Studies on the kinetics of catalytic combustion of deuterium using 0.5% platinum loaded on Dixon ring catalyst

Abstract

When hydrogen isotopes are present in stoichiometric ratio of 2:1 with oxygen in inert gas such as helium, catalytic combustion is the most promising option to reduce the concentration of hydrogen isotopes and to minimize the associated safety hazards. This is the case, when deuterium and oxygen is formed during radiolysis of heavy water in moderator circuit of Pressurized Heavy Water Reactors (PHWR) and mixed with helium in the cover gas system. In order to design the catalytic reactor for recombination of deuterium and oxygen, the data on catalytic combustion kinetics under the similar process conditions are essential. However, the catalytic combustion data is generally reported for combustion of hydrogen in air, where oxygen is available in excess. The studies on the kinetics of catalytic combustion of deuterium where oxygen is present in stoichiometric ratio of 2:1 in an inert gas medium such as helium, is very scarce. In the present study, the multi-step reaction mechanism of catalytic combustion of hydrogen in presence of platinum catalyst is analyzed for the present process conditions. Based on the analysis, a simple rate expression is proposed for the present process conditions of catalytic combustion of deuterium. Further, 0.5% platinum catalyst is prepared on a stainless steel Dixon ring support with an objective to achieve better heat transfer characteristics and lesser reduction in the catalytic activity due to water adsorption. The kinetic data is generated using a differential packed bed reactor operating in a closed loop. The experiments were conducted at different temperatures using a stoichiometric mixture of deuterium and oxygen in helium. The rate constant for the above proposed model is estimated based on the experimental data at different temperatures. Further, the activation energy and frequency factor are determined and the activation energy for the present catalyst is found to be on the lower side in comparison to literature data.