The Oxidative Dissolution Mechanism of Uranium Dioxide. The Effect of pH and Oxygen Partial Pressure

摘要

The dissolution of the unirradiated uranium dioxide, UO_2, is largely affected by chemicul variables like pe, pH and carbonate concentration in solution. In a previous paper [1], we studied the kinetics of the dissolution of UO_2 as a function of pH and oxygen partial pressure and the experimental dissolution rates obtained showed a fractional dependence on both parameters. These fractional orders indicate a dissolution occurring via a surface mediated mechanism. In this work we have developed a mechanism accounting for the oxidative dissolution of UO_2, which depends on the oxygen concentration in solution and on the pH and a general rale equation has been deduced. This mechanism has been used to explain the results obtained by different authors and to explain and predict the dissolution of the spent nuclear fuel matrix.