Engineering topics

Garduno, Katherine

Publications and source records attributed to Garduno, Katherine.

8 records

DOE OSTI2019

Intercomparison of the Radio-Chronometric Ages of Plutonium-Certified Reference Materials with Distinct Isotopic Compositions

In this article, an intercomparison of the radio-chronometric ages of four distinct plutonium-certified reference materials varying in chemical form, isotopic composition, and period of production are presented. The cross-comparison of the different 234 U/ 238 Pu, 235 U/ 239 Pu, 236 U/ 240 Pu, and 241 Am/ 241 Pu model purification ages obtained at four independent analytical facilities covering a range of laboratory environments from bulk sample processing to clean facilities dedicated to nuclear forensic investigation of environmental samples enables a true assessment of the state-of-practice in “age dating capabilities” for nuclear materials. The analytical techniques evaluated used modern mass spectrometer instrumentation including thermal ionization mass spectrometers and inductively coupled plasma mass spectrometers for isotopic abundance measurements. Both multicollector and single collector instruments were utilized to generate the data presented here. Consensus values established in this study make it possible to use these isotopic standards as quality control standards for radio-chronometry applications. Results highlight the need for plutonium isotopic standards that are certified for 234 U/ 238 Pu, 235 U/ 239 Pu, 236 U/ 240 Pu, and 241 Am/ 241 Pu model purification ages as well as other multigenerational radio-chronometers such as 237 Np/ 241 Pu. Due to the capabilities of modern analytical instrumentation, analytical laboratories that focus on trace level analyses can obtain model ages with marginally larger uncertainties than laboratories that handle bulk samples. Lastly, when isotope ratio measurement techniques like thermal ionization mass spectrometry and inductively coupled plasma mass spectrometry with comparable precision are utilized, model purification ages with similar uncertainties are obtained.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Comparison of the Davies and Gray titrimetric method with potassium dichromate and ceric titrants

The modified New Brunswick Laboratory (NBL) Davies and Gray titrimetry method uses potassium dichromate standard 136-f from the National Institute of Standards and Technology for calibration. However, the presence of chromium in the resulting waste stream makes the disposal of waste from this procedure costly. We report that the Actinide Analytical Chemistry (C-AAC) group at Los Alamos National Laboratory investigated and transitioned to a cerium based titrant as an alternative. We present the first long-term analytical study using this ceric-based titration method and compare it with NBL results based on the more-widely used dichromate titrimetric method.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2017

AmO 2 Analysis for Analytical Method Testing and Assessment: Analysis Support for AmO 2 Production

Americium oxide samples will be measured for various analytes to support AmO 2 production. The key analytes that are currently requested by the Am production customer at LANL include total Am content, Am isotopics, Pu assay, Pu isotopics, and trace element content including 237 Np content. Multiple analytical methods will be utilized depending on the sensitivity, accuracy and precision needs of the Am matrix. Traceability to the National Institute of Standards and Technology (NIST) will be achieved, where applicable, by running NIST traceable quality control materials. This given that there are no suitable AmO 2 reference materials currently available for requested analytes. The primary objective is to demonstrate the suitability of actinide analytical chemistry methods to support AmO 2 production operations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

The application of visible absorption spectroscopy to the analysis of uranium in aqueous solutions

Through assay analysis into an excess of 1 M H 2 SO 4 at fixed temperature a technique has been developed for uranium concentration analysis by visible absorption spectroscopy over an assay concentration range of 1.8 – 13.4 mgU/g. Once implemented for a particular spectrophotometer and set of spectroscopic cells this technique promises to provide more rapid results than a classical method such as Davies-Gray (DG) titration analysis. While not as accurate and precise as the DG method, a comparative analysis study reveals that the spectroscopic method can analyze for uranium in well characterized uranyl(VI) solution samples to within 0.3% of the DG results. For unknown uranium solutions in which sample purity is less well defined agreement between the developed spectroscopic method and DG analysis is within 0.5%. The technique can also be used to detect the presence of impurities that impact the colorimetric analysis, as confirmed through the analysis of ruthenium contamination. Finally, extending the technique to other assay solution, 1 M HNO 3 , HCl and Na 2 CO 3 , has also been shown to be viable. As a result, of the four aqueous media the carbonate solution yields the largest molar absorptivity value at the most intensely absorbing band, with the least impact of temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Determination of origin and intended use of plutonium metal using nuclear forensic techniques

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240 Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback and trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239 Pu fission foil targets for physics experiments, such as cross-section measurements, etc.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2016

Forensic investigation of plutonium metal: a case study of CRM 126

In our study, a certified plutonium metal reference material (CRM 126) with a known production history is examined using analytical methods that are commonly employed in nuclear forensics for provenancing and attribution. Moreover, the measured plutonium isotopic composition and actinide assay are consistent with values reported on the reference material certificate. Model ages from U/Pu and Am/Pu chronometers agree with the documented production timeline. Finally, these results confirm the utility of these analytical methods and highlight the importance of a holistic approach for forensic study of unknown materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

Nuclear forensic analysis of a non-traditional actinide sample

Nuclear forensic publications, performance tests, and research and development efforts typically target the bulk global inventory of intentionally safeguarded materials, such as plutonium (Pu) and uranium (U). Other materials, such as neptunium (Np), pose a nuclear security risk as well. Trafficking leading to recovery of an interdicted Np sample is a realistic concern especially for materials originating in countries that reprocesses fuel. Using complementary forensic methods, potential signatures for an unknown Np oxide sample were investigated. Measurement results were assessed against published Np processes to present hypotheses as to the original intended use, method of production, and origin for this Np oxide.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Uranium Detection - Technique Validation Report

As a LANL activity for DOE/NNSA in support of SHINE Medical Technologies™ ‘Accelerator Technology’ we have been investigating the application of UV-vis spectroscopy for uranium analysis in solution. While the technique has been developed specifically for sulfate solutions, the proposed SHINE target solutions, it can be adapted to a range of different solution matrixes. The FY15 work scope incorporated technical development that would improve accuracy, specificity, linearity & range, precision & ruggedness, and comparative analysis. Significant progress was achieved throughout FY 15 addressing these technical challenges, as is summarized in this report. In addition, comparative analysis of unknown samples using the Davies-Gray titration technique highlighted the importance of controlling temperature during analysis (impacting both technique accuracy and linearity/range). To fully understand the impact of temperature, additional experimentation and data analyses were performed during FY16. The results from this FY15/FY16 work were presented in a detailed presentation, LA-UR-16-21310, and an update of this presentation is included with this short report summarizing the key findings. The technique is based on analysis of the most intense U(VI) absorbance band in the visible region of the uranium spectra in 1 M H 2 SO 4 , at λ max = 419.5 nm.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗