Internal correction of spectral interferences and mass bias for selenium metabolism studies using enriched stabel isotopes in combination with multiple linear regression

Kristoffer Lunøe; Justo Giner  Martinez-Sierra; Bente Gammelgaard; J. Ignacio Garcia Alonso

doi:10.1007/s00216-012-5747-7

Internal correction of spectral interferences and mass bias for selenium metabolism studies using enriched stabel isotopes in combination with multiple linear regression

Kristoffer Lunøe, Justo Giner Martinez-Sierra, Bente Gammelgaard, J. Ignacio Garcia Alonso

9 Citationer (Scopus)

Abstract

The analytical methodology for the in vivo study of selenium metabolism using two enriched selenium isotopes has been modified, allowing for the internal correction of spectral interferences and mass bias both for total selenium and speciation analysis. The method is based on the combination of an already described dual-isotope procedure with a new data treatment strategy based on multiple linear regression. A metabolic enriched isotope ( ⁷⁷Se) is given orally to the test subject and a second isotope ( ⁷⁴Se) is employed for quantification. In our approach, all possible polyatomic interferences occurring in the measurement of the isotope composition of selenium by collision cell quadrupole ICP-MS are taken into account and their relative contribution calculated by multiple linear regression after minimisation of the residuals. As a result, all spectral interferences and mass bias are corrected internally allowing the fast and independent quantification of natural abundance selenium ( ^natSe) and enriched ⁷⁷Se. In this sense, the calculation of the tracer/tracee ratio in each sample is straightforward. The method has been applied to study the time-related tissue incorporation of ⁷⁷Se in male Wistar rats while maintaining the ^natSe steady-state conditions. Additionally, metabolically relevant information such as selenoprotein synthesis and selenium elimination in urine could be studied using the proposed methodology. In this case, serum proteins were separated by affinity chromatography while reverse phase was employed for urine metabolites. In both cases, ⁷⁴Se was used as a post-column isotope dilution spike. The application of multiple linear regression to the whole chromatogram allowed us to calculate the contribution of bromine hydride, selenium hydride, argon polyatomics and mass bias on the observed selenium isotope patterns. By minimising the square sum of residuals for the whole chromatogram, internal correction of spectral interferences and mass bias could be accomplished. As a result, the tracer/tracee ratio could be calculated for each selenium-containing species and a time relationship for synthesis and degradation established. Both selenite and selenized yeast labelled with ⁷⁷Se were employed for comparative purposes.

Originalsprog	Engelsk
Tidsskrift	Analytical and Bioanalytical Chemistry
Vol/bind	402
Udgave nummer	9
Sider (fra-til)	2749-2763
ISSN	1618-2642
DOI	https://doi.org/10.1007/s00216-012-5747-7
Status	Udgivet - mar. 2012

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10.1007/s00216-012-5747-7

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Internal correction of spectral interferences and mass bias for selenium metabolism studies using enriched stabel isotopes in combination with multiple linear regression. / Lunøe, Kristoffer; Martinez-Sierra, Justo Giner ; Gammelgaard, Bente et al.

I: Analytical and Bioanalytical Chemistry, Bind 402, Nr. 9, 03.2012, s. 2749-2763.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review

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title = "Internal correction of spectral interferences and mass bias for selenium metabolism studies using enriched stabel isotopes in combination with multiple linear regression",

abstract = "The analytical methodology for the in vivo study of selenium metabolism using two enriched selenium isotopes has been modified, allowing for the internal correction of spectral interferences and mass bias both for total selenium and speciation analysis. The method is based on the combination of an already described dual-isotope procedure with a new data treatment strategy based on multiple linear regression. A metabolic enriched isotope ( 77Se) is given orally to the test subject and a second isotope ( 74Se) is employed for quantification. In our approach, all possible polyatomic interferences occurring in the measurement of the isotope composition of selenium by collision cell quadrupole ICP-MS are taken into account and their relative contribution calculated by multiple linear regression after minimisation of the residuals. As a result, all spectral interferences and mass bias are corrected internally allowing the fast and independent quantification of natural abundance selenium ( natSe) and enriched 77Se. In this sense, the calculation of the tracer/tracee ratio in each sample is straightforward. The method has been applied to study the time-related tissue incorporation of 77Se in male Wistar rats while maintaining the natSe steady-state conditions. Additionally, metabolically relevant information such as selenoprotein synthesis and selenium elimination in urine could be studied using the proposed methodology. In this case, serum proteins were separated by affinity chromatography while reverse phase was employed for urine metabolites. In both cases, 74Se was used as a post-column isotope dilution spike. The application of multiple linear regression to the whole chromatogram allowed us to calculate the contribution of bromine hydride, selenium hydride, argon polyatomics and mass bias on the observed selenium isotope patterns. By minimising the square sum of residuals for the whole chromatogram, internal correction of spectral interferences and mass bias could be accomplished. As a result, the tracer/tracee ratio could be calculated for each selenium-containing species and a time relationship for synthesis and degradation established. Both selenite and selenized yeast labelled with 77Se were employed for comparative purposes.",

keywords = "Former Faculty of Pharmaceutical Sciences",

author = "Kristoffer Lun{\o}e and Martinez-Sierra, {Justo Giner} and Bente Gammelgaard and Alonso, {J. Ignacio Garcia}",

year = "2012",

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doi = "10.1007/s00216-012-5747-7",

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T1 - Internal correction of spectral interferences and mass bias for selenium metabolism studies using enriched stabel isotopes in combination with multiple linear regression

AU - Lunøe, Kristoffer

AU - Martinez-Sierra, Justo Giner

AU - Gammelgaard, Bente

AU - Alonso, J. Ignacio Garcia

PY - 2012/3

Y1 - 2012/3

N2 - The analytical methodology for the in vivo study of selenium metabolism using two enriched selenium isotopes has been modified, allowing for the internal correction of spectral interferences and mass bias both for total selenium and speciation analysis. The method is based on the combination of an already described dual-isotope procedure with a new data treatment strategy based on multiple linear regression. A metabolic enriched isotope ( 77Se) is given orally to the test subject and a second isotope ( 74Se) is employed for quantification. In our approach, all possible polyatomic interferences occurring in the measurement of the isotope composition of selenium by collision cell quadrupole ICP-MS are taken into account and their relative contribution calculated by multiple linear regression after minimisation of the residuals. As a result, all spectral interferences and mass bias are corrected internally allowing the fast and independent quantification of natural abundance selenium ( natSe) and enriched 77Se. In this sense, the calculation of the tracer/tracee ratio in each sample is straightforward. The method has been applied to study the time-related tissue incorporation of 77Se in male Wistar rats while maintaining the natSe steady-state conditions. Additionally, metabolically relevant information such as selenoprotein synthesis and selenium elimination in urine could be studied using the proposed methodology. In this case, serum proteins were separated by affinity chromatography while reverse phase was employed for urine metabolites. In both cases, 74Se was used as a post-column isotope dilution spike. The application of multiple linear regression to the whole chromatogram allowed us to calculate the contribution of bromine hydride, selenium hydride, argon polyatomics and mass bias on the observed selenium isotope patterns. By minimising the square sum of residuals for the whole chromatogram, internal correction of spectral interferences and mass bias could be accomplished. As a result, the tracer/tracee ratio could be calculated for each selenium-containing species and a time relationship for synthesis and degradation established. Both selenite and selenized yeast labelled with 77Se were employed for comparative purposes.

AB - The analytical methodology for the in vivo study of selenium metabolism using two enriched selenium isotopes has been modified, allowing for the internal correction of spectral interferences and mass bias both for total selenium and speciation analysis. The method is based on the combination of an already described dual-isotope procedure with a new data treatment strategy based on multiple linear regression. A metabolic enriched isotope ( 77Se) is given orally to the test subject and a second isotope ( 74Se) is employed for quantification. In our approach, all possible polyatomic interferences occurring in the measurement of the isotope composition of selenium by collision cell quadrupole ICP-MS are taken into account and their relative contribution calculated by multiple linear regression after minimisation of the residuals. As a result, all spectral interferences and mass bias are corrected internally allowing the fast and independent quantification of natural abundance selenium ( natSe) and enriched 77Se. In this sense, the calculation of the tracer/tracee ratio in each sample is straightforward. The method has been applied to study the time-related tissue incorporation of 77Se in male Wistar rats while maintaining the natSe steady-state conditions. Additionally, metabolically relevant information such as selenoprotein synthesis and selenium elimination in urine could be studied using the proposed methodology. In this case, serum proteins were separated by affinity chromatography while reverse phase was employed for urine metabolites. In both cases, 74Se was used as a post-column isotope dilution spike. The application of multiple linear regression to the whole chromatogram allowed us to calculate the contribution of bromine hydride, selenium hydride, argon polyatomics and mass bias on the observed selenium isotope patterns. By minimising the square sum of residuals for the whole chromatogram, internal correction of spectral interferences and mass bias could be accomplished. As a result, the tracer/tracee ratio could be calculated for each selenium-containing species and a time relationship for synthesis and degradation established. Both selenite and selenized yeast labelled with 77Se were employed for comparative purposes.

KW - Former Faculty of Pharmaceutical Sciences

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DO - 10.1007/s00216-012-5747-7

M3 - Journal article

C2 - 22349322

SN - 1618-2642

VL - 402

SP - 2749

EP - 2763

JO - Analytical and Bioanalytical Chemistry

JF - Analytical and Bioanalytical Chemistry

IS - 9

ER -

Internal correction of spectral interferences and mass bias for selenium metabolism studies using enriched stabel isotopes in combination with multiple linear regression

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