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Mercury Reduction by Nanoparticulate Vivianite.

ABSTRACT: Mercury (Hg) is a toxic trace element of global environmental concern which has been increasingly dispersed into the environment since the industrial revolution. In aquatic and terrestrial systems, Hg can be reduced to elemental Hg (Hg⁰) and escape to the atmosphere or converted to methylmercury (MeHg), a potent neurotoxin that accumulates in food webs. Fe^II-bearing minerals such as magnetite, green rusts, siderite, and mackinawite are recognized Hg^II reducers. Another potentially Hg-reducing mineral, which commonly occurs in Fe- and organic/P-rich sediments and soils, is the ferrous iron phosphate mineral vivianite (Fe^II₃(PO₄)₂·8H₂O), but its reaction with Hg^II has not been studied to date. Here, nanoparticulate vivianite (particle size ∼ 50 nm; Fe^II content > 98%) was chemically synthesized and characterized by a combination of chemical, spectroscopic, and microscopic analyses. Its ability to reduce Hg^II was investigated at circumneutral pH under anoxic conditions over a range of Fe^II/Hg^II ratios (0.1-1000). For Fe^II/Hg^II ratios ≥1, which are representative of natural environments, Hg^II was very quickly and efficiently reduced to Hg⁰. The ability of vivianite to reduce Hg^II was found to be similar to those of carbonate green rust and siderite, two of the most effective Hg-reducing minerals. Our results suggest that vivianite may be involved in abiotic Hg^II reduction in Fe and organic/P-rich soils and sediments, potentially contributing to Hg evasion while also limiting MeHg formation in these ecosystems.

SUBMITTER: Etique M

PROVIDER: S-EPMC7931808 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:BackgroundThe reduction-sensitive cationic polymer is a promising nonviral carrier for gene delivery. Until now, disulfide bonds have been the only golden standard for its design. The aim of this research was to develop a novel reduction-responsive cationic polymer as a gene carrier.MethodsPolycationic carriers were synthesized by addition of branched oligoethylenimine 800 Da (OEI(800)) via an active ester containing diselenide bonds. Disulfide bonds cross-linked with OEI(800)-SS(x) and monoselenide bonds linked with OEI(800)-Se(x) were synthesized and compared. Their molecular weights and degradation properties were determined using gel permeation chromatography. Changes in particle size, morphology, and DNA binding were investigated by dynamic light scattering, transmission electron microscopy, and electrophoresis assay in a reduction environment. Cytotoxicity and transfection in vitro were evaluated in a murine melanoma cell line (B16F10) and a human cervical epithelial carcinoma cell line (HeLa), while intracellular degradation and dissociation with DNA were studied by confocal laser scanning microscopy with FITC-labeled OEI(800) derivatives and Cy5-labeled DNA.ResultsDiselenide-conjugated OEI(800) (OEI(800)-SeSe(x)) polymer carriers of high molecular weight were successfully synthesized. After compacting with DNA, the OEI(800)-SeSe(x) polymers formed nanoparticles with an average size of 140 nm at an adequate C/P ratio. OEI(800)-SeSe(x) showed reduction-responsive degradation properties similar to those of the OEI(800)-SS(x) via gel permeation chromatography, dynamic light scattering, and transmission electron microscopy. OEI(800)-SeSe(x) showed much lower cytotoxicity than PEI(25k), and significantly higher transfection efficiency than OEI(800) in both B16F10 and HeLa cells. Transfection of luciferase in the OEI(800)-SeSe(x) group was comparable with that of standard PEI(25k) and traditional reduction-sensitive polymer OEI(800)-SS(x) groups. Furthermore, intracellular degradation of OEI(800)-SeSe(x) and dissociation with DNA were also confirmed by confocal laser scanning microscopy.ConclusionThe OEI(800)-SeSe(x) obtained was able to bind plasmid DNA efficiently to yield nanosized particles and had reduction sensitivity which is as efficient as that for OEI(800)-SS(x). In vitro experiments confirmed its low cytotoxicity and high transfection ability. Diselenide bonds can be used as effective and novel reduction-sensitive linkages for gene delivery.

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Mercury Reduction by Nanoparticulate Vivianite.

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