Executive SummaryThis investigation is focused on refining an in situ technology for vadose zone remediation of uranium by the addition of ammonia (NH 3 ) gas with no addition of water. The objectives were to: a) refine the technique of ammonia gas treatment, b) identify the geochemical changes in uranium surface phases, c) identify broader geochemical changes that occur, and d) predict and test injection of ammonia gas for intermediate-scale systems to identify process interactions that could impact field-scale implementation. For ammonia gas injection into vadose zone sediments to be successful as a uranium remediation technology, it needs to show decreased U mobility of the most mobile U phases (aqueous, adsorbed) in a variety of field conditions. Uranium is present in Hanford sediment include in multiple phases including aqueous U(VI)-carbonate complexes, adsorbed, uranium coprecipitated with carbonates, and U-bearing minerals Na-boltwoodite and uranophane. Ammonia treatment of sediments raises the pH in Hanford sediments from 8.0 to 11-13, which has resulted in a decrease in uranium mobility, as evidenced by decrease in aqueous and adsorbed uranium in 85% of the different sediments tested (different U surface phase distributions or NH 3 treatments) and an increase in 8M HNO 3 extracted U (hard to extract U phases, silicates/phosphates/oxides) for 79% of sediments tested. There were also inconsistent changes in two acetate extractions, likely the result of dissolution of multiple surface U phases (U-carbonates, Na-boltwoodite, uranophane). Surface phase analysis by laser induced fluorescence spectroscopy and extended x-ray absorption structure has showed essentially no U surface mineral change in sediments initially containing Na-boltwoodite, but some U surface phase changes in U-calcite coprecipitates to uranyl oxyhydroxide, Na-boltwoodite, and uranyl tricarbonate. Therefore, the ammonia gas treatment appears most effective for U present in the most mobile phases: aqueous U, adsorbed U, and carbonate associated U. NH 3 -treated sediments containing Na-boltwoodite and uranophane showed decreased leaching even though solid phase analysis showed little changes in the U mineralogy. The decreased leaching may be the result of other mineral precipitates coating these phases. Minerals that leached the most significant mass of ions were montmorillonite, muscovite, and kaolinite. A greater understanding of these dissolution/precipitation/coating processes is needed to predict the long-term impact on uranium mobility.Ammonia gas injection experiments conducted in 20-to 30-ft long 1-D systems and a layered 2-D radial flow system were used to characterize the physicochemical changes at the NH 3 reaction front and treatment coverage in heterogeneous sediments. For 5% NH 3 (95%N 2 ) injection, an average of 234 pore volumes were needed to achieve the elevated pH (10.2 to 11.4) of the reaction front observed, with 465 pore volumes needed to achieve pH equilibrium (pH = 11.88), at 4% water content and 35% porosity. The des...