Thermodynamic Analysis of the Oxidation of Radioactive Graphite in the CuO–NaCl–KCl–Na2CO3–K2CO3 Melt in Water Vapor

Abstract

Graphite is widely used in the atomic industry and nuclear power engineering. In the next 10–15 years, the resource of most blocks in the uranium–graphite reactors in Russia will be exhausted with allowance for the elongation of the service life, as follows from the results of repair-and-renewal operations. High-activity graphite can be processed by flameless oxidation in molten salts. The purpose of this work is to study the behavior of radionuclides during the flameless oxidation of radioactive graphite in the CuO–NaCl–KCl–Na2CO3–K2CO3 melt in water vapor using a thermodynamic simulation and the Terra software package. A thermodynamic simulation is an effective and unique method used to investigate diverse high-temperature processes of thermal decomposition, reduction, and synthesis. The calculation is performed using a reference datable of the properties of individual substances. Graphite burns up at 573 K. The condensed compounds of cesium, chlorine, and uranium evaporate at 1673 K. An increase in the temperature to 1973 K leads to the vapor pressure of the condensed compounds of beryllium, calcium, and strontium. The condensed oxide of europium(III) and the condensed oxide of plutonium(IV) transform into a vapor state at 2173 K. The condensed oxide of nickel transforms into a vapor state at 2473 K. A further increase in the temperature to 2773 K leads to the transformation of the condensed oxide of americium(III) into a vapor state. Only a vapor–gas phase is present in the isolated system in the temperature range from 2773 to 3273 K.