Study of interaction between radioactive nuclides and graphite surface by the first-principles and statistic physics

The adsorption and desorption of four kinds of main radioactive productions (cesium, iodine, strontium and silver) on graphite surface in high temperature gas cooled reactors (HTGRs) have been studied. Using the first-principles density-functional theory, adsorptive geometry, energy and electron structure on the perfect and defective graphite surfaces have been calculated. It turns out that the adsorption of Cs, I and Sr atoms belongs to chemisorption while the adsorption of Ag is a pure physisorption. When introducing a vacancy in graphite surface, nuclide adatoms will be trapped by the vacancy and form chemical bonds with three nearest neighbor carbon atoms, leading to significant increase of the adsorption energy. In addition, a model of grand canonical ensemble is employed to deduce the adsorption rate as a function of temperature and partial pressure of nuclides produced. The transition temperate from adsorption to desorption of nuclides on graphite surface is defined as the inflexion point of the adsorption rate and its variation with nuclide density is obtained.