Comparison of Raman and mid-infrared spectroscopy for quantification of nitric acid in PUREX-relevant mixtures

被引:4
作者
McFarlan, Catriona [1 ,2 ]
Nordon, Alison [1 ,2 ]
Sarsfield, Mark [3 ]
Taylor, Robin [3 ]
Chen, Hongyan [4 ]
机构
[1] Univ Strathclyde, Dept Pure & Appl Chem, WestCHEM, 295 Cathedral St, Glasgow G1 1XL, Scotland
[2] Univ Strathclyde, Ctr Proc Analyt & Control Technol, 295 Cathedral St, Glasgow G1 1XL, Scotland
[3] Natl Nucl Lab, Cent Lab, Seascale CA20 1PG, Cumbria, England
[4] Univ Manchester, Sch Chem Engn & Analyt Sci, Oxford Rd, Manchester M13 9PL, England
关键词
Nitric acid; Liquid-liquid extraction; Process analysis; Raman spectroscopy; Mid-infrared spectroscopy; Chemometrics; BUTYL-PHOSPHATE SOLVENT; 3RD PHASE-FORMATION; MULTIVARIATE-ANALYSIS; AQUEOUS-SOLUTIONS; FT-IR; EXTRACTION; SPECIATION; COMPLEXATION; URANIUM(VI); NEPTUNIUM;
D O I
10.1016/j.pnucene.2023.104898
中图分类号
TL [原子能技术]; O571 [原子核物理学];
学科分类号
0827 ; 082701 ;
摘要
During the plutonium uranium reduction extraction (PUREX) process, nitric acid facilitates the extraction of actinides from the aqueous phase into the organic phase by forming neutral, organic soluble complexes with trin-butyl phosphate (TBP). The concentration of nitric acid is generally measured by titration; however, titration is a time-consuming method that generates significant volumes of additional waste. Optical spectroscopic techniques can be used to perform fast, automated measurements off-line or on-line, without generating any waste. In this work, the effectiveness of Raman and mid-infrared (MIR) spectroscopy has been compared for the first time as an alternative to titration for the quantification of nitric acid in PUREX-relevant mixtures. Samples of 0-12 M nitric acid in the aqueous phase and 0-1.10 M nitric acid in the organic phase (TBP/odourless kerosene (OK)- H2O-HNO3 model system) were analysed and partial least squares (PLS) regression models were built to predict nitric acid concentration. MIR spectra required less pre-processing than Raman spectra and more accurate predictions of nitric acid concentration were obtained for MIR spectroscopy than for Raman spectroscopy, with root mean square error of prediction (RMSEP) values of 0.099 M versus 0.148 M obtained for the aqueous phase and root mean square error of cross validation (RMSECV) values of 0.006 M versus 0.013 M obtained for the organic phase. To investigate the ability to predict nitric acid concentration in the presence of uranyl nitrate, samples containing uranium (0-100 g/L) and nitric acid (0.15-0.64 M) in the organic phase (U-TBP/OKH2O-HNO3 model system) were analysed by Raman and MIR spectroscopy. The RMSECV was 0.027 M and 0.066 M for MIR and Raman spectroscopy, respectively; these values are higher than those obtained in the absence of uranyl nitrate owing to differences in the experimental approaches employed. Therefore, the results obtained demonstrate that MIR or Raman spectroscopy could be used to measure the concentration of nitric acid in the organic and aqueous phases in the PUREX process.
引用
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页数:9
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