The Effects of the Degradation of Organic Materials in the Near Field of a Radioactive Waste Repository

Abstract

ABSTRACTUK Nirex Ltd are seeking to develop a deep underground repository for the disposal of solid ILW and LLW in the UK. The formation of water-soluble complexants from the degradation of the solid organic polymers and cellulosic materials present in such wastes may influence the solubility and sorption properties of a number of radioelements. A number of materials have been chemically degraded under alkaline, anaerobic conditions representative of the near field of the repository. Measurements of plutonium solubility in the leachates obtained show that the degradation of cellulose is of particular concern; the effects on the solubility can be several orders of magnitude greater than those of other organic materials. Products formed from the degradation of ion-exchange resins were found to have little effect. Solubilities of a number of other radioelements in aerobically degraded cellulose leachates are also given. The effect of reducing the ratio of celluloseto cement in the degradation experiments results in a decrease in plutonium solubility in the corresponding leachate. Several of the likely degradation products of cellulose have been individually synthesised including isosaccharinic acid, a key degradation product of cellulose. Enhanced plutonium solubilities have been measured in 10-3M solutions of these compounds. Sorption of plutonium onto cement from leachates obtained by the degradation of 10% cellulose in cement is reduced by about two orders of magnitude. Interaction with cement removes significant concentrations of complexants from solution. Thermodynamic modelling studies show that hydroxyl groups present in the compounds which result from the alkaline degradation of cellulose can strongly complex with plutonium.