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High-sensitivity thiocyanate spectrophotometric method for determination of perrhenate, an analogue of radioactive pertechnetate, under acidic condition

  • Hui Hu
  • Long-Li Sun
  • Yan-Ling Gao
  • Tian Wang
  • Yue-Fei Zhang
  • Hui-Xiong Wu
  • Xiao-Hui Chen
Original Paper
  • 15 Downloads

Abstract

Spectrophotometric method is a simple and effective in situ analytical method for contaminants monitoring, but further improvement of its sensitivity and detection limit for radionuclides determination remains highly desirable. Herein, we report a simple and highly sensitive thiocyanate spectrophotometric method for the determination of radioactive Tc(VII) by studying its chemical analogue Re(VII) in different aqueous media. The colorless thiocyanate reacted with Re(VII) in hydrochloric acid solution in the presence of SnCl2 producing a stable colored Re(IV)-SCN complex, which was extracted into ethyl acetate and then measured at 427 nm. Under optimized conditions, a strong linear relationship can be obtained in the range of 0.25–10 mg L−1 for Re(VII) with R2 value > 0.9942, and the sensitivity of the method was found to be 0.004 μg cm−2 with detection limit of 0.027 mg L−1. This assay provides highly sensitive detection of Re(VII) in environmental media that is high in NO3, Cu2+, and Fe3+. We applied it to the determination of Re(VII) in the wide range of background solutions, including deionized water, groundwater, and seawater, and analysis results showed that none of the molar absorptivities for both groundwater and seawater backgrounds was statistically different from the deionized water background when the paired Student’s t test, at 95% confidence level, was applied. The operational simplicity, accuracy, and precision of the proposed method suggest that it can be a good alternative for the in situ analysis of pertechnetate in environmental media.

Keywords

Pertechnetate Spectrophotometry Thiocyanate High sensitivity In situ analysis 

Supplementary material

11696_2018_660_MOESM1_ESM.doc (10.1 mb)
Supplementary material 1 (DOC 10370 kb)

References

  1. Acox TA (1983) Proc. 4th DOE environmental protection information meeting. CONF-821215, 77–85Google Scholar
  2. Agnihotri P, Deb M, Thakur M, Mishra R (1998) Spectrophotometric determination of rhenium with thiocyanate, TX-100 and N,N’’-diphenyl-benzamidine. J Chin Chem Soc 45:401–406.  https://doi.org/10.1002/jccs.199800063 CrossRefGoogle Scholar
  3. Alamdari EK, Sadrnezhaad SK, Shabestari ZM (2005) Chloroform aided extraction spectrophotometric determination of rhenium using thiocyanate complexing agent. J Mater Sci Technol 21:239–242Google Scholar
  4. Asmussen RM, Pearce CI, Miller BW, Lawter AR, Neeway JJ, Lukens WW, Bowden ME, Miller MA, Buck EC, Serne RJ, Qafoku NP (2018) Getters for improved technetium containment in cementitious waste forms. J Hazard Mater 341:238–247.  https://doi.org/10.1016/j.jhazmat.2017.07.055 CrossRefPubMedGoogle Scholar
  5. Banerjee D, Kim D, Schweiger MJ, Kruger AA, Thallapally PK (2016) Removal of TcO4 ions from solution: materials and future outlook. Chem Soc Rev 45:2724–2739.  https://doi.org/10.1039/c5cs00330j CrossRefPubMedGoogle Scholar
  6. Bao Y, Grutzeck MW, Jantzen CM (2005) Preparation and properties of hydroceramic waste forms made with simulated hanford low-activity waste. J Am Ceram Soc 88:3287–3302.  https://doi.org/10.1111/j.1551-2916.2005.00775.x CrossRefGoogle Scholar
  7. Bard AJ, Parsons R, Jordan J (1985) Standard potentials in aqueous solution. Marcel Dekker, New YorkGoogle Scholar
  8. Bonnesen PV, Brown GM, Alexandratos SD, Bavoux LB, Presley DJ (2000) Development of bifunctional anion-exchange resins with improved selectivity and sorptive kinetics for pertechnetate: batch-equilibrium experiments. Environ Sci Technol 34:3761–3766.  https://doi.org/10.1021/es990858s CrossRefGoogle Scholar
  9. Bozhko OD, Jordano N, Borikwa LV (1988) Spectrophotometric determination of rhenium with dithio-oxamide in strongly alkaline medium. Talanta 35:62–64.  https://doi.org/10.1016/0039-9140(88)80014-6 CrossRefGoogle Scholar
  10. Burns DT, Tungkananuruk N (1988) Spectrophotometric determination of rhenium as perrhenate after extraction of its brilliant green ion-pair with microcrystalline benzophenone. Anal Chim Acta 204:359–363.  https://doi.org/10.1016/s0003-2670(00)86376-X CrossRefGoogle Scholar
  11. del Cul GD, Bostick WD, Trotter DR, Osborne PE (1993) Technetium-99 removal from process solutions and contaminated groundwater. Sep Sci Technol 28:551–564CrossRefGoogle Scholar
  12. Dutta G, Sur B (1986) Spectrophotometric determination of rhenium using 2-pyridyl thiourea. Mikrochim Acta 1:359–369.  https://doi.org/10.1007/bf01206730 CrossRefGoogle Scholar
  13. Evdokimova OV, Pechishcheva NV, Shunyaev KY (2012) Up-to-date methods for the determination of rhenium. J Anal Chem 67:741–753.  https://doi.org/10.1134/s1061934812090043 CrossRefGoogle Scholar
  14. Evdokimova O, Zaitceva P, Pechishcheva N, Pupyshev A, Shunyaev K (2014) The rhenium determination in copper and molybdenum oresand concentrates by ICP atomic emission spectrometry. Curr Anal Chem 10:449–456.  https://doi.org/10.2174/157341101004140701102351 CrossRefGoogle Scholar
  15. Gangopadhyay S, Gangopadhyay P, Shome S (1976) Spectrophotometric determination of rhenium with thiobenzhydrazide. Anal Chim Acta 83:409–413.  https://doi.org/10.1016/s0003-2670(01)84673-0 CrossRefGoogle Scholar
  16. Hu H, Jiang B, Wu H, Zhang J, Chen X (2016) Bamboo (Acidosasa edulis) shoot shell biochar: its potential isolation and mechanism to perrhenate as a chemical surrogate for pertechnetate. J Environ Radioact 165:39–46.  https://doi.org/10.1016/j.jenvrad.2016.09.004 CrossRefPubMedGoogle Scholar
  17. Jones E, Munkley CG, Philips ED, Stedman G (1996) Kinetics and equilibria in the nitric acid-nitrous acid-sodium thiocyanate system. J Chem Soc Dalton Trans 9:1915–1920CrossRefGoogle Scholar
  18. Karadjov M, Velitchkova N, Veleva O, Velichkov S, Markov P, Daskalova N (2016) Spectral interferences in the determination of rhenium in molybdenum and copper concentrates by inductively coupled plasma optical emission spectrometry (ICP-OES). Spectrochim Acta B 119:76–82.  https://doi.org/10.1016/j.sab.2016.03.011 CrossRefGoogle Scholar
  19. Klofutar C, Podobnik B, Krasovee F, Stular V (1969) Spectrophotometric determination of rhenium in the presence of molybdenum and tungsten. Microchim Acta 4:758–763.  https://doi.org/10.1007/bf01216310 CrossRefGoogle Scholar
  20. Lee CH, Lee MH, Han SH, Ha YK, Kyuseok S (2011) Systematic radiochemical separation for the determination of 99Tc, 90Sr, 94Nb, 55Fe and 59,63Ni in low and intermediate radioactive waste samples. J Radioanal Nucl Chem 288:319–325.  https://doi.org/10.1007/s10967-011-0984-3 CrossRefGoogle Scholar
  21. Lenell BA, Arai Y (2016) Evaluation of perrhenate spectrophotometric methods in bicarbonate and nitrate media. Talanta 150:690–698.  https://doi.org/10.1016/j.talanta.2015.10.063 CrossRefPubMedGoogle Scholar
  22. Levitskaia TG, Chatterjee S, Pence NK, Romero J, Varga T, Engelhard MH, Du Y, Kovarik L, Arey BW, Bowden ME, Walter ED (2016) Inorganic tin aluminophosphate nanocomposite for reductive separation of pertechnetate. Environ Sci Nano 3:1003–1013.  https://doi.org/10.1039/C6EN00130K CrossRefGoogle Scholar
  23. Li J, Zhong LF, Tu XL, Liang XR, Xu JF (2010) Determination of rhenium content in molybdenite by ICP-MS after separation of the major matrix by solvent extraction with N-benzoyl-N-phenylhydroxalamine. Talanta 81:954–958.  https://doi.org/10.1016/j.talanta.2010.01.043 CrossRefPubMedGoogle Scholar
  24. Pegg IL (2015) Behavior of technetium in nuclear waste vitrification processes. J Radioanal Nucl Chem 305:287–292.  https://doi.org/10.1007/s10967-014-3900-9 CrossRefPubMedPubMedCentralGoogle Scholar
  25. Pepper SE, Ogden MD (2013) Perrhenate extraction studies by Cyphos 101-IL; screening for implementation in technetium removal. Sep Purif Technol 118:847–852.  https://doi.org/10.1016/j.seppur.2013.08.029 CrossRefGoogle Scholar
  26. Rayson MS, Mackie JC, Kennedy EM, Dlugogorski BZ (2011) Experimental study of decomposition of aqueous nitrosyl thiocyanate. Inorg Chem 50:7440–7452.  https://doi.org/10.1021/ic102445d CrossRefPubMedGoogle Scholar
  27. Savariar CP, Hariharan TR (1975) An extraction-spectrophotometric method for the determination of rhenium using mixed ligands. Microchim Acta 63:477–483.  https://doi.org/10.1007/bf01217310 CrossRefGoogle Scholar
  28. Seliman AF, Helariutta K, Wiktorowicz SJ, Tenhu H, Harjula R (2013) Stable and selective scintillating anion-exchange sensors for quantification of 99TcO4 in natural freshwaters. J Environ Radioact 126:156–164.  https://doi.org/10.1016/j.jenvrad.2013.07.025 CrossRefPubMedGoogle Scholar
  29. Stedman G, Whincup PAE (1963) The equilibrium constant for the formation of nitrosyl thiocyanate in aqueous solution. J Chem Soc 56:5796–5799.  https://doi.org/10.1039/jr9630005796 CrossRefGoogle Scholar
  30. Tagami K, Uchida S (2007) Determination of rhenium in manganese nodules by inductively coupled plasma mass spectrometry. J Radioanal Nucl Chem 273:147–150.  https://doi.org/10.1007/s10967-007-0726-8 CrossRefGoogle Scholar
  31. Thompson RJ, Gore RH, Trusell F (1964) Methyl-2-pyridyl ketoxime as a colorimetric regent for rhenium. Anal Chim Acta 3:590–594.  https://doi.org/10.1016/s0003-2670(00)88880-7 CrossRefGoogle Scholar
  32. Um W, Chang HS, Icenhower JP, Lukens WW, Serne RJ, Qafoku NP, Westsik JH, Buck EC, Smith SC (2011) Immobilization of 99-technetium (VII) by Fe(II)-goethite and limited reoxidation. Environ Sci Technol 45:4904–4913.  https://doi.org/10.1021/es104343p CrossRefPubMedGoogle Scholar
  33. Vorlicek TP, Chappaz A, Groskreutz LM, Young N, Lyons TW (2015) A new analytical approach to determining Mo and Re speciation in sulfidic waters. Chem Geol 403:52–57.  https://doi.org/10.1016/j.chemgeo.2015.03.003 CrossRefGoogle Scholar
  34. Wahi A, Kakkar LR (1993) Extractive-photometric determination of rhenium with dimethylglyoxime and thiocyanate ion. Anal Sci 9:409–413.  https://doi.org/10.2116/analsci.9.409 CrossRefGoogle Scholar
  35. Wang L, Tang L, Yang T, Yang Y, Yang L (2012) Determination of technetium-99 from complex matrix. J Radioanal Nucl Chem 296:739–742.  https://doi.org/10.1007/s10967-012-2023-4 CrossRefGoogle Scholar
  36. Zhang Q, Zhu H, Chang Z, Luo Z, Bai X, Li D (2016) A quantitative method study on pertechnetate in aqueous solution using Raman spectroscopy. Anal Methods 8:1549–1556.  https://doi.org/10.1039/C5AY03254G CrossRefGoogle Scholar

Copyright information

© Institute of Chemistry, Slovak Academy of Sciences 2018

Authors and Affiliations

  • Hui Hu
    • 1
  • Long-Li Sun
    • 1
  • Yan-Ling Gao
    • 1
  • Tian Wang
    • 2
  • Yue-Fei Zhang
    • 3
  • Hui-Xiong Wu
    • 4
  • Xiao-Hui Chen
    • 1
  1. 1.School of Chemical EngineeringFuzhou UniversityFuzhouChina
  2. 2.Army Infantry CollegeNanchangChina
  3. 3.School of Chemistry and Biological EngineeringChangsha University of Science and TechnologyChangshaChina
  4. 4.Hualu Engineering and Technology Co., LTDShanxiChina

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