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Microbiological, Geochemical and Hydrologic Processes Controlling Uranium Mobility: An Integrated Field Scale Subsurface Research Challenge Site at Rifle, Colorado February 2011 to January 2012 Annual Report to the U.S. Department of Energy Office of Science, Subsurface Biogeochemistry Research Program P.E. Long, Principal Investigator and Director February 2012 Prepared for the U.S. Department of Energy By Lawrence Berkeley National Laboratory Berkeley, California

At the Hanford Site, chromate was used throughout the 100 Areas (100-B, 100-C, 100-D/DR, 100-F, 100-H, and 100 K) as a corrosion inhibitor in reactor cooling water. Chromate was delivered in rail cars, tanker trucks, barrels, and local pipelines as dichromate granular solid or stock solution. In many occasions, chromate was inevitably discharged to surface or near-surface ground through spills during handling, pipeline leaks, or during disposal to cribs. The composition of the liquids that were discharged is not known and it is quite possible that Cr(VI) fate and transport in the contaminated sediments would be a function of the chemical composition of the waste fluids. The major objectives of this investigation which was limited in scope by the financial resources available, were to 1) determine the leaching characteristics of hexavalent chromium [Cr(VI)] from contaminated sediments collected from 100-D Area spill sites; 2) elucidate possible Cr(VI) mineral and/or chemical associations that may be responsible for Cr(VI) retention in the Hanford Site 100 Areas through the use of macroscopic leaching studies, and microscale characterization of contaminated sediments; and 3) provide information to construct a conceptual model of Cr(VI) geochemistry in the Hanford 100 Area vadose zone that can be used for developing options for environmental remediation. The information gathered from this research effort will help to further improve our understanding of Cr(VI) behavior in the vadose zone and will also help in accelerating the 100 Area Columbia River Corridor cleanup by providing valuable information to develop remedial action based on a fundamental understanding of Cr(VI) vadose zone geochemistry. A series of column experiments were conducted with contaminated sediments to study Cr(VI) desorption patterns. Column experiments used the field size fraction of the sediment samples and a simulated Hanford Site groundwater solution. Periodic stop flow events were applied to evaluate the change in elemental concentration during time periods of no flow and greater fluid residence time. Sediments were characterized for the spatial and mineralogical associations of the contamination using some microscale techniques such as X-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, and Mossbauer spectroscopy.

This report summarizes the methodology used to test the sequestration of technetium-99 present in both deionized water and simulated Hanford Tank Waste Treatment and Immobilization Plant waste solutions.

The project has been focused on biochemical processes in subsurface sediments involving Fe that control the valence state, solubility, and effective mobility of 99Tc. Our goal has been to understand the Tc biogeochemistry as it may occur in suboxic and biostimulated subsurface environments. Two objectives have been pursued: (1) To determine the relative reaction rates of 99Tc(VII)O2(aq) with metal reducing bacteria and biogenic Fe(II); and to characterize the identity, structure, and molecular speciation of Tc(IV) products formed through reaction with both biotic and abiotic reductants. (2) To quantify the biogeochemical factors controlling the reaction rate of O2 with Tc(IV)O2?nH2O in sediment resulting from the direct enzymatic reduction of Tc(VII) by DIRB and/or the reaction of Tc(VII) with the various types of biogenic Fe(II) produced by DIRB.

This report describes the advances that have been made over the past two years in testing and characterizing waste material in Hanford tanks.