Isotope Fractionation from <i>In Vivo</i> Methylmercury Detoxification in Waterbirds

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Author(s): Poulin, BA; Janssen, SE; Rosera, TJ; Krabbenhoft, DP; Eagles-Smith, CA; Ackerman, JT; Stewart, AR; Kim, E; Baumann, Z; JH; Manceau, A | Abstract: The robust application of stable mercury (Hg) isotopes for source apportionment and risk assessment necessitates the understanding mass-dependent fractionation (MDF) as a result internal transformations within organisms. Here, we used high energy-resolution X-ray absorption near edge structure spectroscopy isotope ratios total (?202THg) methylmercury (?202MeHg) to elucidate chemical speciation Hg resultant MDF MeHg demethylation in waterbirds. In three waterbirds (Clark's grebe, Forster's tern, south polar skua), between 17 86% was demethylated inorganic (iHg) species primarily liver kidneys Hg-tetraselenolate [Hg(Sec)4] minor Hg-dithiolate [Hg(SR)2] complexes. Tissular differences ?202THg ?202MeHg correlated linearly with %iHg [Hg(Sec)4 + Hg(SR)2] were interpreted reflect kinetic effect during vivo demethylation. product-reactant isotopic enrichment factor (?p/r) ? Hg(Sec)4 -2.2 ± 0.1‰. values unvarying each bird, regardless abundance, indicating fast cycling or replenishment relative Our findings document universal selenium-dependent reaction birds, provide new insights on Hg(Sec)4, allow mathematical correction reaction.

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ژورنال

عنوان ژورنال: ACS earth and space chemistry

سال: 2021

ISSN: ['2472-3452']

DOI: https://doi.org/10.1021/acsearthspacechem.1c00051