Abstract:
14C has become the nuclide that contributes the most to the annual effective dose to the surrounding public among the radioactive effluents during normal operation of nuclear power plants, but for a long time, domestic nuclear power units have not been equipped with airborne
14C treatment facilities, it is important and urgent to seek technical methods to reduce
14C emissions based on potential and actual needs under the requirements of the existing emission limits. Domestic nuclear power units under construction and in operation are mainly pressurized water reactors (more than 95% of the total), and the airborne
14C in this type of reactors mainly exists in the form of alkane compounds. Therefore, in this study,
14CH
4, which accounts for the largest proportion of
14C alkane compounds and has the most stable chemical properties, was taken as the treatment target, and low-temperature plasma technology was introduced to investigate its discharge behavior and CH
4 treatment performance. The results show that under the optimal conditions of normal temperature and pressure, output voltage of 17.89 kV, and gas flow rate of 0.83 cm/s, the plasma’s CH
4 treatment efficiency can reach 99.37%, and the CO
2 selectivity can reach 46.99%. The plasma’s CH
4 treatment performance can be improved by increasing the output voltage, reaction temperature, and decreasing the gas flow rate. However, since increasing the reaction temperature would bring problems about energy consumption, safety, and equipment complexity, increasing the reaction temperature is not the first choice. In addition to CO
2, there are more than thirty kinds of by-products produced in the process of plasma treatment of CH
4, which are dominated by organic substances. The kinetics process of plasma treatment of CH
4 is in accordance with the quasi-primary reaction kinetics model, and the corresponding rate constants are 1.104 8 m
3/(kW·h). The above results indicate that plasma technology has a broad development prospect in the field of airborne
14C treatment and monitoring, especially in the treatment of
14C alkane compounds. The focus of subsequent research should be focused on optimizing the reaction pathway, lowering the reaction barriers, further increasing the proportion of CH
4 directed oxidation to CO
2, and significantly reducing the formation of by-products.