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1 2This report fulfills the M3 milestone (M3FT+13PN0810027) to report on a radiolysis computer model analysis that estimates the generation of radiolytic products for a storage canister. The analysis considers radiolysis outside storage canister walls and within the canister fill gas over a possible 300+year lifetime. Previous work relied on estimates based directly on a water radiolysis G+value. a This work also includes that effect with the addition of coupled kinetics for 111 reactions for 40 gas species to account for radiolytic+induced chemistry, which includes water recombination and reactions with air.The main results for radiolysis inside the canister fill gas are described as follows.Significant radiolysis of water vapor requires the presence of residual air to disable recombination.Reactions between residual water (1 L) and air in 4500 L of free space result in percent levels of H 2 , O 2 and HNO 3 at 300 years, and about one+half the maximum values reached in the first 16 years.Calculations indicate that a much greater volume of residual water (20 L) would be required to reach the 4% H 2 flammability limit in 16 years, and between 3 and 4 L of water would be required to reach the 4% H 2 flammability limit in 300 years.Increased residual air results in greater H 2 and HNO 3 concentrations, but also in the depletion of O 2 because it is more effectively removed by a radiolytically induced reaction with N 2 .For lower (0.1%) residual air, O 2 is initially depleted and then generated for storage times greater than 50 years, resulting in approximately 0.5% O 2 .For lower (0.1 L) residual water and 1% air, all radiolytic products are less than 1%.The main results for radiolysis outside the canister follow.The main radiolytic products formed in moist air are HNO 3 , N 2 O, NO 2 , CO, and small amounts of O 3 . Even for extremely long residence times, the highest concentrations are less than 50 ppm and are less than 1 ppm for more typical flow conditions. Dry air gives similar concentrations as moist air with the exception of increased NO 2 and the near absence of HNO 3 .