Improvement of Ethylene Removal Performance by Adsorption/Oxidation in a Pin-Type Corona Discharge Coupled with Pd/ZSM-5 Catalyst

Abstract

The adsorption and plasma-catalytic oxidation of dilute ethylene were performed in a pin-type corona discharge-coupled Pd/ZSM-5 catalyst. The catalyst has an adsorption capacity of 320.6 μ mol   g cat − 1 . The catalyst was found to have two different active sites activated at around 340 and 470 °C for ethylene oxidation. The removal of ethylene in the plasma catalyst was carried out by cyclic operation consisting of repetitive steps: (1) adsorption (60 min) followed by (2) plasma-catalytic oxidation (30 min). For the purpose of comparison, the removal of ethylene in the continuous plasma-catalytic oxidation mode was also examined. The ethylene adsorption performance of the catalyst was improved by the cyclic plasma-catalytic oxidation. With at least 80% of C2H4 in the feed being adsorbed, the cyclic plasma-catalytic oxidation was carried out for the total adsorption time of 8 h, whereas it occurred within 2 h of early adsorption in the case of catalyst alone. There was a slight decrease in catalyst adsorption capability with an increased number of adsorption cycles due to the incomplete release of CO2 during the plasma-catalytic oxidation step. However, the decreased rate of adsorption capacity was negligible, which is less than one percent per cycle. Since the activation temperature of all active sites of Pd/ZSM-5 for ethylene oxidation is 470 °C, the specific input energy requirement by heating the feed gas in order to activate the catalyst is estimated to be 544 J/L. This value is higher than that of the continuous plasma-catalytic oxidation (450 J/L) for at least 86% ethylene conversion. Interestingly, the cyclic adsorption and plasma-catalytic oxidation of ethylene is not only a low-temperature oxidation process but also reduces energy consumption. Specifically, the input energy requirement was 225 J/L, which is half that of the continuous plasma-catalytic oxidation; however, the adsorption efficiency and conversion rate were maintained. To summarize, cyclic plasma treatment is an effective ethylene removal technique in terms of low-temperature oxidation and energy consumption.