Raman Spectroscopy Based On-Line, Real-Time Monitoring to Reduce Composition Uncertainties: Enhanced sensitivity through optimization of Raman Parameters

Technical Report · Sun Aug 01 04:00:00 EDT 2021

DOI:https://doi.org/10.2172/1989700· OSTI ID:1989700

Lines, Amanda M. ^[1]; Felmy, Heather M. ^[1]; Bryan, Samuel A. ^[1]; Minette, Michael J. ^[1]

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1. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Optical spectroscopy-based on-line monitoring of Hanford processing streams can enable real-time characterization of chemical composition of process streams and batches, ultimately enabling and enhancing process control. It can provide immediate feedback on process conditions and has the potential to reduce the needed number of grab sample collections, thereby reducing times and costs associated with laboratory processing. Here we discuss the utilization of Raman spectroscopy to quantify multiple target analytes that are common within Hanford tanks and waste processing streams. Analytes include: nitrate, nitrite, carbonate, chromate, sulfate, phosphate, hydroxide, oxalate, ammonia, and aluminate. Most notably in this work, Raman applications to low-concentration streams are explored and optimized. Raman instrument specifications are compared; specifically, the impact of utilizing three different Raman excitation wavelengths, 405, 532, and 671 nm, is discussed. Also, Raman data collection parameters such as collection time and spectral averaging are measured and discussed. Finally, optical libraries of chemical targets were collected using optimized collection parameters and chemometric models were built to automate quantification of chemical targets. These models were validated through application to simulants and real Hanford process samples. Chemometric models performed well on both training and validation sets, suggesting these approaches can be successfully applied to on-line and real-time monitoring of low concentration Hanford processing streams. The use of the combine Raman wave lengths with the enhanced chemometric models for the low concentration streams significantly improved the chemical detection levels and significantly reduced uncertainties of those measurements.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); USDOE Office of River Protection (ORP), Richland, WA (United States)
• Sponsoring Organization: USDOE Office of Environmental Management (EM)
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1989700
• Report Number(s): PNNL--31681
• Country of Publication: United States
• Language: English

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