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Calixarene-based extraction chromatographic separation of 135Cs and 137Cs in environmental and waste samples prior to sector field ICP-MS analysis

Calixarene-based extraction chromatographic separation of 135Cs and 137Cs in environmental and waste samples prior to sector field ICP-MS analysis
Calixarene-based extraction chromatographic separation of 135Cs and 137Cs in environmental and waste samples prior to sector field ICP-MS analysis
Advances in the sensitivities achievable by sector field inductively coupled plasma mass spectrometry (ICP-SFMS) offer the prospect of low-level measurement of shorter and longer lived radionuclides, thus expanding options for environmental and radioactively contaminated land assessment. In ICP-SFMS, the critical requirement for accurate detection is the effective chemical separation of isobaric and polyatomic interferences prior to sample introduction. As instrumental detection limit capability improves, accurate radionuclide determination requires highly effective separation materials that combine high analyte selectivity with subsequent quantitative analyte recovery compatible with ICP-SFMS detection. Two radioactive isotopes measurable by ICP-SFMS are the high yield fission products 135Cs and 137Cs that have entered the environment as a result of anthropogenic nuclear activities. ICP-SFMS enables reliable measurement of 135Cs/137Cs ratios, which can be used as a forensic tool in determining the source of nuclear contamination. The critical requirement for accurate detection is the effective removal of isobaric interferences from 135Ba and 137Ba prior to measurement. A number of exchange materials can effectively extract Cs; however, non-quantitative elution of Cs makes subsequent ICP-SFMS quantification challenging. A novel extraction chromatographic resin has been developed by dissolving calix[4]arene-bis(tert-octylbenzo-crown-6) (BOBCalixC6) in octan-1-ol and loading onto an Amberchrom CG-71 prefilter resin material. Preparation of the material takes less than 1 h and, at an optimal concentration of 3 M HNO3, shows high selectivity toward Cs, which is effectively eluted in 0.05 M HNO3. The procedure developed shows high Cs selectivity and Ba decontamination from digests of complex matrixes including a saltmarsh sediment contaminated by aqueous discharges from a nuclear fuel reprocessing facility. Repeated tests show the resin can be reused up to four times. For low-level ICP-SFMS quantification, more complex sample matrixes benefit from a cation resin cleanup stage prior to using BOBCalixC6 that serves to enhance Ba decontamination and Cs recovery.
0003-2700
11890-11896
Russell, Ben C.
856d9c75-b693-489f-88c2-1d614116688e
Warwick, Phil E.
f2675d83-eee2-40c5-b53d-fbe437f401ef
Croudace, Ian W.
24deb068-d096-485e-8a23-a32b7a68afaf
Russell, Ben C.
856d9c75-b693-489f-88c2-1d614116688e
Warwick, Phil E.
f2675d83-eee2-40c5-b53d-fbe437f401ef
Croudace, Ian W.
24deb068-d096-485e-8a23-a32b7a68afaf

Russell, Ben C., Warwick, Phil E. and Croudace, Ian W. (2014) Calixarene-based extraction chromatographic separation of 135Cs and 137Cs in environmental and waste samples prior to sector field ICP-MS analysis. Analytical Chemistry, 86 (23), 11890-11896. (doi:10.1021/ac5036988).

Record type: Article

Abstract

Advances in the sensitivities achievable by sector field inductively coupled plasma mass spectrometry (ICP-SFMS) offer the prospect of low-level measurement of shorter and longer lived radionuclides, thus expanding options for environmental and radioactively contaminated land assessment. In ICP-SFMS, the critical requirement for accurate detection is the effective chemical separation of isobaric and polyatomic interferences prior to sample introduction. As instrumental detection limit capability improves, accurate radionuclide determination requires highly effective separation materials that combine high analyte selectivity with subsequent quantitative analyte recovery compatible with ICP-SFMS detection. Two radioactive isotopes measurable by ICP-SFMS are the high yield fission products 135Cs and 137Cs that have entered the environment as a result of anthropogenic nuclear activities. ICP-SFMS enables reliable measurement of 135Cs/137Cs ratios, which can be used as a forensic tool in determining the source of nuclear contamination. The critical requirement for accurate detection is the effective removal of isobaric interferences from 135Ba and 137Ba prior to measurement. A number of exchange materials can effectively extract Cs; however, non-quantitative elution of Cs makes subsequent ICP-SFMS quantification challenging. A novel extraction chromatographic resin has been developed by dissolving calix[4]arene-bis(tert-octylbenzo-crown-6) (BOBCalixC6) in octan-1-ol and loading onto an Amberchrom CG-71 prefilter resin material. Preparation of the material takes less than 1 h and, at an optimal concentration of 3 M HNO3, shows high selectivity toward Cs, which is effectively eluted in 0.05 M HNO3. The procedure developed shows high Cs selectivity and Ba decontamination from digests of complex matrixes including a saltmarsh sediment contaminated by aqueous discharges from a nuclear fuel reprocessing facility. Repeated tests show the resin can be reused up to four times. For low-level ICP-SFMS quantification, more complex sample matrixes benefit from a cation resin cleanup stage prior to using BOBCalixC6 that serves to enhance Ba decontamination and Cs recovery.

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More information

Accepted/In Press date: 6 November 2014
e-pub ahead of print date: 6 November 2014
Published date: 2 December 2014
Organisations: Geochemistry

Identifiers

Local EPrints ID: 373105
URI: http://eprints.soton.ac.uk/id/eprint/373105
ISSN: 0003-2700
PURE UUID: 38cec8ea-b38d-44be-9c55-d9dff6a1f21d
ORCID for Phil E. Warwick: ORCID iD orcid.org/0000-0001-8774-5125

Catalogue record

Date deposited: 06 Jan 2015 14:11
Last modified: 15 Mar 2024 02:49

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Contributors

Author: Ben C. Russell
Author: Phil E. Warwick ORCID iD
Author: Ian W. Croudace

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