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U-Sr isotopic speedometer: Fluid flow and chemical weatheringrates inaquifers

Description: Both chemical weathering rates and fluid flow are difficultto measure in natural systems. However, these parameters are critical forunderstanding the hydrochemical evolution of aquifers, predicting thefate and transport of contaminants, and for water resources/water qualityconsiderations. 87Sr/86Sr and (234U/238U) activity ratios are sensitiveindicators of water-rock interaction, and thus provide a means ofquantifying both flow and reactivity. The 87Sr/86Sr values in groundwaters are controlled by the ratio of the dissolution rate to the flowrate. Similarly, the (234U/238U) ratio of natural ground waters is abalance between the flow rate and the dissolution of solids, andalpha-recoil loss of 234U from the solids. By coupling these two isotopesystems it is possible to constrain both the long-term (ca. 100's to1000's of years) flow rate and bulk dissolution rate along the flow path.Previous estimates of the ratio of the dissolution rate to theinfiltration flux from Sr isotopes (87Sr/86Sr) are combined with a modelfor (234U/238U) to constrain the infiltration flux and dissolution ratefor a 70-m deep vadose zone core from Hanford, Washington. The coupledmodel for both (234U/238U) ratios and the 87Sr/86Sr data suggests aninfiltration flux of 5+-2 mm/yr, and bulk silicate dissolution ratesbetween 10-15.7 and 10-16.5 mol/m2/s. The process of alpha-recoilenrichment, while primarily responsible for the observed variation in(234U/238U) of natural systems, is difficult to quantify. However, therate of this process in natural systems affects the interpretation ofmost U-series data. Models for quantifying the alpha-recoil loss fractionbased on geometric predictions, surface area constraints, and chemicalmethods are also presented. The agreement between the chemical andtheoretical methods, such as direct measurement of (234U/238U) of thesmall grain size fraction and geometric calculations for that sizefraction, is quite good.
Date: December 27, 2005
Creator: Maher, Kate; DePaolo, Donald J. & Christensen, John N.
Partner: UNT Libraries Government Documents Department

Uranium-series comminution ages of continental sediments: Case study of a Pleistocene alluvial fan

Description: Obtaining quantitative information about the timescales associated with sediment transport, storage, and deposition in continental settings is important but challenging. The uranium-series comminution age method potentially provides a universal approach for direct dating of Quaternary detrital sediments, and can also provide estimates of the sediment transport and storage timescales. (The word"comminution" means"to reduce to powder," reflecting the start of the comminution age clock as reduction of lithic parent material below a critical grain size threshold of ~;;50 mu m.) To test the comminution age method as a means to date continental sediments, we applied the method to drill-core samples of the glacially-derived Kings River Fan alluvial deposits in central California. Sediments from the 45 m core have independently-estimated depositional ages of up to ~;;800 ka, based on paleomagnetism and correlations to nearby dated sediments. We characterized sequentially-leached core samples (both bulk sediment and grain size separates) for U, Nd, and Sr isotopes, grain size, surface texture, and mineralogy. In accordance with the comminution age model, where 234U is partially lost from small sediment grains due to alpha recoil, we found that (234U/238U) activity ratios generally decrease with age, depth, and specific surface area, with depletions of up to 9percent relative to radioactive equilibrium. The resulting calculated comminution ages are reasonable, although they do not exactly match age estimates from previous studies and also depend on assumptions about 234U loss rates. The results indicate that the method may be a significant addition to the sparse set of available tools for dating detrital continental sediments, following further refinement. Improving the accuracy of the method requires more advanced models or measurements for both the recoil loss factor fa and weathering effects. We discuss several independent methods for obtaining fa on individual samples that may be useful for future studies.
Date: April 30, 2010
Creator: Lee, Victoria E.; DePaolo, Donald J. & Christensen, John N.
Partner: UNT Libraries Government Documents Department

An Assay Method for Determining Extra-Cellular Lipases from Pseudomonas aeruginosa

Description: The applicability of an isotopically labelled assay system to determine the lipase production in Pseudomonas aeruginosa was evaluated. Supernatant from cultures of Pseudomonas aeruginosa grown in a medium containing olive oil was incubated with a substrate containing labelled trioleate. Fatty acids were isolated by means of a liquid-liquid partition system. Enzyme activity was determined by measuring the amounts of free fatty acid by liquid scintillation counting. Findings indicate that the isotopicallylabelled, liquid-liquid partitioning assay is reliable, sensitive and adaptable to rapid assay conditions. It was also determined that different strains of Pseudomonas aeruginosa produce varying amounts of lipase. Partial purification of supernatant by gel filtration produced two protein peaks showing enzymatic activity.
Date: May 1978
Creator: Christensen, John N.
Partner: UNT Libraries

Sediment transport time measured with U-Series isotopes: Resultsfrom ODP North Atlantic Drill Site 984

Description: High precision uranium isotope measurements of marineclastic sediments are used to measure the transport and storage time ofsediment from source to site of deposition. The approach is demonstratedon fine-grained, late Pleistocene deep-sea sediments from Ocean DrillingProgram Site 984A on the Bjorn Drift in the North Atlantic. The sedimentsare siliciclastic with up to 30 percent carbonate, and dated by sigma 18Oof benthic foraminifera. Nd and Sr isotopes indicate that provenance hasoscillated between a proximal source during the last three interglacialperiods volcanic rocks from Iceland and a distal continental sourceduring glacial periods. An unexpected finding is that the 234U/238Uratios of the silicate portion of the sediment, isolated by leaching withhydrochloric acid, are significantly less than the secular equilibriumvalue and show large and systematic variations that are correlated withglacial cycles and sediment provenance. The 234U depletions are inferredto be due to alpha-recoil loss of234Th, and are used to calculate"comminution ages" of the sediment -- the time elapsed between thegeneration of the small (<_ 50 mu-m) sediment grains in the sourceareas by comminution of bedrock, and the time of deposition on theseafloor. Transport times, the difference between comminution ages anddepositional ages, vary from less than 10 ky to about 300 to 400 ky forthe Site 984A sediments. Long transport times may reflect prior storagein soils, on continental shelves, or elsewhere on the seafloor. Transporttime may also be a measure of bottom current strength. During the mostrecent interglacial periods the detritus from distal continental sourcesis diluted with sediment from Iceland that is rapidly transported to thesite of deposition. The comminution age approach could be used to dateQuaternary non-marine sediments, soils, and atmospheric dust, and may beenhanced by concomitant measurement of 226Ra/230Th, 230Th/234U, andcosmogenic nuclides.
Date: June 5, 2006
Creator: DePaolo, Donald J.; Maher, Kate; Christensen, John N. & McManus,Jerry
Partner: UNT Libraries Government Documents Department

Isotopic Tracers for Biogeochemical Processes and Contaminant Transport: Hanford, Washington

Description: Our goal is to use isotopic measurements to understand how contaminants are introduced to and stored in the vadose zone, and what processes control migration from the vadose zone to groundwater and then to surface water. We have been using the Hanford Site in south-central Washington as our field laboratory, and our investigations are often stimulated by observations made as part of the groundwater monitoring program and vadose zone characterization activities. Understanding the transport of contaminants at Hanford is difficult due to the presence of multiple potential sources within small areas, the long history of activities, the range of disposal methods, and the continuing evolution of the hydrological system. Observations often do not conform to simple models, and cannot be adequately understood with standard characterization approaches, even though the characterization activities are quite extensive. One of our objectives is to test the value of adding isotopic techniques to the characterization program, which has the immediate potential benefit of addressing specific remediation issues, but more importantly, it allows us to study fundamental processes at the scale and in the medium where they need to be understood. Here we focus on two recent studies at the waste management area (WMA) T-TX-TY, which relate to the sources and transport histories of vadose zone and groundwater contamination and contaminant fluid-sediment interaction. The WMA-T and WMA-TX-TY tank farms are located within the 200 West Area in the central portion of the Hanford Site (Fig. 2). They present a complicated picture of mixed groundwater plumes of nitrate, {sup 99}Tc, Cr{sup 6+}, carbon tetrachloride, etc. and multiple potential vadose zone sources such as tank leaks and disposal cribs (Fig. 3). To access potential vadose zone sources, we analyzed samples from cores C3832 near tank TX-104 and from C4104 near tank T-106. Tank T-106 was involved in a ...
Date: April 19, 2007
Creator: DePaolo, Donald J.; Christensen, John N.; Conrad, Mark E. & Dresel, and P. Evan
Partner: UNT Libraries Government Documents Department

Laboratory Experiments Bearing on the Origin and Evolution of Olivine-rich Chondrules

Description: Evaporation rates of K2O, Na2O, and FeO from chondrule-like liquids and the associated potassium isotopic fractionation of the evaporation residues were measured to help understand the processes and conditions that affected the chemical and isotopic compositions of olivine-rich Type IA and Type IIA chondrules from Semarkona. Both types of chondrules show evidence of having been significantly or totally molten. However, these chondrules do not have large or systematic potassium isotopic fractionation of the sort found in the laboratory evaporation experiments. The experimental results reported here provide new data regarding the evaporation kinetics of sodium and potassium from a chondrule-like melt and the potassium isotopic fractionation of evaporation residues run under various conditions ranging from high vacuum to pressures of one bar of H2+CO2, or H2, or helium. The lack of systematic isotopic fractionation of potassium in the Type IIA and Type IA chondrules compared with what is found in the vacuum and one-bar evaporation residues is interpreted as indicating that they evolved in a partially closed system where the residence time of the surrounding gas was sufficiently long for it to have become saturated in the evaporating species and for isotopic equilibration between the gas and the melt. A diffusion couple experiment juxtaposing chondrule-like melts with different potassium concentrations showed that the diffusivity of potassium is sufficiently fast at liquidus temperatures (DK&gt;2-10-4cm2/s at 1650-C) that diffusion-limited evaporation cannot explain why, despite their having been molten, the Type IIA and Type IA chondrules show no systematic potassium isotopic fractionation.
Date: June 24, 2011
Creator: Richter, Frank M.; Mendybaev, Ruslan A.; Christensen, John N.; Ebel, Denton & Gaffney, Amy
Partner: UNT Libraries Government Documents Department

Pb Isotopes as an Indicator of the Asian Contribution to Particulate Air Pollution in Urban California

Description: During the last two decades, expanding industrial activity in east Asia has led to increased production of airborne pollutants that can be transported to North America. Previous efforts to detect this trans-Pacific pollution have relied upon remote sensing and remote sample locations. We tested whether Pb isotope ratios in airborne particles can be used to directly evaluate the Asian contribution to airborne particles of anthropogenic origin in western North America, using a time series of samples from a pair of sites upwind and downwind of the San Francisco Bay Area. Our results for airborne Pb at these sites indicate a median value of 29 Asian origin, based on mixing relations between distinct regional sample groups. This trans-Pacific Pb is present in small quantities but serves as a tracer for airborne particles within the growing Asian industrial plume. We then applied this analysis to archived samples from urban sites in central California. Taken together, our results suggest that the analysis of Pb isotopes can reveal the distribution of airborne particles affected by Asian industrial pollution at urban sites in northern California. Under suitable circumstances, this analysis can improve understanding of the global transport of pollution, independent of transport models.
Date: October 25, 2010
Creator: Ewing, Stephanie A.; Christensen, John N.; Brown, Shaun T.; Vancuren, Richard A.; Cliff, Steven S. & DePaolo, Donald J.
Partner: UNT Libraries Government Documents Department

Isotopic Tracking of Hanford 300 Area Derived Uranium in the Columbia River

Description: Our objectives in this study are to quantify the discharge rate of uranium (U) to the Columbia River from the Hanford Site's 300 Area, and to follow that U down river to constrain its fate. Uranium from the Hanford Site has variable isotopic composition due to nuclear industrial processes carried out at the site. This characteristic makes it possible to use high-precision isotopic measurements of U in environmental samples to identify even trace levels of contaminant U, determine its sources, and estimate discharge rates. Our data on river water samples indicate that as much as 3.2 kg/day can enter the Columbia River from the 300 Area, which is only a small fraction of the total load of dissolved natural background U carried by the Columbia River. This very low-level of Hanford derived U can be discerned, despite dilution to &lt; 1 percent of natural background U, 350 km downstream from the Hanford Site. These results indicate that isotopic methods can allow the amounts of U from the 300 Area of the Hanford Site entering the Columbia River to be measured accurately to ascertain whether they are an environmental concern, or are insignificant relative to natural uranium background in the Columbia River.
Date: October 31, 2010
Creator: Christensen, John N.; Dresel, P. Evan; Conrad, Mark E.; Patton, Gregory W. & DePaolo, Donald J.
Partner: UNT Libraries Government Documents Department

Multi-Scale Mass Transfer Processes Controlling Natural Attenuation and Engineered Remediation: An IFRC Focused on Hanford’s 300 Area Uranium Plume

Description: The Integrated Field-Scale Subsurface Research Challenge (IFRC) at the Hanford Site 300 Area uranium (U) plume addresses multi-scale mass transfer processes in a complex hydrogeologic setting where groundwater and riverwater interact. A series of forefront science questions on mass transfer are posed for research which relate to the effect of spatial heterogeneities; the importance of scale; coupled interactions between biogeochemical, hydrologic, and mass transfer processes; and measurements and approaches needed to characterize and model a mass-transfer dominated system. The project was initiated in February 2007, with CY 2007 and CY 2008 progress summarized in preceding reports. The site has 35 instrumented wells, and an extensive monitoring system. It includes a deep borehole for microbiologic and biogeochemical research that sampled the entire thickness of the unconfined 300 A aquifer. Significant, impactful progress has been made in CY 2009 with completion of extensive laboratory measurements on field sediments, field hydrologic and geophysical characterization, four field experiments, and modeling. The laboratory characterization results are being subjected to geostatistical analyses to develop spatial heterogeneity models of U concentration and chemical, physical, and hydrologic properties needed for reactive transport modeling. The field experiments focused on: (1) physical characterization of the groundwater flow field during a period of stable hydrologic conditions in early spring, (2) comprehensive groundwater monitoring during spring to characterize the release of U(VI) from the lower vadose zone to the aquifer during water table rise and fall, (3) dynamic geophysical monitoring of salt-plume migration during summer, and (4) a U reactive tracer experiment (desorption) during the fall. Geophysical characterization of the well field was completed using the down-well Electrical Resistance Tomography (ERT) array, with results subjected to robust, geostatistically constrained inversion analyses. These measurements along with hydrologic characterization have yielded 3D distributions of hydraulic properties that have been incorporated into an updated and ...
Date: February 1, 2010
Creator: Zachara, John M.; Bjornstad, Bruce N.; Christensen, John N.; Conrad, Mark E.; Fredrickson, Jim K.; Freshley, Mark D. et al.
Partner: UNT Libraries Government Documents Department

Multi-Scale Mass Transfer Processes Controlling Natural Attenuation and Engineered Remediation: An IFRC Focused on Hanford’s 300 Area Uranium Plume January 2010 to January 2011

Description: The Integrated Field Research Challenge (IFRC) at the Hanford Site 300 Area uranium (U) plume addresses multi-scale mass transfer processes in a complex subsurface hydrogeologic setting where groundwater and riverwater interact. A series of forefront science questions on reactive mass transfer focus research. These questions relate to the effect of spatial heterogeneities; the importance of scale; coupled interactions between biogeochemical, hydrologic, and mass transfer processes; and measurements and approaches needed to characterize and model a mass-transfer dominated system. The project was initiated in February 2007, with CY 2007, CY 2008, and CY 2009 progress summarized in preceding reports. A project peer review was held in March 2010, and the IFRC project has responded to all suggestions and recommendations made in consequence by reviewers and SBR/DOE. These responses have included the development of “Modeling” and “Well-Field Mitigation” plans that are now posted on the Hanford IFRC web-site. The site has 35 instrumented wells, and an extensive monitoring system. It includes a deep borehole for microbiologic and biogeochemical research that sampled the entire thickness of the unconfined 300 A aquifer. Significant, impactful progress has been made in CY 2010 including the quantification of well-bore flows in the fully screened wells and the testing of means to mitigate them; the development of site geostatistical models of hydrologic and geochemical properties including the distribution of U; developing and parameterizing a reactive transport model of the smear zone that supplies contaminant U to the groundwater plume; performance of a second passive experiment of the spring water table rise and fall event with a associated multi-point tracer test; performance of downhole biogeochemical experiments where colonization substrates and discrete water and gas samplers were deployed to the lower aquifer zone; and modeling of past injection experiments for model parameterization, deconvolution of well-bore flow effects, system understanding, and ...
Date: February 1, 2011
Creator: Zachara, John M.; Bjornstad, Bruce N.; Christensen, John N.; Conrad, Mark S.; Fredrickson, Jim K.; Freshley, Mark D. et al.
Partner: UNT Libraries Government Documents Department

Multi-Scale Mass Transfer Processes Controlling Natural Attenuation and Engineered Remediation: An IFRC Focused on Hanford’s 300 Area Uranium Plume January 2011 to January 2012

Description: The Integrated Field Research Challenge (IFRC) at the Hanford Site 300 Area uranium (U) plume addresses multi-scale mass transfer processes in a complex subsurface biogeochemical setting where groundwater and riverwater interact. A series of forefront science questions on reactive mass transfer motivates research. These questions relate to the effect of spatial heterogeneities; the importance of scale; coupled interactions between biogeochemical, hydrologic, and mass transfer processes; and measurements and approaches needed to characterize and model a mass-transfer dominated biogeochemical system. The project was initiated in February 2007, with CY 2007, CY 2008, CY 2009, and CY 2010 progress summarized in preceding reports. A project peer review was held in March 2010, and the IFRC project acted upon all suggestions and recommendations made in consequence by reviewers and SBR/DOE. These responses have included the development of 'Modeling' and 'Well-Field Mitigation' plans that are now posted on the Hanford IFRC web-site, and modifications to the IFRC well-field completed in CY 2011. The site has 35 instrumented wells, and an extensive monitoring system. It includes a deep borehole for microbiologic and biogeochemical research that sampled the entire thickness of the unconfined 300 A aquifer. Significant, impactful progress has been made in CY 2011 including: (i) well modifications to eliminate well-bore flows, (ii) hydrologic testing of the modified well-field and upper aquifer, (iii) geophysical monitoring of winter precipitation infiltration through the U-contaminated vadose zone and spring river water intrusion to the IFRC, (iv) injection experimentation to probe the lower vadose zone and to evaluate the transport behavior of high U concentrations, (v) extended passive monitoring during the period of water table rise and fall, and (vi) collaborative down-hole experimentation with the PNNL SFA on the biogeochemistry of the 300 A Hanford-Ringold contact and the underlying redox transition zone. The modified well-field has functioned superbly without ...
Date: March 5, 2012
Creator: Zachara, John M.; Bjornstad, Bruce N.; Christensen, John N.; Conrad, Mark S.; Fredrickson, Jim K.; Freshley, Mark D. et al.
Partner: UNT Libraries Government Documents Department

Identifying the sources of subsurface contamination at the Hanford site in Washington using high-precision uranium isotopic measurements

Description: In the mid-1990s, a groundwater plume of uranium (U) was detected in monitoring wells in the B-BX-BY Waste Management Area (WMA) at the Hanford Site in Washington. This area has been used since the late 1940s to store high-level radioactive waste and other products of U fuel-rod processing. Using multiple collector ICP source magnetic sector mass spectrometry (MC ICPMS) high precision uranium isotopic analyses were conducted of samples of vadose zone contamination and of groundwater. The ratios {sup 236}U/{sup 238}U, {sup 234}U/{sup 238}U and {sup 238}U/{sup 235}U are used to distinguish contaminant sources. Based on the isotopic data, the source of the groundwater contamination appears to be related to a 1951 overflow event at tank BX-102 that spilled high level U waste into the vadose zone. The U isotopic variation of the groundwater plume is a result of mixing between contaminant U from this spill and natural background U. Vadose zone U contamination at tank B-110 likely predates the recorded tank leak and can be ruled out as a source of groundwater contamination, based on the U isotopic composition. The locus of vadose zone contamination is displaced from the initial locus of groundwater contamination, indicating that lateral migration in the vadose zone was at least 8 times greater than vertical migration. The time evolution of the groundwater plume suggests an average U migration rate of {approx}0.7-0.8 m/day showing slight retardation relative to a ground water flow of {approx}1 m/day.
Date: March 30, 2004
Creator: Christensen, John N.; Dresel, P. Evan; Conrad, Mark E.; Maher, Kate & DePaolo, Donald J.
Partner: UNT Libraries Government Documents Department