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DOE OSTI2024

Chlorine Worth Study Nuclear Data

The Chlorine Worth Study (CWS) was a series of experiments that took place at the National Criticality Experiments Research Center (NCERC), operated by Los Alamos National Laboratory (LANL). The focus of the experiments was to develop new integral benchmarks for the International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook with high sensitivity to chlorine in the thermal neutron energy region and which match sensitivities of aqueous chloride operations at LANL. This work discusses the experiment and how the experimental and simulated results using different nuclear data libraries compare to each other.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Benchmark of the Chlorine Worth Study Experiments in Support of Chlorine Nuclear Data Validation for Nuclear Criticality Safety

The Chlorine Worth Study (CWS) was a critical experiment to address an urgent need for thermal chlorine nuclear data validation in plutonium systems. This urgent need is tied directly to plutonium recycle and recovery operations in the plutonium facility at Los Alamos National Laboratory, where exceptionally conservative criticality safety limits are used because no credit is taken for the neutron capture by chlorine. The experiment used weapons-grade plutonium metal plates clad in stainless steel, known as the PANN (plutonium aluminum no nickel) ZPPR (zero power physics reactor) plates. The plutonium was reflected and moderated by high-density polyethylene and included combinations of polyvinyl chloride (PVC) and chlorinated polyvinyl chloride (CPVC) as absorbers. The experiment and benchmark included three configurations mimicking 30 g 239 Pu/L plutonium, 300 g 239 Pu/L plutonium, and 600 g 239 Pu/L plutonium in an aqueous chloride solution. Uncertainties in the benchmark included five broad categories: (1) criticality measurement, (2) mass and density, (3) dimensions, (4) material compositions, and (5) positioning. The largest contribution to the overall uncertainties for all three cases came from the material compositions, in particular the PVC and CPVC absorber compositions. A detailed model was created to be a near match (that is within expectations of transport code users) and a simplified model was created to minimize offset dimensions and expedite modeling for code validation. Sample calculations were completed in MCNP6.3 with ENDF/B-VIII.0 and ENDF/B-VII.1 nuclear data. For the detailed and simplified models, the average difference between the computed and experimental k eff was 951 pcm. CWS will serve as the key validation experiment for nuclear criticality safety in support of aqueous chloride operations. The sensitivity to the chlorine capture cross section is orders of magnitude greater than other existing benchmarks. The current limits, as defined by nuclear criticality safety, are 520 g Pu per batch, i.e. the minimum critical mass of the Pu solution infinitely reflected by water [Criticality Handbook: Volume II, (1969)]. This extremely conservative critical mass limit does not credit any neutron capture by chlorine (in particular neutron capture by 35 Cl) and greatly impedes the throughput required for current and future operations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Final Design for Additional Thermal/Epithermal eXperiments (TEX) with Sodium Chloride Absorbers to Provide Validation Benchmarks for TerraPower

The first set of Thermal/Epithermal eXperiments (TEX) with chlorine absorbers (TEX-Cl) were executed in Q4FY24 and are in the process of being benchmarked for the ICSBEP. TEX-Cl builds upon the TEX-HEU baseline cases that were published in the 2022 International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook. TEX-HEU, like TEX-Pu, was designed to be modular to allow for the incorporation of various absorbers and reflectors to test nuclear data and application case needs. For example, TEX-HEU with hafnium (TEX-Hf) utilizes hafnium plates as both absorbers and reflectors, depending on the tested configuration. A second set of chlorine experiments, dubbed More TEX-Cl, are laid out in this report to meet the needs of TerraPower for chlorine validation for their Molten Chloride Fast Reactor (MCFR) systems. TerraPower’s Molten Chloride Reactor Experiment (MCRE) and MCFR are fast molten salt reactors that utilize sodium chloride (NaCl) salt eutectics as the fuel and coolant. The MCRE eutectic is a mixture of NaCl and uranium trichloride (UCl 3 ). An abundant need for chlorine absorption validation has been expressed by multiple members of the community, including Y-12 (whose needs were addressed with the first set of experiments), LANL (whose needs were addressed with the Chlorine Worth Study (CWS)), TerraPower, institute de radioprotection et de sûreté nucléaire (IRSN), Savannah River Nuclear Solutions (SNRS), and others. Of the members who have expressed interest in this validation, most are interested in the fast neutron energy region, where the 35 Cl(n,p) reaction is most prominent. New 35 Cl(n,p) differential cross section measurements performed by LANL at LANCSE show substantial changes to the cross sections (Figure 1) and may be validated through these experiments as some configurations are optimally sensitive to this cross section.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗