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Extended total number density compensation for uranium determination by laser-induced breakdown spectroscopy.

Weilun Gu1, Zongyu Hou2, Weiran Song1

  • 1State Key Laboratory of Power System Operation and Control, Tsinghua-Rio Tinto Joint Research Centre for Resources, Energy and Sustainable Development, International Joint Laboratory on Low Carbon Clean Energy Innovation, Institute for Carbon Neutrality, Department of Energy and Power Engineering, Tsinghua University, Beijing, 100084, China.

Analytica Chimica Acta
|January 14, 2024
PubMed
Summary

A new method called extended total number density compensation (ETNDC) improves laser-induced breakdown spectroscopy (LIBS) for uranium determination. ETNDC reduces signal uncertainty and matrix effects, enhancing accuracy in complex samples.

Keywords:
Laser-induced breakdown spectroscopyMatrix effectsPre-processingQuantitative analysisUncertainty reductionUranium determination

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Area of Science:

  • Analytical Chemistry
  • Spectroscopy
  • Materials Science

Background:

  • Plasma property variations in laser-induced breakdown spectroscopy (LIBS) cause signal uncertainty and matrix effects.
  • Accurate compensation for total number density variation is challenging due to unreliable spectroscopic parameters.
  • Previous total number density compensation (TNDC) methods have limitations with complex samples.

Purpose of the Study:

  • To introduce an extended total number density compensation (ETNDC) method for improved LIBS analysis.
  • To reduce signal uncertainty and matrix effects in uranium determination using LIBS.
  • To enhance the accuracy and robustness of LIBS for complex sample matrices.

Main Methods:

  • Developed ETNDC by weighting spectral lines from major elements to reflect total number density variations.
  • Incorporated temperature and electron density compensation into ETNDC weighting coefficients.
  • Applied ETNDC as a pre-processing step for uranium determination in yellow cake samples using regression models.

Main Results:

  • ETNDC significantly reduced the mean relative standard deviation (RSD) of U II 417.159 nm from 4.92% to 2.27%.
  • The root mean square error of prediction (RMSEP) decreased from 4.81% to 1.93% with ETNDC.
  • ETNDC demonstrated superior average performance and robustness across multiple validation sets and line combinations compared to baseline methods.

Conclusions:

  • ETNDC is the first method to explicitly address temperature and electron density variations alongside total number density compensation.
  • Inaccurate spectroscopic parameters are avoided by fitting related quantities using concentration information.
  • ETNDC significantly improves signal repeatability and analytical performance for accurate uranium quantification via LIBS.