Quantification of Hydrogen Isotopes Utilizing Raman Spectroscopy Paired with Chemometric Analysis for Application across Multiple Systems

Felmy, Heather M.; Cox, Richard M.; Espley, Alyssa F.; Campbell, Emily L.; Campbell, Emily L.; Lackey, Hope E.; Branch, Shirmir D.; Bryan, Samuel A.; Lines, Amanda M.

doi:10.1021/acs.analchem.4c00802

Title: Quantification of Hydrogen Isotopes Utilizing Raman Spectroscopy Paired with Chemometric Analysis for Application across Multiple Systems

Journal Article · 24 April 2024 · Analytical Chemistry

DOI: https://doi.org/10.1021/acs.analchem.4c00802 · OSTI ID:2446787

^[1]; Cox, Richard M. ^[1]; Espley, Alyssa F. ^[1];

^[1];

^[1]; Lackey, Hope E. ^[1]; Branch, Shirmir D. ^[1];

^[1]; Lines, Amanda M. ^[1]

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

On-line and real-time analysis of a chemical process is a major analytical challenge that can drastically change the way the chemical industry or chemical research operates. With in situ analyses, new and powerful understanding of chemistry can be gained; however, building robust tools for long-term monitoring faces many challenges that include compensating for instrument drift, instrument replacement, and sensor or probe replacement. Accounting for these changes by recollecting calibration data and rebuilding quantification models can be costly and time consuming. Here, in this study, methods to overcome these challenges are demonstrated with an application of Raman spectroscopy to monitoring hydrogen isotopes with varied speciation within dynamic gas streams. Specifically, chemical data science tools such as chemometric modeling are leveraged along with several examples of calibration transfer approaches. Furthermore, the optimization of instrument and sensors cell parameters for targeted gas phase analyses is discussed. While the particular focus on hydrogen is highly beneficial within the nuclear energy sector, mechanisms built and demonstrated here are widely applicable to optical spectroscopy monitoring in numerous other chemical systems that can be leveraged in other hazardous processes.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS); USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2446787

Report Number(s):: PNNL-SA--194339

Journal Information:: Analytical Chemistry, Journal Name: Analytical Chemistry Journal Issue: 18 Vol. 96; ISSN 0003-2700

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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