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Survey of prospective techniques for molten salt reactor feed monitoring

Journal Article · · Annals of Nuclear Energy

Safeguards verification measurements of nuclear material content in fresh fuel salt for liquid-fueled molten salt reactors (MSRs) are likely to be required as part of nuclear material accountancy for International Atomic Energy Agency safeguards. Here, this paper presents a comprehensive review and evaluation of 18 potential candidate techniques to quantify total uranium and 235U for input accountancy measurements for liquid-fueled MSRs. As part of an overall screening and down-selection effort to identify the most promising techniques for further development for an MSR feed monitoring system, this paper defines eight figures of merit (FOMs): reasonably achievable measurement uncertainty, measurement time required, capital cost, burden upon the facility operator, maintenance intensity, technological maturity, human capital requirements for operation, and whether the technique introduces a path for potential material removal. Each candidate technique is then evaluated across these FOMs to identify the techniques with the highest potential for future development for fresh fuel accountancy measurements in MSRs. Our findings indicate that no single technique or combination thereof currently has the requisite technological maturity for immediate implementation in nuclear material accountancy at a liquid-fueled MSR facility. While several promising techniques are identified, there is a critical lack of experimental data for most systems in the context of molten salt applications.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2438899
Journal Information:
Annals of Nuclear Energy, Vol. 208; ISSN 0306-4549
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (86)

Spectroscopic monitoring of spent nuclear fuel reprocessing streams: an evaluation of spent fuel solutions via Raman, visible, and near-infrared spectroscopy journal September 2011
Measuring Lanthanide Concentrations in Molten Salt Using Laser-Induced Breakdown Spectroscopy (LIBS) journal September 2014
Microfluidic Alpha Spectrometry of UOX PWR UNF in a Molten Salt journal August 2017
Actinides recovery from irradiated metallic fuel in LiCl–KCl melts journal November 2015
Determination of uranium, thorium and plutonium isotopes by ICP-MS journal September 2012
Overcoming Oxidation State-Dependent Spectral Interferences: Online Monitoring of U(VI) Reduction to U(IV) via Raman and UV–vis Spectroscopy journal April 2020
Fission-product gamma-ray line pairs sensitive to fissile material and neutron energy
  • Marrs, R. E.; Norman, E. B.; Burke, J. T.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 592, Issue 3 https://doi.org/10.1016/j.nima.2008.04.032
journal July 2008
Isotopic analysis of uranium by laser induced breakdown spectroscopy journal May 2020
A fast-neutron coincidence collar using liquid scintillators for fresh fuel verification journal August 2017
Analysis of fissile materials by high-energy neutron-induced fission decay gamma-rays journal July 2005
Identification of short-lived fission products in delayed gamma-ray spectra for nuclear material signature verifications
  • Tohamy, M.; Crochemore, J. M.; Abbas, K.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 978 https://doi.org/10.1016/j.nima.2020.164347
journal October 2020
Material mixture solution analysis by a hybrid L-edge/L-XRF densitometer journal January 2019
Detection of U(VI) on the surface of altered depleted uranium by time-resolved laser-induced fluorescence spectroscopy (TRLFS) journal August 2006
Monitoring Noble Gases (Xe and Kr) and Aerosols (Cs and Rb) in a Molten Salt Reactor Surrogate Off-Gas Stream Using Laser-Induced Breakdown Spectroscopy (LIBS) journal May 2022
Novel methodology for the quantitative assay of fissile materials using temporal and spectral β-delayed γ-ray signatures
  • Chivers, D. H.; Alfonso, K.; Goldblum, B. L.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 269, Issue 16 https://doi.org/10.1016/j.nimb.2011.05.013
journal August 2011
A new method to measure the U-235 content in fresh LWR fuel assemblies via fast-neutron passive self-interrogation
  • Menlove, Howard; Belian, Anthony; Geist, William
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 877, 238-245 https://doi.org/10.1016/j.nima.2017.09.038
journal January 2018
Communication—Quantitative Voltammetric Analysis of High Concentration Actinides in Molten Salts journal December 2016
A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy
  • Knowles, Justin; Skutnik, Steven; Glasgow, David
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 833 https://doi.org/10.1016/j.nima.2016.06.112
journal October 2016
Time-Resolved Laser-Induced Spectrofluorometry of UO22+ in Nitric Acid Solutions. Preliminary Results for On-Line Uranium Monitoring Applications journal January 1993
Review—Concentration Measurements In Molten Chloride Salts Using Electrochemical Methods journal December 2021
Characterization of a Thermodynamic Reference Electrode for Molten LiF-BeF 2 (FLiBe) journal January 2017
Methods for Determining the Working Electrode Interfacial Area for Electroanalytical Measurements of Metal Ions in Molten LiCl-KCl journal August 2016
One candidate method based on short-lived indicator for burnup analysis journal September 2018
Performance testing of the upgraded uranium isotopics multi-group analysis code MGAU
  • Berlizov, A. N.; Gunnink, R.; Zsigrai, J.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 575, Issue 3 https://doi.org/10.1016/j.nima.2007.02.099
journal June 2007
Investigation of intrinsic origins of the signal uncertainty for laser-induced breakdown spectroscopy journal March 2019
Laser-Induced Breakdown Spectroscopy (LIBS) Measurement of Uranium in Molten Salt journal June 2018
Electrochemical and Laser-Induced Breakdown Spectroscopy Signal Fusion for Detection of UCl 3 -GdCl 3 -MgCl 2 in LiCl-KCl Molten Salt journal September 2020
Field testing of a fast-neutron coincidence collar for fresh uranium fuel verification
  • Beaumont, Jonathan; Lee, Taehoon; Mayorov, Mikhail
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 962 https://doi.org/10.1016/j.nima.2020.163682
journal February 2020
Quantitative analysis of trivalent uranium and lanthanides in a molten chloride by absorption spectrophotometry journal August 2012
In Situ Quantitative Measurement of Rare Earth Elements in Uranium Oxides by Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry journal February 2013
Basic characterization of uranium by high-resolution gamma spectroscopy journal August 2018
Determination of ultra traces amount of uranium in raffinates of Purex process by laser fluorimetry journal September 2011
Sensitivity of the active neutron coincidence collar response during simulated and experimental fresh fuel assay
  • Broughton, D. P.; Grund, M. S.; Renha, G.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 1001 https://doi.org/10.1016/j.nima.2021.165243
journal June 2021
Quantitative prediction of rare earth concentrations in salt matrices using laser-induced breakdown spectroscopy for application to molten salt reactors and pyroprocessing journal January 2021
Uranium Enrichment Determination Using a New Analysis Code for the U XKα Region: HyperGam-U journal June 2016
Determination of thorium and uranium in solution by laser-induced breakdown spectrometry journal January 2008
Quantification of Trace-Level Fissile Samples via Short-Lived Delayed Gamma Spectroscopy journal August 2019
Laser-induced breakdown spectroscopy measurements of uranium and thorium powders and uranium ore journal May 2013
Design, modeling and viability analysis of an online uranium Enrichment Monitor conference October 2011
Determination of 235U isotope abundance by measuring selected pairs of fission products
  • Yahua, Qiao; Jizong, Wu; Yi, Yang
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 665 https://doi.org/10.1016/j.nima.2011.10.020
journal February 2011
Determination of Uranium in Solution Using Laser-Induced Breakdown Spectroscopy journal August 1987
Electrochemical Analysis of Metal Stability in Candidate Reference Electrode Fluoride Salts (FLiNaK + 1 wt% AgF, MnF2, or NiF2) journal February 2024
Two-dimensional fluorescence spectroscopy of uranium isotopes in femtosecond laser ablation plumes journal June 2017
Application of Voltammetry for Quantitative Analysis of Actinides in Molten Salts journal January 2015
Laser-Induced Breakdown Spectroscopy (LIBS) in a Novel Molten Salt Aerosol System journal June 2016
Development and validation of hybrid K-edge/K-XRF densitometer for assay of nuclear fuel from reprocessing plants journal April 2020
Deployment of quasi-digital sensor for high temperature molten salt level measurement in pyroprocessing plants journal April 2018
Accurate determination of density, surface tension, and vessel depth using a triple bubbler system journal July 2018
Total dissolution of environmental samples for the determination of uranium and thorium by ICP-MS and alpha-particle spectrometry journal March 2022
Uranium enrichment measurement by X- and γ-ray spectrometry with the “URADOS” process journal August 1998
On-stream analysis of iron ore slurry using laser-induced breakdown spectroscopy journal November 2017
Simple method for liquid analysis by laser-induced breakdown spectroscopy (LIBS) journal July 2018
MCNP6 simulations of gamma line emissions from fission products and their comparisons to plutonium and uranium measurements journal March 2015
Automated high-temperature liquid level measurement system using a dynamic tube pressure technique journal May 2017
Identification of fissile materials from fission product gamma-ray spectra
  • Beddingfield, D. H.; Cecil, F. E.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 417, Issue 2-3 https://doi.org/10.1016/S0168-9002(98)00781-5
journal November 1998
Determination of uranium and plutonium in mixed oxide samples by X-ray methods and their comparison with potentiometry journal August 2022
A new generation of uranium coincidence fast neutron collars for assay of LWR fresh fuel assemblies
  • Swinhoe, M. T.; Menlove, H. O.; de Baere, P.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 1009 https://doi.org/10.1016/j.nima.2021.165453
journal September 2021
Measurement of Cerium and Gadolinium in Solid Lithium Chloride–Potassium Chloride Salt Using Laser-Induced Breakdown Spectroscopy (LIBS) journal July 2017
Laser-induced fluorescence spectroscopy of uranium monofluoride journal October 2022
A quantitative Monte Carlo modelling of the uranium and plutonium X-ray fluorescence (XRF) response from a hybrid K-edge/K-XRF densitometer
  • Berlizov, A. N.; Sharikov, D. A.; Ottmar, H.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 615, Issue 1 https://doi.org/10.1016/j.nima.2010.01.010
journal March 2010
Short-lived fission product measurements from >0.1 MeV neutron-induced fission using boron carbide journal February 2012
Stability of a Ni/NiF2 Reference Electrode with a Metallic Membrane for Use in Molten Fluoride Salts journal July 2024
Laser Ablation Plasmas and Spectroscopy for Nuclear Applications journal December 2023
Signatures of fissile materials: high-energy γ rays following fission
  • Norman, Eric B.; Prussin, Stanley G.; Larimer, Ruth-Mary
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 521, Issue 2-3 https://doi.org/10.1016/j.nima.2003.10.097
journal April 2004
In Situ Spectroscopy and Spectroelectrochemistry of Uranium in High-Temperature Alkali Chloride Molten Salts journal September 2008
In-Line Uranium Monitoring in Reprocessing Waste Solution by Time-Resolved Laser-Induced Fluorometry journal July 1992
Measurement of molten salt Raman spectra by the use of fiber optics journal May 1992
Uranium measurements using laser-induced breakdown spectroscopy in lithium chloride-potassium chloride salt of pyroprocessing journal May 2020
Sensor Fusion: Comprehensive Real-Time, On-Line Monitoring for Process Control via Visible, Near-Infrared, and Raman Spectroscopy journal July 2020
High concentration measurements of U and Pu with nondestructive and standardless K‐edge densitometer device journal September 2017
Isotopic concentration of uranium from alpha spectrum of electrodeposited source on 4H-SiC detector at 500 °C journal March 2019
The matrix influence on the determination of low uranium concentrations by laser induced fluorescence method journal November 2014
Feasibility study of 235U and 239Pu characterization in radioactive waste drums using neutron-induced fission delayed gamma rays
  • Nicol, T.; Pérot, B.; Carasco, C.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 832 https://doi.org/10.1016/j.nima.2016.06.055
journal October 2016
Electroanalytical measurements of binary-analyte mixtures in molten LiCl-KCl eutectic: Uranium(III)- and Magnesium(II)-Chloride journal April 2017
Quantification of Lanthanides in a Molten Salt Reactor Surrogate Off-Gas Stream Using Laser-Induced Breakdown Spectroscopy journal March 2022
In Situ High-Temperature Raman Spectroscopy of UCl3: A Combined Experimental and Theoretical Study journal November 2023
A new fast neutron collar for safeguards inspection measurements of fresh low enriched uranium fuel assemblies containing burnable poison rods
  • Evans, Louise G.; Swinhoe, Martyn T.; Menlove, Howard O.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 729 https://doi.org/10.1016/j.nima.2013.08.028
journal November 2013
Concept for an irradiation experiment to test a laser-induced breakdown spectroscopy off-gas sensor for molten salt systems journal January 2023
Development of quantitative analytical methods for the control of actinides in a pyrochemical partitioning process journal January 2005
Determination of 235U isotopic abundance by fission-yield difference method
  • Qiao, Yahua; Zhang, Ming; Yang, Yi
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 739 https://doi.org/10.1016/j.nima.2013.11.035
journal March 2014
Simultaneous quantification of Zr, Mo, U, Np and Pu in technological solutions of spent nuclear fuel reprocessing with a potentiometric multisensor system journal April 2023
Uranium and plutonium solution assays by transmission-corrected x-ray fluorescence spectrometry journal July 1999
New approach of a transient ICP-MS measurement method for samples with high salinity journal March 2017
Determination of plutonium in spent nuclear fuel using high resolution X-ray journal August 2015
Uranium enrichment measurements using the intensity ratios of self-fluorescence X-rays to 92keV gamma ray in UXKα spectral region journal April 2009
Electrochemical measurement of high concentrations of UCl3 and GdCl3 in molten LiCl-KCl eutectic journal November 2018