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Remote Americium Detection Using an Optical Sensor: A D-Optimal Strategy for Efficient PLS-Based Modeling

Journal Article · · Sensors
DOI:https://doi.org/10.3390/s25227022· OSTI ID:3004276
A fiber-optic visible–near-infrared absorption spectroscopy system in a glove box was demonstrated for remote quantification of Am(III) (0–500 µM) and HNO3 (0.1–9 M) using partial least squares regression (PLSR) models. The sensor platform, featuring a simple plug-and-play spectrophotometer, can enable noninvasive, real-time monitoring of actinide process solutions. To establish a flexible PLSR model calibration strategy, a D-optimal design developed using Nd(III) in previous studies was successfully extended to an actinide system with Am(III) to effectively minimize sample set size while maintaining robust prediction performance. The results suggest strong spectral similarities between Nd(III) and Am(III) and validate Nd(III) as an effective optical surrogate for trivalent actinide species. This work also supports the generalizability of a D-optimal training set selection approach for two-factor systems. The PLS1 models for Am(III) and HNO3 outperformed a PLS2 model and maintained reasonable performance in the presence of interfering U(VI). The resulting sensor system and multivariate approach provides a flexible and scalable solution for process monitoring, control, and safety in diverse nuclear applications.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Grant/Contract Number:
AC05-00OR22725; AR0001689
OSTI ID:
3004276
Journal Information:
Sensors, Journal Name: Sensors Journal Issue: 22 Vol. 25; ISSN 1424-8220
Publisher:
MDPI AGCopyright Statement
Country of Publication:
United States
Language:
English

References (44)

A closer look at the bias-variance trade-off in multivariate calibration journal March 1999
The utility of multivariate design in PLS modeling journal March 2004
A review on the mass spectrometric studies of americium: Present status and future perspective: MASS SPECTROMETRIC STUDIES OF AMERICIUM journal May 2016
Assessing and improving the stability of chemometric models in small sample size situations journal January 2008
UV–Vis spectroscopy with chemometric data treatment: an option for on-line control in nuclear industry journal April 2017
A systematic view of optical absorption spectra in the actinide series journal August 1986
Extractive—spectrophotometric determination of americium at trace levels with arsenazo-III journal June 1982
PLS-regression: a basic tool of chemometrics journal October 2001
Capability of detection of an analytical method evaluating false positive and false negative (ISO 11843) with partial least squares journal November 2003
A UV/Vis spectrophotometric methodology for quality control of stevia-based extracts in the food industry journal July 2022
Beyond U/Pu separation: Separation of americium from the highly active PUREX raffinate journal August 2023
Concentration determination of inorganic acids that do not absorb near-infrared (NIR) radiation through recognizing perturbed NIR water bands by them and investigation of accuracy dependency on their acidities journal June 2018
Americium and Plutonium Purification by Extraction (the AMPPEX process): Development of a new method to separate 241Am from aged plutonium dioxide for use in space power systems journal July 2018
Nd(III) hypersensitive peak as an optical absorption probe for determining nitric acid in aqueous solution: An application to aqueous raffinate solutions in nuclear reprocessing journal August 2021
Leveraging visible and near-infrared spectroelectrochemistry to calibrate a robust model for Vanadium(IV/V) in varying nitric acid and temperature levels journal July 2023
Multivariate chemometric methods and Vis-NIR spectrophotometry for monitoring plutonium-238 anion exchange column effluent in a radiochemical hot cell journal August 2022
IUPAC-Consistent Approach to the Limit of Detection in Partial Least-Squares Calibration journal July 2014
Optimization of Partial-Least-Squares Calibration Models by Simulation of Instrumental Perturbations journal August 1997
Comparing Sensor Fusion and Multimodal Chemometric Models for Monitoring U(VI) in Complex Environments Representative of Irradiated Nuclear Fuel journal January 2024
Spectroscopic Properties of Americium(III) in Mineral Acid Media journal July 2025
Practical Guide to Chemometric Analysis of Optical Spectroscopic Data journal June 2023
Characterization of the ALSEP Process at Equilibrium: Speciation and Stoichiometry of the Extracted Complex journal March 2020
Design of Experiments, Chemometrics, and Raman Spectroscopy for the Quantification of Hydroxylammonium, Nitrate, and Nitric Acid journal February 2022
Pursuit of the Ultimate Regression Model for Samarium(III), Europium(III), and LiCl Using Laser-Induced Fluorescence, Design of Experiments, and a Genetic Algorithm for Feature Selection journal January 2023
PCA and PLS Analysis of Lanthanides Using Absorbance and Single-Beam Visible Spectra journal July 2024
Optimal experimental design journal July 2018
The nature of chemical bonding in actinide and lanthanide ferrocyanides determined by X-ray absorption spectroscopy and density functional theory journal January 2016
Trends in process analytical technology journal January 2010
One-Factor-at-a-Time versus Designed Experiments journal May 1999
An Expository Paper on Optimal Design journal July 2011
Optical Absorption Characteristics For  7F0'→5L6' and  7F0'→ 7F6' Transitions of Trivalent Americium Ion in Aqueous Electrolyte Mixtures journal July 2017
A Piecewise Local Partial Least Squares (PLS) Method for the Quantitative Analysis of Plutonium Nitrate Solutions journal October 2017
A Review of Calibration Transfer Practices and Instrument Differences in Spectroscopy journal October 2017
Monitoring the Caustic Dissolution of Aluminum Alloy in a Radiochemical Hot Cell Using Raman Spectroscopy journal July 2020
Measuring Nd(III) Solution Concentration in the Presence of Interfering Er(III) and Cu(II) Ions: A Partial Least Squares Analysis of Ultraviolet–Visible Spectra journal October 2021
Comparing Designed Training Sets to Optimize Multivariate Regression Models for Pr, Nd, and Nitric Acid Using Spectrophotometry journal March 2024
Effect of Experimental Design on the Prediction Performance of Calibration Models Based on Near-Infrared Spectroscopy for Pharmaceutical Applications journal December 2012
Production of Cf-252 and other transplutonium isotopes at Oak Ridge National Laboratory journal September 2020
Spectroscopic monitoring of spent nuclear fuel reprocessing streams: an evaluation of spent fuel solutions via Raman, visible, and near-infrared spectroscopy journal September 2011
Determination of Americium in a Nitric Acid Medium Using Second-Order Derivative Spectrophotometry journal June 1996
The First Isolation Of Americium In The Form Of Pure Compounds - The Specific Alpha-Activity And Half-Life Of Am241 report July 1950
Reduction Rates for Higher Americium Oxidation States in Nitric Acid report September 2015
Leveraging design of experiments to build chemometric models for the quantification of uranium (VI) and HNO3 by Raman spectroscopy journal August 2024
Hierarchical Modeling to Enhance Spectrophotometry Measurements—Overcoming Dynamic Range Limitations for Remote Monitoring of Neptunium journal May 2023

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