| 1. |
- Capo, Eric, et al.
(författare)
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A consensus protocol for the recovery of mercury methylation genes from metagenomes
- 2023
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Ingår i: Molecular Ecology Resources. - : John Wiley & Sons. - 1755-098X .- 1755-0998. ; 23:1, s. 190-204
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Tidskriftsartikel (refereegranskat)abstract
- Mercury (Hg) methylation genes (hgcAB) mediate the formation of the toxic methylmercury and have been identified from diverse environments, including freshwater and marine ecosystems, Arctic permafrost, forest and paddy soils, coal-ash amended sediments, chlor-alkali plants discharges and geothermal springs. Here we present the first attempt at a standardized protocol for the detection, identification and quantification of hgc genes from metagenomes. Our Hg-cycling microorganisms in aquatic and terrestrial ecosystems (Hg-MATE) database, a catalogue of hgc genes, provides the most accurate information to date on the taxonomic identity and functional/metabolic attributes of microorganisms responsible for Hg methylation in the environment. Furthermore, we introduce "marky-coco", a ready-to-use bioinformatic pipeline based on de novo single-metagenome assembly, for easy and accurate characterization of hgc genes from environmental samples. We compared the recovery of hgc genes from environmental metagenomes using the marky-coco pipeline with an approach based on coassembly of multiple metagenomes. Our data show similar efficiency in both approaches for most environments except those with high diversity (i.e., paddy soils) for which a coassembly approach was preferred. Finally, we discuss the definition of true hgc genes and methods to normalize hgc gene counts from metagenomes.
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| 2. |
- Lian, Peng, et al.
(författare)
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Mechanistic Investigation of Dimethylmercury Formation Mediated by a Sulfide Mineral Surface
- 2021
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 125:24, s. 5397-5405
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Tidskriftsartikel (refereegranskat)abstract
- Mercury (Hg) pollution is a global environmental problem. The abiotic formation of dimethylmercury (DMeHg) from monomethylmercury (MMeHg) may account for a large portion of DMeHg in oceans. Previous experimental work has shown that abiotic formation of DMeHg from MMeHg can be facilitated by reduced sulfur groups on sulfide mineral surfaces. In that work, a mechanism was proposed in which neighboring MMeHg moieties bound to sulfide sites on a mineral surface react through an SN2-type mechanism to form DMeHg and incorporate the remaining Hg atoms into the mineral surface. Here, we perform density functional theory calculations to explore the mechanisms of DMeHg formation on the 110 surface of a CdS(s) (hawleyite) nanoparticle. We show that coordination of MMeHg substituents to adjacent reduced sulfur groups protruding from the surface indeed facilitates DMeHg formation and that the reaction proceeds through direct transmethylation from one MMeHg substituent to another. Coordination of Hg by multiple S atoms provides a transition-state stabilization and activates a C–Hg bond for methyl transfer. In addition, solvation effects play an important role in the surface reconstruction of the nanoparticle and in decreasing the energetic barrier for DMeHg formation relative to the corresponding reaction in vacuo.
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| 3. |
- Wang, Wei, et al.
(författare)
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Ag@SiO2 Core-Shell Nanoparticles for Probing Spatial Distribution of Electromagnetic Field Enhancement via Surface-Enhanced Raman Scattering
- 2009
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 3:11, s. 3493-3496
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Tidskriftsartikel (refereegranskat)abstract
- We show that the spatial distribution of the electromagnetic (EM) field enhancement can be probed directly via dynamic evolution of surface-enhanced Raman scattering (SERS) of rhodamine 6G (R6G) molecules as they diffuse into Ag@SiO2 core-shell nanoparticles. The porous silica shell limits the diffusion of R6G molecules toward Inner Ag cores, thereby allowing direct observation and quantification of the spatial distribution of SERS enhancement as molecules migrate from the low to high EM fields inside the dielectric silica shell. Our experimental evidence is validated by the generalized Mie theory, and the approach can potentially offer a novel platform for further investigating the site and spatial distribution of the EM fields and the EM versus chemical enhancement of SERS due to molecular confinement within the Ag@SiO2 nanoshell.
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| 4. |
- Zhao, Ke, et al.
(författare)
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One-dimensional arrays of nanoshell dimers for single molecule spectroscopy via surface-enhanced raman scattering
- 2006
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 125:8
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Tidskriftsartikel (refereegranskat)abstract
- The optical properties of one-dimensional arrays of metal nanoshell dimers are studied systematically using the T-matrix method based on Mie theory, within the context of surface enhanced Raman scattering (SERS). It is shown that the local electromagnetic enhancement can be as high as similar to 4.5x10(13) for nanoshell dimer arrays with optimal geometry, and sensitive tunability in the resonant frequency can be gained by varying the geometrical parameters, making such structures appealing templates for SERS measurements with single molecule sensitivity. The extraordinarily high enhancement is attributed to a collective photonic effect constructively superposed onto the intrinsic enhancement associated with an isolated nanoshell dimer. (c) 2006 American Institute of Physics.
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