Processing ix spent resin waste for C-14 isotope recovery (1991)

A process developed at Ontario Hydro for recovering carbon-14 (C-14) from spent ion exchange resin wastes is described. Carbon-14 is an undesirable by-product of CANDU{sup 1} nuclear reactor operation. It has an extremely long (5730 years) half-life and can cause dosage to inhabitants by contact, inhalation, or through the food cycle via photosynthesis. Release of carbon-14 to the environment must be minimized. Presently, all the C-14 produced in the Moderator and Primary Heat Transport (PHT) systems of the reactor is effectively removed by the respective ion exchange columns, and the spent ion exchange resins are stored in suitably engineered concrete structures. Because of the large volumes of spent resin waste generated each year this method of disposal by long term storage tends to be uneconomical; and may also be unsatisfactory considering the long half-life of the C-14. However, purified C-14 is a valuable commercial product for medical, pharmaceutical, agricultural, and organic chemistry research. Currently, commercial C-14 is made artificially in research reactors by irradiating aluminum nitride targets for 4.5 years. If the C-14 containing resin waste can be used to reduce this unnecessary production of C-14, the total global build-up of this radioactive chemical can be reduced. There is much incentive in removing the C-14 from the resin waste to reduce the volume of C-14 waste, and also in purifying the recovered C-14 to supply the commercial market. The process developed by Ontario Hydro consists of three main steps: C-14 removal from spent resins, enrichment of recovered C-14, and preparation of final product. Components of the process have been successfully tested at Ontario Hydro's Research Division, but the integration of the process is yet to be demonstrated. A pilot scale plant capable of processing 4 m{sup 3} of spent resins annually is being planned for demonstrating the technology. The measured C-14 activity levels on the spent resins ranged from 47-213 Ci/m{sup 3} for the Moderator spent resins generated by CANDU reactors. For an estimated average C-14 activity level of 100 Ci/m{sup 3}, a total of 400 Ci of C-14 can be produced each year. Based on the current market value of the C-14 isotope, the cost of the demonstration plant can be recovered in less than two years. Upon successful demonstration, the process can be scaled up. The volume of resin wastes produced by the stations can readily supply a full scale production of 2000 Ci or more per annum. Several alternative routes have been considered for this process which include: thermal stripping vs. acid stripping of the spent resins, laser enrichment vs. cryogenic distillation for the enrichment of the gaseous intermediate product, and direct gas phase reaction vs. liquid phase ionic precipitation of the final product. Analysis of the experimental results obtained at Ontario Hydro Research Division and also those reported in the literature has led to the selection of the following process: The C-14 is first removed by acid stripping the resins to form carbon dioxide. The gas is then separated from the carrier gas and converted by reaction with zinc to carbon monoxide, which is cryogenically distilled. Essentially pure C-14 monoxide is obtained and oxidized to produce C-14 dioxide. The gas is then reacted with a suitable hydroxide to produce the desired carbonate product.