This laboratory-scale investigation focused on decreasing uranium mobility in subsurface contaminated sediments in the vadose zone by in situ geochemical manipulation at low water content. This geochemical manipulation of the sediment surface phases included reduction, pH change (acidic and alkaline), and additions of chemicals (phosphate and ferric iron) to form specific precipitates. Reactants were advected into one-dimensional columns packed with uranium-contaminated sediment from the 200 Area of the Hanford Site as a reactive gas (for CO 2 , NH 3 , H 2 S, SO 2 ), with a 0.1% water content mist [for NaOH, Fe(III), HCl, PO 4 ] and with a 1% water content foam (for PO 4 ).Uranium is present in the sediment in multiple phases that include (in decreasing mobility) the following: aqueous U(VI) complexes, adsorbed uranium, reduced U(IV) precipitates, rind-carbonates, total carbonates, oxides, silicates, and phosphates. Geochemical changes were evaluated in the ability to change the mixture of surface uranium phases to less mobile forms, as defined by a series of liquid extractions that dissolve progressively less soluble phases. Although liquid extractions provide some useful information as to the generalized uranium surface phases (and are considered operational definitions of extracted phases), positive identification of surface phase changes by electron microprobe analysis is in progress. Some of the changes in uranium mobility directly involve uranium phases, whereas other changes result in precipitate coatings on uranium surface phases. The long-term implication of the uranium surface phase changes to alter uranium mass mobility in the vadose zone was then investigated using simulations of one-dimensional infiltration and downward migration of six uranium phases to the water table.In terms of the short-term decrease in uranium mobility (in decreasing order), NH 3 , NaOH mist, CO 2 , HCl mist, and Fe(III) mist showed 20% to 35% change in uranium surface phases. Difference in treatment effectiveness between sediments likely reflects mineralogy. Phosphate addition (mist or foam advected) showed inconsistent change in aqueous and adsorbed uranium, but significant coating (likely phosphates) on uranium carbonates. The two reductive gas treatments (H 2 S and SO 2 ) showed little change. For long-term decrease in uranium reduction, mineral phases created that had low solubility (phosphates and silicates) were desired, so NH 3 , phosphates (mist and foam delivered), and NaOH mist showed the greatest formation of these minerals. In addition, simulations of uranium movement in the vadose zone showed that these treatments greatly decreased uranium transport to groundwater. Advection of reactive gasses was the easiest to implement into low water content sediments at the laboratory-scale (and presumably field-scale) experiments. Both mist and foam advection show potential and need further development, but current implementation techniques move reactants shorter distances relative to reactive gasses. Overall, the am...