Modeling and experimental investigation for development of Combined Electrolysis and Catalytic Exchange process for hydrogen isotope separation

Abstract

A process based on the Combined Electrolysis and Catalytic Exchange (CECE) has been developed for separation of hydrogen isotopes. Indigenously developed Platinum supported on Carbon Aerogel based hydrophobic catalyst was used for hydrogen-water isotope exchange reaction combined with hydrophilic packing in a catalytic exchange column. The exchange column has been studied in detail for various operating conditions in this study. The intrinsic kinetics for the catalytic reaction was determined through spinning basket reactor experiments, and activation energy was estimated to be 29.7 kJ/mol. The overall mass transfer co-efficient in a mixture of hydrophilic packing and hydrophobic catalyst packed bed was determined experimentally in a pilot scale counter current trickle bed reactor to be in the range of 0.15–0.25 s-1 for the proposed range of operating conditions. Individual mass transfer resistances for vapour-liquid mass transfer, external gas mass transfer and gas-solid mass transfer were estimated using widely accepted empirical correlations. Under benchmark operating conditions, the Damkohler number for the exchange column was found to be between 0.10 and 0.16, indicating a significant contribution of surface reaction to overall mass transfer resistance. The vapour liquid mass transfer was found to be fast compared to the gas-vapour reaction. Therefore, increasing hydrophobic catalyst proportion relative to hydrophilic packing was found to increase the overall mass transfer. A steady state process model has been developed to predict the performance of overall exchange process using the experimentally determined parameters. Validation of the process model was carried out using the experimental data generated on the pilot scale trickle bed reactor. Optimum operating conditions of temperature, hydrophobic catalyst to hydrophilic packing ratio, gas and liquid superficial velocities were determined.