Acetylene photocatalytic oxidation using continuous flow reactor: Gas phase and adsorbed phase investigation, assessment of the photocatalyst deactivation

• Simultaneous characterisation of the gas phase and adsorbed phase by-products.
• Evidence of photocatalyst deactivation due to adsorbed carboxylic acids.
• Recovery of the oxidation efficiency using regeneration sequences.
• Long term efficiency using the cyclic treatment/regeneration approach.

Acetylene, used as a model volatile organic compound (VOC), is submitted to photocatalytic oxidation. This study is based on the simultaneous characterisation of: (i) the gas phase at the reactor outlet; (ii) the adsorbed phase on the photocatalytic media. Experiments are performed in a continuous flow reactor, and analytical procedures have been developed to identify and quantify the gaseous and adsorbed side-products. The photocatalytic media consists in P25 Degussa TiO2 nanoparticles deposited on glass fibres. First, the process efficiency is investigated through C2H2 conversion rate and mineralisation. The treatment performances tend to decrease with time regarding conversion and mineralisation. Then, the oxidation process is investigated through gaseous and adsorbed by-products. Three carboxylic acids have been quantified in the adsorbed phase during oxidative treatment; their temporal evolutions are determined. Their contribution to the carbon balance is discussed. It is evidenced that their adsorption on the photocatalytic media leads to a saturation of the surface. Formaldehyde, glyoxal and formic acid are quantified in the gas phase. Their cumulative temporal profiles and their contribution to the carbon balance confirm the hypothesis of a surface deactivation. The decrease of the process performances with time and the increase of gaseous by-products are correlated with the photocatalyst coverage by adsorbed acids. Carbon balances calculated for various treatment times, give an overview of the process evolution. The regeneration of the photocatalyst surface is possible under synthetic air; 80% of the adsorbed compounds are mineralised. The performances of a cyclic procedure (treatment/regeneration) are evaluated. This approach preserves the photocatalyst performances and ensures a mineralisation of 85% of the converted acetylene.

Contributions of CO, CO2, adsorbed carboxylic acids and identified gas phase organic intermediates to the carbon balance as a function of irradiation time during the photocatalytic dynamic flow treatment of acetylene.Figure optionsDownload as PowerPoint slide