[en] Reagents used in spent nuclear fuel recycling impart unique contaminant patterns into the product stream of the process. Efforts are underway at Pacific Northwest National Laboratory to characterize and understand the relationship between these patterns and the process that created them. A main challenge to this effort, recycling processes that were employed at the Hanford site from 1944-1989 have been retired for decades. This precludes direct measurements of the contaminant patterns that propagate within product streams of these facilities. In the absence of any operating recycling facilities at Hanford, we have taken a multipronged approach to cataloging contaminants of U.S. reprocessing activities using: (1) historical records summarizing contaminants within the final Pu metal button product of these facilities; (2) samples of opportunity that represent intermediate products of these processes; and (3) lab-scale experiments and model simulations designed to replicate contaminant patterns at each stage of nuclear fuel reprocessing. Examples are provided here to illustrate how each of these approaches may be utilized in concert to help reconstruct contaminant patterns within the U.S. Pu stockpile produced at the Hanford site.

[en] A unique set of fission product gamma spectra was collected at short times (4 minutes to 1 week) on various fissionable materials. Gamma spectra were collected from the neutron-induced fission of uranium, neptunium, and plutonium isotopes at thermal, epithermal, fission spectrum, and 14-MeV neutron energies. This report describes the experimental methods used to produce and collect the gamma data, defines the experimental parameters for each method, and demonstrates the consistency of the measurements.

[en] During reactor operations and fuel burn up, some isotopic abundances change due to nuclear reactions and provide sensitive indicators of neutron fluence and fuel burnup. Secondary ion mass spectrometry (SIMS) analysis has been used to directly measure isotope ratios of selected impurity elements in irradiated nuclear reactor materials. Direct in situ SIMS measurements were made in graphite and metal samples, following shaping and surface cleaning. Other elements such as Be must be chemically separated and purified prior to SIMS analyses. Elements such as pre-existing impurity U and Pu produced from the U, are in low abundance and must also be chemically separated and are measured by thermal ionization mass spectrometry (TIMS). Studies combining SIMS and TIMS analyses demonstrate the value of this approach in determining reactor fluence profiles, power production, and other parameters. Future work proceeding from this analytical work will include developing monitoring devices designed for relatively easy placement and retrieval in a reactor, and direct SIMS analyses after exposure.