Citation: Dan Zhou, Liangjin Bao, Haoqi Long, Duo Zhou, Yuwei Xu, Bo Wang, Chuanqin Xia, Liang Xian, Chengbin Zheng. Capillary electrophoresis as sample introduction system for highly sensitive and interference-free determination of ⁹⁹Tc by ICP-MS[J]. Chinese Chemical Letters, ;2025, 36(4): 110093. doi: 10.1016/j.cclet.2024.110093 shu

Capillary electrophoresis as sample introduction system for highly sensitive and interference-free determination of ⁹⁹Tc by ICP-MS

Dan Zhou ^{a, c} ,
Liangjin Bao ^b ,
Haoqi Long ^b ,
Duo Zhou ^b ,
Yuwei Xu ^b ,
Bo Wang ^b ,
Chuanqin Xia ^a ,
Liang Xian ^{b, *,} ,
Chengbin Zheng ^{a, *,}

a.
Key Laboratory of Green Chemistry & Technology of MOE, College of Chemistry, Sichuan University, Chengdu 610064, China
b.
Department of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, China
c.
State Key Laboratory of Radiation Medicine and Protection, School of Radiation Medicine and Protection, Collaborative Innovation Center of Radiological Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, China

13552063239@139.com

abinscu@scu.edu.cn

Received Date: 29 January 2024
Revised Date: 23 May 2024
Accepted Date: 5 June 2024
Available Online: 5 June 2024

Figures(3)

Although inductively coupled plasma mass spectrometry (ICP-MS) retains high sensitivity and has been intensively used for the measurement of ⁹⁹Tc, it usually suffers from tedious, expensive, and time-consuming sample pretreatments due to the isobaric interferences from ⁹⁹Ru and ⁹⁸Mo¹H. Herein, capillary electrophoresis (CE) was applied as sample introduction system for the sensitive, and interference-free determination of ⁹⁹TcO₄^- from RuO₄^-, and MoO₄^2- by ICP-MS with a simple sample treatment. Compared to the conventional methods, the hyphenated CE-ICP-MS avoids the use of expensive separation resins and reduces the consumption of mineral acid, representing a simpler, more efficient and environmentally benign approach. Moreover, the proposed method exhibits higher accuracy compared with the mathematical correction method using the natural isotope ratio of ⁹⁹Ru and ¹⁰¹Ru, and significantly reduces sample consumption and the amount of waste, thus remarkably alleviating the radioactive exposure to operators and the pressure of radioactive waste treatment. Under the optimized conditions, the detection limits of 25 µg/L and 0.06 µg/L were obtained for RuO₄^- and ReO₄^- (Tc was replaced by Re), respectively, with relative standard deviation (RSD) lower than 5%. In addition, efficient recoveries of RuO₄^-, ReO₄^-, and ⁹⁹TcO₄^- from simulated Hanford site groundwater were achieved. The method is expected to be a promising candidate for sensitive and accurate analysis of ⁹⁹Tc from contaminated environmental samples.
1. [1]
  M. García-León, J. Nucl. Radiochem. Sci. 6 (2005) 253–259.
2. [2]
  A.H. Meena, Y. Arai, Environ. Chem. Lett. 15 (2017) 241–263. doi: 10.1007/s10311-017-0605-7
3. [3]
  J.P. Icenhower, N.P. Qafoku, J.M. Zachara, W.J. Martin, Am. J. Sci. 310 (2010) 721–752. doi: 10.2475/08.2010.02
4. [4]
  K.L. Shi, X.L. Hou, P. Roos, W.S. Wu, Anal. Chim. Acta 709 (2012) 1–20.
5. [5]
  H. Ji, Y. Zhu, J. Duan, et al., Chin. Chem. Lett. 30 (2019) 2163–2168. doi: 10.1016/j.cclet.2019.06.004
6. [6]
  K.L. Shi, X.L. Hou, P. Roos, W.S. Wu, Anal. Chem. 84 (2012) 2009–2016. doi: 10.1021/ac203139q
7. [7]
  S.M. Keogh, A. Aldahan, G. Possnert, et al., J. Environ. Radioact. 95 (2007) 23–38. doi: 10.1016/j.jenvrad.2007.01.009
8. [8]
  E.H. Schulte, P. Scoppa, Sci. Total Environ. 64 (1987) 163–179.
9. [9]
  D.M. LaSage, A.E. Fryar, A. Mukherjee, N.C. Sturchio, L.J. Heraty, J. Hydrol. 360 (2008) 265–280.
10. [10]
  Q.J. Chen, H. Dahlgaard, H.J.M. Hansen, A. Aarkrog, Anal. Chim. Acta 228 (1990) 163–167.
11. [11]
  F. Wigley, P.E. Warwick, I.W. Croudace, J. Caborn, A.L. Sanchez, Anal. Chim. Acta 380 (1999) 73–82.
12. [12]
  S. Foti, E. Delucchi, V. Akamian, Anal. Chim. Acta 60 (1972) 269–276. doi: 10.1016/S0003-2670(01)95002-0
13. [13]
  X.L. Hou, P. Roos, Anal. Chim. Acta 608 (2008) 105–39. doi: 10.1016/j.aca.2007.12.012
14. [14]
  K. Tagami, S. Uchida, T. Hamilton, W. Robison, Appl. Radiat. Isot. 53 (2000) 75–9.
15. [15]
  L. Skipperud, D.H. Oughton, L.S. Rosten, et al., J. Environ. Radioact. 98 (2007) 251–263.
16. [16]
  L. Yang, W.T. Bu, K. Xiong, Y.Q. Yang, T.Z. Yang, Spectrochim. Acta B 198 (2022) 106564.
17. [17]
  B.C. Russell, P.E. Warwick, H. Mohamud, et al., J. Anal. At. Spectrom. 38 (2023) 97–110. doi: 10.1039/d2ja00174h
18. [18]
  W.T. Bu, L. Yang, L. Tang, et al., J. Anal. At. Spectrom. 37 (2022) 1174–1178. doi: 10.1039/d2ja00104g
19. [19]
  S.W. Downey, N.S. Nogar, C.M. Miller, Int. J. Mass Spectrom. Ion Process 61 (1984) 337–345.
20. [20]
  L.X. Wang, L. Tang, T.Z. Yang, Y.Q. Yang, L. Yang, J. Radioanal. Nucl. Chem. 296 (2013) 739–742. doi: 10.1007/s10967-012-2023-4
21. [21]
  P. Dixon, D.B. Curtis, J. Musgrave, et al., Anal. Chem. 69 (1997) 1692–1699. doi: 10.1021/ac961159q
22. [22]
  B.A. Bergquist, A.A. Marchetti, R.E. Martinelli, et al., Nucl. Instrum. Meth. Phy. Res. B 172 (2000) 328–332. doi: 10.1016/S0168-583X(00)00084-7
23. [23]
  K.L. Shi, X.L. Hou, J.X. Qiao, et al., Anal. Chem. 88 (2016) 11931–11937. doi: 10.1021/acs.analchem.6b03837
24. [24]
  M.A. French, H. Zhang, J.M. Pates, S.E. Bryan, R.C. Wilson, Anal. Chem. 77 (2005) 135–139. doi: 10.1021/ac048774b
25. [25]
  J.M. Más, M. Garcia-León, J.P. Bolívar, Nucl. Instrum. Meth. Phy. Res. A 484 (2002) 660–667. doi: 10.1016/S0168-9002(01)02031-9
26. [26]
  J.H. Chao, C.L. Tseng, C.J. Lee, J. Radioanal. Nucl. Chem. 251 (2002) 105–112. doi: 10.1023/A:1015054529857
27. [27]
  J.C. Butterworth, F.R. Livens, P.R. Makinson, Sci. Total Environ. 173/174 (1995) 293–300. doi: 10.1016/0048-9697(95)04774-3
28. [28]
  J.L. Mas, M. García-León, J.P. Bolívar, Appl. Radiat. Isot. 64 (2006) 502–507. doi: 10.1016/j.apradiso.2005.11.005
29. [29]
  C.S. Dileep, P. Jagasia, P.S. Dhami, et al., Desalination 232 (2008) 157–165. doi: 10.1016/j.desal.2007.11.053
30. [30]
  S.B. Jenkinson, D. McCubbin, P.H.W. Kennedy, et al., J. Environ. Radioact. 133 (2014) 40–47. doi: 10.1016/j.jenvrad.2013.05.004
31. [31]
  H. Sahli, S. Röllin, J.A.C. Alvarado, J. Radioanal. Nucl. Chem. 311 (2017) 1633–1642. doi: 10.1007/s10967-016-5145-2
32. [32]
  K.L. Shi, J.X. Qiao, W.S. Wu, P. Roos, X.L. Hou, Anal. Chem. 84 (2012) 6783–6789. doi: 10.1021/ac301319a
33. [33]
  K. Kołacińska, M. Trojanowicz, Talanta 125 (2014) 131–145. doi: 10.1016/j.talanta.2014.02.057
34. [34]
  Y. Jiang, M.Y. He, W.J. Zhang, et al., Chin. Chem. Lett. 28 (2017) 1640–1652. doi: 10.1016/j.cclet.2017.05.008
35. [35]
  R. Rodríguez, L. Leal, S. Miranda, et al., Talanta 133 (2015) 88–93. doi: 10.1097/01.ccm.0000474175.19795.59
36. [36]
  S. Walas, K. Kleszcz, A. Tobiasz, H. Mrowiec, J.W. Mietelski, Anal. Lett. 49 (2016) 2755–2765. doi: 10.1080/00032719.2016.1156119
37. [37]
  M. Matsueda, K. Yanagisawa, K. Koarai, et al., ACS Omega 6 (2021) 19281–19290. doi: 10.1021/acsomega.1c02756
38. [38]
  C.K. Kim, C.S. Kim, B.H. Rho, J.I. Lee, J. Radioanal. Nucl. Chem. 252 (2002) 421–427. doi: 10.1023/A:1015799229683
39. [39]
  O. Egorov, M.J. O'Hara, J. Ruzicka, J.W. Grate, Anal. Chem. 70 (1998) 977–984. doi: 10.1021/ac971121t
40. [40]
  S. Diez-Fernández, H. Isnard, A. Nonell, C. Bresson, F. Chartier, J. Anal. At. Spectrom. 35 (2020) 2793–2819. doi: 10.1039/d0ja00211a
41. [41]
  C. Willberger, D. Leichtfuß, S. Amayri, T. Reich, Inorg. Chem. 58 (2019) 4851–4858. doi: 10.1021/acs.inorgchem.8b03407
42. [42]
  C. Willberger, S. Amayri, V. Haußler, R. Scholze, T. Reic, Anal. Chem. 91 (2019) 11537–11543. doi: 10.1021/acs.analchem.9b00997
43. [43]
  L. Li, X.Q. Xue, H.G. Zhang, et al., Chin. Chem. Lett. 32 (2021) 2139–2142. doi: 10.1016/j.cclet.2020.11.022
44. [44]
  X.L. Liu, F. Poineau, M. Fattahi, B. Grambow, L. Vichot, Radiochim. Acta 93 (2005) 305–309. doi: 10.1524/ract.93.5.305.64276
45. [45]
  T. Haraga, K. Ouchi, Y. Sato, et al., Anal. Chim. Acta 1032 (2018) 188–196. doi: 10.1016/j.aca.2018.05.077
46. [46]
  E. Ianovici, M. Kosinski, P. Lerch, A.G. Maddoc, J. Radioanal. Chem. 64 (1981) 315–326.
47. [47]
  B. Fourest, A. Maslennikov, F. David, M. Masson, Radiochim. Acta 91 (2003) 479–485.
48. [48]
  E.W. Mei, H. Ichihashi, W.F. Gu, S. Yamasaki, Anal. Chem. 69 (1997) 2187–2192.
49. [49]
  G. Álvarez-Llamas, M.D.R.F. D laCampa, A. Sanz-Medel, Trends Analyt. Chem. 24 (2005) 28–36.
50. [50]
  J.W. Olesik, J.A. Kinzer, S.V. Olesik, Anal. Chem. 67 (1995) 1–12. doi: 10.1021/ac00097a003
51. [51]
  E.A. Katayev, G.V. Kolesnikov, J.L. Sessler, Chem. Soc. Rev. 38 (2009) 1572–1586. doi: 10.1039/b806468g
52. [52]
  D. Banerjee, D. Kim, M.J. Schweiger, A.A. Krugerc, P.K. Thallapally, Chem. Soc. Rev. 45 (2016) 2724–2739.
53. [53]
  E.A. EL-Ghany, F.F. Attia, F. Marzouk, M.T. EL-Kolaly, J. Radioanal. Nucl. Chem. 245 (2000) 237–242.
54. [54]
  D. Zhou, Y. Lin, H.Q. Long, et al., Spectrochim. Acta B 180 (2021) 106211.
55. [55]
  I.I. Stewart, J.W. Olesik, J. Chromatogr. A 872 (2000) 227–246.
56. [56]
  L.H. Liu, Z.J. Yun, B. He, G.B. Jiang, Anal. Chem. 86 (2014) 8167–8175. doi: 10.1021/ac501347d
57. [57]
  Z.K. Shihabi, J. Chromatogr. A 902 (2000) 107–117.
58. [58]
  S.R. Wallenborg, L. Nyholm, C.E. Lunte, Anal. Chem. 71 (1999) 544–549.
59. [59]
  X.F. Guo, Z.H. Wang, S.P. Zhou, Talanta 64 (2004) 135–139.
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Capillary electrophoresis as sample introduction system for highly sensitive and interference-free determination of 99Tc by ICP-MS

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Capillary electrophoresis as sample introduction system for highly sensitive and interference-free determination of ⁹⁹Tc by ICP-MS