Systematic study of the selenium fractionation in human plasma from a cancer prevention trial using HPLC hyphenated to I
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RESEARCH PAPER
Systematic study of the selenium fractionation in human plasma from a cancer prevention trial using HPLC hyphenated to ICP-MS and ESI-MS/MS Christian L. Ward-Deitrich 1 & Emily Whyte 1 & Christopher Hopley 1 & Margaret P. Rayman 2 & Yasumitsu Ogra 3 & Heidi Goenaga-Infante 1 Received: 22 July 2020 / Revised: 10 September 2020 / Accepted: 5 October 2020 # Springer-Verlag GmbH Germany, part of Springer Nature 2020
Abstract This work represents the first systematic speciation study of selenium (Se) in plasma from subjects participating in a pilot study for a cancer prevention trial (PRECISE). This involved supplementation of elderly British and Danish individuals with selenised yeast for 6 months and 5 years, respectively, at 100, 200, and 300 μg Se/day or placebo. Speciation data was obtained for male plasma using HPLC-ICP-MS and HPLC-ESI-MS/MS. With the proposed strategy, approximately 1.5 mL of plasma was needed to determine total Se concentration and the fractionation of Se in high molecular weight (HMW) and low molecular weight (LMW) pools, and for quantification and identification of small Se species. For the first time, Se-methyl-selenocysteine (MSC) and methyl-2-acetamido-2deoxy1-seleno-β-D-galactopyranoside (Selenosugar-1) were structurally confirmed in plasma after supplementation with selenised yeast within the studied range. Determination of selenomethionine (SeMet) incorporated nonspecifically into albumin (SeALB) was achieved by HPLC-ICP-MS after hydrolysis. By subtracting this SeMet concentration from the total Se in the HMW pool, the concentration of Se incorporated into selenoproteins was calculated. Results from the speciation analysis of the free Se metabolite fraction (5% of total plasma Se) suggest a significant increase in the percentage of Se (as SeMet plus Selenosugar-1) of up to 80% of the total Se in the LMW fraction after 6 months of supplementation. The Se distribution in the HMW fraction reflects a significant increase in SeALB with Se depletion from selenoproteins, which occurs most significantly at doses of over 100 μg Se/day after 5 years. The results of this work will inform future trial design.
Keywords Selenium . Speciation . PRECISE trial . HPLC/ICP-MS . Human plasma
Introduction Published in the topical collection featuring Female Role Models in Analytical Chemistry. Supplementary Information The online version of this article (https:// doi.org/10.1007/s00216-020-02988-9) contains supplementary material, which is available to authorized users. * Heidi Goenaga-Infante [email protected] 1
LGC Limited, Queens Road, Teddington, Middlesex TW11 0LY, UK
2
Department of Nutritional Sciences, University of Surrey, Guildford GU2 7XH, UK
3
Laboratory of Toxicology and Environmental Health, Graduate School of Pharmaceutical Sciences, Chiba University, 1-8-1 Inohana, Chuo, Chiba 260-8675, Japan
Selenium (Se) is a nutritional trace element essential to human health [1]. Increasing evidence suggests that Se is a natural anti-carcinogenic agent, playing an
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