The CH2M HILL Hanford Group, Inc. (CH2M HILL) is producing risk/performance assessments to support the closure of single-shell tanks at the U.S. Department of Energy's Hanford Site. As part of this effort, staff at Pacific Northwest National Laboratory were asked to develop release models for contaminants of concern that are present in residual sludge remaining in tank 241-C-106 (C-106) after final retrieval of waste from the tank. The primary contaminants of concern in the sludge are 99 Tc, 238 U, 129 I, and Cr because of their potential mobility in the environment and the long half-lives of the radionuclides. A key result from this work is that high percentages (>90%) of these primary contaminants are not readily leachable from the residual waste. This minimizes their future release rates to the environment, and is similar to 99 Tc results found in related studies of sludges from tanks AY-102, C-203, and C-204.Developing release models consists of laboratory testing to produce contaminant release data and a conceptual source release model. After development, the release model can be incorporated into a fate and transport model as part of a long-term risk assessment for the closed tank.Initial laboratory tests (Tier 1) were conducted to characterize the sludge and identify water-leachable constituents. Based on the results of Tier 1 tests, additional analyses were performed to augment the characterization of the material and determine the controlling mechanism(s) for release of contaminants. Tier 2 tests consisted of X-ray diffraction (XRD) and scanning electron microscopy/energy dispersive spectrometry (SEM/EDS) analyses of the solids to identify reactive phases, and selective extractions to quantify the release of contaminants from particular solid phases.The laboratory results of sludge and liquid testing were used to develop source term models that describe the release of contaminants as infiltrating water contacts the solids in the future. These models simulate the geochemical system in the tank sludge and take into account interactions between the solution phase and the contaminant-containing solids. The release models are simplifications of the complex geochemical interactions occurring; however, they adequately represent the release of the primary contaminants of concern from the sludge as measured in the laboratory tests.Because of the highly complex chemical nature of tank C-106 residual sludge, clear and quantitative phase associations of the contaminants of concern with the phases known to exist in the sludge are difficult to specify. Although the various characterization methods employed in this study have revealed a number of important observations and have provided valuable data for constructing a scientifically defensible release model, many questions remain. Because a thorough understanding of all the important phase associations for the contaminants of concern cannot be developed at this time, an empirically based release model has been developed. Although less satisfying from a mechanistic ...