independent of reactor type, catalyst concentration, irradiance levels and hydrodynamic conditions were determined by fitting the experimental data to the model results. It was shown that the model parameters were independent of the type of catalyst used, although the catalyst exhibited significantly different optical properties.