Changes in the pore network structure of Hanford sediment after reaction with caustic tank wastes

At the former nuclear weapon production site in Hanford, WA, caustic radioactive tank waste leaks into subsurface sediments and causes dissolution of quartz and aluminosilicate minerals, and precipitation of sodalite and cancrinite. This work examines changes in pore structure due to these reactions in a previously-conducted column experiment. The column was sectioned and 2D images of the pore space were generated using backscattered electron microscopy and energy dispersive X-ray spectroscopy. A pre-precipitation scenario was created by digitally removing mineral matter identified as secondary precipitates. Porosity, determined by segmenting the images to distinguish pore space from mineral matter, was up to 0.11 less after reaction. Erosion-dilation analysis was used to compute pore and throat size distributions. Images with precipitation had more small and fewer large pores. Precipitation decreased throat sizes and the abundance of large throats. These findings agree with previous findings based on 3D X-ray CMT imaging, observing decreased porosity, clogging of small throats, and little change in large throats. However, 2D imaging found an increase in small pores, mainly in intragranular regions or below the resolution of the 3D images. Also, an increase in large pores observed via 3D imaging was not observed in the 2D analysis. Changes in flow conducting throats that are the key permeability-controlling features were observed in both methods.     

Reducing security vulnerabilities for critical infrastructure

In this paper, we show the need for improved Process Control System (PCS) security, and describe some of the promising research areas in PCS security. One implementation of PCS in critical infrastructure and factory automation is a supervisory, control, and data acquisition (SCADA) system, a real-time industrial process control system which centrally monitors and controls remote and/or local processes utilizing plant, equipment, or devices (such as switches, valves, pumps, relays, etc.) while collecting and logging field data. Current SCADA systems are distributed, networked, and dependent on open protocols for the internet, which are exposed to remote cyber terrorism. They are particularly vulnerable to unauthorized access. We give some examples of SCADA processes with natural gas control systems in USA and the Ubiquitous Sensor Network (USN) in Korea. We also examine a representative vulnerability and corresponding measures for security, and present an example of concrete measures for the security of mass transportation as a critical infrastructure.     

U(VI) adsorption on aquifer sediments at the Hanford Site

Aquifer sediments collected via split-spoon sampling in two new groundwater wells in the 200-UP-1 operable unit at the Hanford Site were characterized and showed typical Ringold Unit E Formation properties dominated by gravel and sand. High iron-oxide content in Fe oxide/clay coatings caused the highest U(VI) adsorption as quantified by batch K(d) values, indicating iron oxides are the key solid adsorbent in the 200-UP-1 sediments that affect U(VI) fate and mobility. Even though U(VI) adsorption on the gravel-sized fraction of the sediments is considered to be negligible, careful characterization should be conducted to determine U(VI) adsorption on gravel, because of presence of Fe oxides coatings and diffusion-controlled adsorption into the gravel particles' interior surfaces. A linear adsorption isotherm was observed up to 10(-6) M (238 microg/L) of total U(VI) concentration in batch U(VI) adsorption tests with varying total U(VI) concentrations in spiked groundwater. U(VI) adsorption decreased with increasing concentrations of dissolved carbonate, because strong anionic aqueous uranium-carbonate complexes formed at high pH and high alkalinity conditions. Noticeable uranium desorption hysteresis was observed in a flow-through column experiment, suggesting that desorption K(d) values for aged uranium-contaminated sediments at the Hanford Site can be larger than adsorption K(d) values determined in short-term laboratory experiments and slow uranium release from contaminated sediments into the groundwater is expected.     

Settling and dewatering characteristics of granulated methane-oxidizing bacteria

We evaluated the settling ability and dewaterability of granulated methane-oxidizing bacteria (GMOB) after granulation using a continuous-flow reactor. A comparative analysis on settling and dewatering characteristics due to changes in sludge retention time (SRT, 10, 15 and 20 days) during cultivation of GMOB was conducted. In assessing dewaterability, the specific resistance to filtration (SRF) of activated sludge and GMOB was found to be 8.21×1013-2.38×1014 and 4.88 × 1012-1.98×1013 m/kg, respectively. It was confirmed that as SRT decreased, SRF of GMOB increased. In the case of bound extracellular polymeric substance (EPS), activated sludge registered 147.5 mg/g-VSS while GMOB exhibited 171-177.2 mg/g-VSS. In the case of extracellular polymeric substance soluble EPS in effluent, activated sludge measured 62 mg/L and GMOB had 17.4-21.4 mg/L. The particle size analysis showed that mean particle diameters of GMOB were 402, 369, and 350 μm, respectively, at SRTs of 20, 15 and 10 days. In addition, it was found that GMOB had a larger mean particle diameter and exhibited much better settleability and dewaterability than activated sludge did.     

Enhanced radionuclide immobilization and flow path modifications by dissolution and secondary precipitates

Caustic radioactive wastes that have leaked at Hanford Site (Richland, WA) induce mineral dissolution and subsequent secondary precipitation that influence the fate and transport of contaminants present in the waste solutions. The effects of secondary mineral precipitates, formed after contacting solids with simulated caustic wastes, on the flow path changes and radionuclide immobilization were investigated by reacting quartz, a mixture of quartz and biotite, and a Hanford sediment (Warden soil: coarse-silty, mixed, superactive, mesic Xeric Haplocambids) with simulated caustic tank waste solution. Continuous Si dissolution and concomitant secondary mineral precipitation were the principal reactions observed in both batch and flow-through tests. Nitrate-cancrinite was the dominant secondary precipitate on mineral surfaces after 3- to 10-d reaction times in batch experiments. X-ray microtomography images of a reacted quartz column revealed that secondary precipitates cemented quartz grains together and modified pore geometry in the center of the column. Along the circumference of the packed column, however, quartz dissolution continuously occurred, suggesting that wastes that leaked from buried tanks in the past likely did not migrate vertically as modeled in risk assessments but rather the pathways likely changed to be dominantly horizontal on precipitation of secondary precipitate phases in the Hanford vadose zone. Based on batch equilibrium sorption results on the reacted sediments, the dominant secondary precipitates (cancrinites) on the mineral surfaces enhanced the sorption capacity of typical Hanford sediment for radionuclides 129I(-I), 79Se(VI), 99Tc(VII), and 90Sr(II), all of which are of major concern at the Hanford Site.     

Investigation of 3H, 99Tc,and 90Sr transport in fractured rock and the effects of fracture-filling/coating material at LILW disposal facility

Environmental Geochemistry and Health - Batch adsorption, batch diffusion, and flow-through column experiments were conducted using groundwater and fractured rock collected in unsaturated zone to...