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Title: Development of On-Line Spectroscopic pH Monitoring for Nuclear Fuel Reprocessing Plants: Weak Acid Schemes

Abstract

Knowledge of real-time solution properties and composition is a necessity for any spent nuclear fuel reprocessing method. Metal-ligand speciation in aqueous solutions derived from the dissolved commercial spent fuel is highly dependent upon the acid concentration/pH, which influences extraction efficiency and the resulting speciation in the organic phase. Spectroscopic process monitoring capabilities, incorporated in a counter current centrifugal contactor bank, provide a pathway for on-line real-time measurement of solution pH. The spectroscopic techniques are process-friendly and can be easily configured for on-line applications, while classic potentiometric pH measurements require frequent calibration/maintenance and have poor long-term stability in aggressive chemical and radiation environments. Our research is focused on developing a general method for on-line determination of pH of aqueous solutions through chemometric analysis of Raman spectra. Interpretive quantitative models have been developed and validated under the range of chemical composition and pH using a lactic acid/lactate buffer system. The developed model was applied to spectra obtained on-line during solvent extractions performed in a centrifugal contactor bank. The model predicted the pH within 11% for pH > 2, thus demonstrating that this technique could provide the capability of monitoring pH on-line in applications such as nuclear fuel reprocessing.

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1214877
Report Number(s):
PNNL-SA-107022
AF5805010
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Analytical Chemistry, 87(10):5139-5147
Additional Journal Information:
Journal Name: Analytical Chemistry, 87(10):5139-5147
Country of Publication:
United States
Language:
English
Subject:
pH, spectroscopic monitoring, on-line monitoring, weak acid, lactic acid, solvent extraction

Citation Formats

Casella, Amanda J., Hylden, Laura R., Campbell, Emily L., Levitskaia, Tatiana G., Peterson, James M., Smith, Frances N., and Bryan, Samuel A. Development of On-Line Spectroscopic pH Monitoring for Nuclear Fuel Reprocessing Plants: Weak Acid Schemes. United States: N. p., 2015. Web. doi:10.1021/ac504578t.
Casella, Amanda J., Hylden, Laura R., Campbell, Emily L., Levitskaia, Tatiana G., Peterson, James M., Smith, Frances N., & Bryan, Samuel A. Development of On-Line Spectroscopic pH Monitoring for Nuclear Fuel Reprocessing Plants: Weak Acid Schemes. United States. doi:10.1021/ac504578t.
Casella, Amanda J., Hylden, Laura R., Campbell, Emily L., Levitskaia, Tatiana G., Peterson, James M., Smith, Frances N., and Bryan, Samuel A. Tue . "Development of On-Line Spectroscopic pH Monitoring for Nuclear Fuel Reprocessing Plants: Weak Acid Schemes". United States. doi:10.1021/ac504578t.
@article{osti_1214877,
title = {Development of On-Line Spectroscopic pH Monitoring for Nuclear Fuel Reprocessing Plants: Weak Acid Schemes},
author = {Casella, Amanda J. and Hylden, Laura R. and Campbell, Emily L. and Levitskaia, Tatiana G. and Peterson, James M. and Smith, Frances N. and Bryan, Samuel A.},
abstractNote = {Knowledge of real-time solution properties and composition is a necessity for any spent nuclear fuel reprocessing method. Metal-ligand speciation in aqueous solutions derived from the dissolved commercial spent fuel is highly dependent upon the acid concentration/pH, which influences extraction efficiency and the resulting speciation in the organic phase. Spectroscopic process monitoring capabilities, incorporated in a counter current centrifugal contactor bank, provide a pathway for on-line real-time measurement of solution pH. The spectroscopic techniques are process-friendly and can be easily configured for on-line applications, while classic potentiometric pH measurements require frequent calibration/maintenance and have poor long-term stability in aggressive chemical and radiation environments. Our research is focused on developing a general method for on-line determination of pH of aqueous solutions through chemometric analysis of Raman spectra. Interpretive quantitative models have been developed and validated under the range of chemical composition and pH using a lactic acid/lactate buffer system. The developed model was applied to spectra obtained on-line during solvent extractions performed in a centrifugal contactor bank. The model predicted the pH within 11% for pH > 2, thus demonstrating that this technique could provide the capability of monitoring pH on-line in applications such as nuclear fuel reprocessing.},
doi = {10.1021/ac504578t},
journal = {Analytical Chemistry, 87(10):5139-5147},
number = ,
volume = ,
place = {United States},
year = {2015},
month = {5}
}