The Radiation Induced Chemistry of the Uranyl Cation in Carbonate -Bicarbonate Solutions as Followed by NMR Spectroscopy

摘要

Hydrogen peroxide formed by radiolysis of carbonate -bicarbonate media was followed by ~(13)C NMR using dissolved ~(233)UO_2(~(13)CO_3)_3~(4-) as the alpha source (D_α= 12.1 Gy/hr). It is shown that the speciation of the peroxide carbonates (or other species) that are formed in the pH region 5.9 and 11.6 by titration with hydrogen peroxide are common to those formed by hydrogen peroxide generated by radiolysis. Radiolytic generation of hydrogen peroxide was followed by observing the formation of a uranyl peroxide carbonate complex. Complex formation was observed to accelerate for about 1200 hours and to terminate between 1 x 10~(-4) and 5 x 10~(-4) M. It is assumed that either a steady state H_2O_2 production rate was established in solution or that some limiting feature of the experiment was responsible for slowing the yield of product.