SUMMARYMaterials were developed and tested in support of the U.S. Department of Energy, Office of Nuclear Energy, Fuel Cycle Technology Separations and Waste Forms Campaign. Specifically, materials are being developed for the removal and immobilization of iodine and krypton from gaseous products of nuclear fuel reprocessing unit operations.During FY 2011, aerogel materials were investigated for removal and immobilization of 129 I. Two aerogel formulations were investigated, one based on functionalized silica and the second on chalcogenbased glasses (i.e., chalcogels). A silica aerogel was tested at ORNL for total I 2 sorption capacity. It was determined to have 48 mass% capacity while having little physisorbed I 2 (I 2 not chemically bound within the aerogel). Metal organic framework (MOF) structures were investigated for the removal and storage of Kr and a new MOF with about 8 mass% capacity for Xe and Kr was formulated and tested. The selectivity can be changed from Xe > Kr to Xe < Kr simply by changing the temperature. A patent disclosure has been filed. Lastly, silicon carbide (SiC) was loaded with Kr. The diffusion of Kr in SiC was found to be less than detectable values at temperatures as high as 500°C.