The University of Manchester Greg BlackThesis submitted for the degree of Doctor of EngineeringIrradiated Graphite Waste: Analysis and Modelling of Radionuclide Production with a View to Long Term Disposal23rd June 2014The UK has predominantly used graphite moderator reactor designs in both its research and civil nuclear programmes. This material will become activated during operation and, once all reactors are shutdown, will represent a waste legacy of 96,000 tonnes . The safe and effective management of this material will require a full understanding of the final radiological inventory. The activity is known to arise from impurities present in the graphite at start of life as well as from contamination products transported from other components in the reactor circuit. The process is further complicated by radiolytic oxidation which leads to considerable weightloss of the graphite components. A comprehensive modelling methodology has been developed and validated to estimate the activity of the principle radionuclides of concern, 3H, 14C, 36Cl and 60Co. This methodology involves the simulation of neutron flux using the reactor physics code WIMS, and radiation transport code MCBEND. Activation calculations have been performed using the neutron activation software FISPACT. The final methodology developed allows full consideration of all processes which may contribute to the final radiological inventory of the material. The final activity and production pathway of each radionuclide has been researched in depth, as well as operational parameters such as the effect of changes in flux, fuel burnup, graphite weightloss and irradiation time. Methods to experimentally determine the activity, and distribution of key radionuclides within irradiated graphite samples have been developed in this research using a combination of both gamma spectroscopy and autoradiography. This work has been externally validated and provides confidence in the accuracy of the final modelling predictions. This work has been undertaken as part of the EU FP7 EURATOM Project: CARBOWASTE, and was funded by the Office for Nuclear Regulation.