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Lu, Xia

Publications and source records attributed to Lu, Xia.

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Adsorption and intracellular uptake of mercuric mercury and methylmercury by methanotrophs and methylating bacteria

The cell surface adsorption and intracellular uptake of mercuric mercury Hg(II) and methylmercury (MeHg) are important in determining the fate and transformation of Hg in the environment. However, current information is limited about their interactions with two important groups of microorganisms, i.e., methanotrophs and Hg(II)-methylating bacteria, in aquatic systems. This study investigated the adsorption and uptake dynamics of Hg(II) and MeHg by three strains of methanotrophs, Methylomonas sp. strain EFPC3, Methylosinus trichosporium OB3b, and Methylococcus capsulatus Bath, and two Hg(II)-methylating bacteria, Pseudodesulfovibrio mercurii ND132 and Geobacter sulfurreducens PCA. Distinctive behaviors of these microorganisms towards Hg(II) and MeHg adsorption and intracellular uptake were observed. The methanotrophs took up 55–80% of inorganic Hg(II) inside cells after 24 h incubation, lower than methylating bacteria (>90%). Approximately 80–95% of MeHg was rapidly taken up by all the tested methanotrophs within 24 h. In contrast, after the same time, G. sulfurreducens PCA adsorbed 70% but took up <20% of MeHg, while P. mercurii ND132 adsorbed <20% but took up negligible amounts of MeHg. These results suggest that microbial surface adsorption and intracellular uptake of Hg(II) and MeHg depend on the specific types of microbes and appear to be related to microbial physiology that requires further detailed investigation. Despite being incapable of methylating Hg(II), methanotrophs play important roles in immobilizing both Hg(II) and MeHg, potentially influencing their bioavailability and trophic transfer. Furthermore, methanotrophs are not only important sinks for methane but also for Hg(II) and MeHg and can influence the global cycling of C and Hg.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Isotope Exchange between Mercuric [Hg(II)] Chloride and Hg(II) Bound to Minerals and Thiolate Ligands: Implications for Enriched Isotope Tracer Studies

Enriched mercury (Hg) stable isotopes have been widely used as tracers in field and laboratory investigations of Hg(II) biogeochemical transformations such as methylation and demethylation. Few studies, however, have considered concurrent isotope exchange reactions between newly spiked and pre-existing Hg(II) in environmental matrices, which may alter redistribution and thus transformation of the spiked and pre-existing Hg(II). Using enriched 198 Hg [as mercuric Hg(II) or HgCl n species], this study investigated isotope exchange between 198 Hg and pre-existing Hg(II) bound to metacinnabar (β-HgS), sediments, low-molecular-weight (LMW) thiols, and dissolved organic matter (DOM). The impact of isotope exchange on methylmercury production in the presence of organic ligands was also evaluated with an iron-reducing bacterium Geobacter sulfurreducens PCA in a phosphate buffered solution (pH 7.4). Here, we found that spiked 198 Hg readily exchanged with mineral-bound ambient Hg(II) despite concurrent Hg(II) adsorption and immobilization on the solids. Rapid exchange (<3 min) was also observed between spiked 198 Hg and 200 Hg pre-equilibrated with LMW thiols and DOM in solution. While the exchange did not cause net changes in Hg(II) chemical speciation, it resulted in redistribution of Hg(II) isotopes bound to the ligands and thus an apparently similar methylation rate and magnitude of the spiked 198 Hg and pre-existing 200 Hg by PCA cells when 198 Hg and 200 Hg were added at 1:1 ratio. These observations underscore the importance of isotope exchange when an enriched Hg isotope is applied in environmental matrices, as the exchange could potentially lead to biased rate calculations of Hg(II) transformation and bioaccumulation and thus risk assessments of new Hg(II) input to the natural ecosystems.

58 GEOSCIENCES↗
DOE OSTI2020

Synergistic Effects of a Chalkophore, Methanobactin, on Microbial Methylation of Mercury

Microbial production of the neurotoxin methylmercury (MeHg) is a significant health and environmental concern, as it can bioaccumulate and biomagnify in the food web. A chalkophore or a copper-binding compound, termed methanobactin (MB), has been shown to form strong complexes with mercury [as Hg(II)] and also enables some methanotrophs to degrade MeHg. It is unknown, however, if Hg(II) binding with MB can also impede Hg(II) methylation by other microbes. Contrary to expectations, MB produced by the methanotroph Methylosinus trichosporium OB3b (OB3b-MB) enhanced the rate and efficiency of Hg(II) methylation more than that observed with thiol compounds (such as cysteine) by the mercury-methylating bacteria Desulfovibrio desulfuricans ND132 and Geobacter sulfurreducens PCA. Compared to no-MB controls, OB3b-MB decreased the rates of Hg(II) sorption and internalization, but increased methylation by 5- to 7-fold, suggesting that Hg(II) complexation with OB3b-MB facilitated exchange and internal transfer of Hg(II) to the HgcAB proteins required for methylation. Conversely, addition of excess amounts of OB3b-MB or a different form of MB from Methylocystis strain SB2 (SB2-MB) inhibited Hg(II) methylation, likely due to greater binding of Hg(II). Collectively, our results underscore the complex roles of microbial exogenous metal-scavenging compounds in controlling net production and bioaccumulation of MeHg in the environment. Some anaerobic microorganisms convert inorganic mercury (Hg) into the neurotoxin methylmercury, which can bioaccumulate and biomagnify in the food web. While the genetic basis of microbial mercury methylation is known, factors that control net methylmercury production in the environment are still poorly understood. Here, it is shown that mercury methylation can be substantially enhanced by one form of an exogenous copper-binding compound (methanobactin) produced by some methanotrophs, but not by another. This novel finding illustrates that complex interactions exist between microbes and that these interactions can potentially affect the net production of methylmercury in situ .

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Mercury Uptake by Desulfovibrio desulfuricans ND132: Passive or Active?

Recent studies have identified HgcAB proteins as being responsible for mercury [Hg(II)] methylation by certain anaerobic microorganisms. However, it remains controversial whether microbes take up Hg(II) passively or actively. Here, we examine the dynamics of concurrent Hg(II) adsorption, uptake, and methylation by both viable and inactivated cells (heat-killed or starved) or spheroplasts of the sulfate-reducing bacterium Desulfovibrio desulfuricans ND132 in laboratory incubations. We show that, without addition of thiols, >60% of the added Hg(II) (25 nM) was taken up passively in 48 h by live and inactivated cells and also by cells treated with the proton gradient uncoupler, carbonylcyanide-3-chlorophenylhydrazone (CCCP). Inactivation abolished Hg(II) methylation, but the cells continued taking up Hg(II), likely through competitive binding or ligand exchange of Hg(II) by intracellular proteins or thiol-containing cellular components. Similarly, treatment with CCCP impaired the ability of spheroplasts to methylate Hg(II) but did not stop Hg(II) uptake. Spheroplasts showed a greater capacity to adsorb Hg(II) than whole cells, and the level of cytoplasmic membrane-bound Hg(II) correlated well with MeHg production, as Hg(II) methylation is associated with cytoplasmic HgcAB. Our results indicate that active metabolism is not required for cellular Hg(II) uptake, thereby providing an improved understanding of Hg(II) bioavailability for methylation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

The Application and Potential Artifacts of Zeeman Cold Vapor Atomic Absorption Spectrometry in Mercury Stable Isotope Analysis

Zeeman cold vapor atomic absorption spectrometry (CVAAS) has been widely used for environmental mercury (Hg) detection and quantification for decades, but little is known about its utility and potential artifacts in analyzing Hg with varying isotope compositions. We show that each Hg isotope responds differently by CVAAS analysis, with 200 Hg and 202 Hg isotopes exhibiting signal intensities ~10 times greater than those of 198 Hg and 201 Hg isotopes. However, all Hg isotopes show a linear correlation between Hg concentration and signal intensity, validated by both measurements and theoretical simulations. Zeeman CVAAS could thus offer a convenient, inexpensive tool for determining Hg isotopes, particularly in using one or two enriched Hg isotopes for tracing Hg biogeochemical transformations, such as partitioning, ion exchange, sorption–desorption, and methylation–demethylation in environmental matrices. Additionally, we caution that care must be taken when CVAAS is used for quantifying Hg in samples with changing isotope compositions to avoid measurement errors.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Mercury Sorption and Desorption on Organo-Mineral Particulates as a Source for Microbial Methylation

In natural freshwater and sediments, mercuric mercury (Hg(II)) is largely associated with particulate minerals and organics, but it remains unclear under what conditions particulates may become a sink or a source for Hg(II) and whether the particulate-bound Hg(II) is bioavailable for microbial uptake and methylation. In this study, we investigated Hg(II) sorption–desorption characteristics on three organo-coated hematite particulates and a Hg-contaminated natural sediment and evaluated the potential of particulate-bound Hg(II) for microbial methylation. Mercury rapidly sorbed onto particulates, especially the cysteine-coated hematite and sediment, with little desorption observed (0.1–4%). However, the presence of Hg-binding ligands, such as low-molecular-weight thiols and humic acids, resulted in up to 60% of Hg(II) desorption from the Hg-laden hematite particulates but <6% from the sediment. Importantly, the particulate-bound Hg(II) was bioavailable for uptake and methylation by a sulfate-reducing bacterium Desulfovibrio desulfuricans ND132 under anaerobic incubations, and the methylation rate was 4–10 times higher than the desorption rate of Hg(II). These observations suggest direct contacts and interactions between bacterial cells and the particulate-bound Hg(II), resulting in rapid exchange or uptake of Hg(II) by the bacteria. The results highlight the importance of Hg(II) partitioning at particulate–water interfaces and the role of particulates as a significant source of Hg(II) for methylation in the environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Li-ion battery material under high pressure: amorphization and enhanced conductivity of Li 4 Ti 5 O 12

Lithium titanium oxide (Li 4 Ti 5 O 12 , LTO), a 'zero-strain' anode material for lithium-ion batteries, exhibits excellent cycling performance. However, its poor conductivity highly limits its applications. Here, the structural stability and conductivity of LTO were studied using in situ high-pressure measurements and first-principles calculations. LTO underwent a pressure-induced amorphization (PIA) at 26.9 GPa. The impedance spectroscopy revealed that the conductivity of LTO improved significantly after amorphization and that the conductivity of decompressed amorphous LTO increased by an order of magnitude compared with its starting phase. Furthermore, our calculations demonstrated that the different compressibility of the LiO 6 and TiO 6 octahedra in the structure was crucial for the PIA. The amorphous phase promotes Li + diffusion and enhances its ionic conductivity by providing defects for ion migration. Our results not only provide an insight into the pressure depended structural properties of a spinel-like material, but also facilitate exploration of the interplay between PIA and conductivity.

25 ENERGY STORAGE↗
DOE OSTI2018

Unraveling Microbial Communities Associated with Methylmercury Production in Paddy Soils

Here, we report rice consumption is now recognized as an important pathway of human exposure to the neurotoxin methylmercury (MeHg), particularly in countries where rice is a staple food. Although the discovery of a two-gene cluster hgcAB has linked Hg methylation to several phylogenetically diverse groups of anaerobic microorganisms converting inorganic mercury (Hg) to MeHg, the prevalence and diversity of Hg methylators in microbial communities of rice paddy soils remain unclear. We characterized the abundance and distribution of hgcAB genes using third-generation PacBio long-read sequencing and Illumina short-read metagenomic sequencing, in combination with quantitative PCR analyses in several mine-impacted paddy soils from southwest China. Both Illumina and PacBio sequencing analyses revealed that Hg methylating communities were dominated by iron-reducing bacteria (i.e., Geobacter ) and methanogens, with a relatively low abundance of hgcA + sulfate-reducing bacteria in the soil. A positive correlation was observed between the MeHg content in soil and the relative abundance of Geobacter carrying the hgcA gene. Phylogenetic analysis also uncovered some hgcAB sequences closely related to three novel Hg methylators, Geobacter anodireducens , Desulfuromonas sp. DDH964, and Desulfovibrio sp. J2, among which G. anodireducens was validated for its ability to methylate Hg. Lastly, these findings shed new light on microbial community composition and major clades likely driving Hg methylation in rice paddy soils.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Quantitative Proteomic Analysis of Biological Processes and Responses of the Bacterium Desulfovibrio desulfuricans ND132 upon Deletion of Its Mercury Methylation Genes

Recent studies of microbial mercury (Hg) methylation revealed a key gene pair, hgcAB , which is essential for methylmercury (MeHg) production in the environment. However, many aspects of the mechanism and biological processes underlying Hg methylation, as well as any additional physiological functions of the hgcAB genes, remain unknown. Here, quantitative proteomics are used to identify changes in potential functional processes related to hgcAB gene deletion in the Hg-methylating bacterium Desulfovibrio desulfuricans ND132. Global proteomics analyses indicate that the wild type and Δ hgcAB strains are similar with respect to the whole proteome and the identified number of proteins, but differ significantly in the abundance of specific proteins. The authors observe changes in the abundance of proteins related to the glycolysis pathway and one-carbon metabolism, suggesting that the hgcAB gene pair is linked to carbon metabolism. Unexpectedly, the authors find that the deletion of hgcAB significantly impacts a range of metal transport proteins, specifically membrane efflux pumps such as those associated with heavy metal copper (Cu) export, leading to decreased Cu uptake in the Δ hgcAB mutant. This observation indicates possible linkages between this set of proteins and metal homeostasis in the cell. However, hgcAB gene expression is not induced by Hg, as evidenced by similarly low abundance of HgcA and HgcB proteins in the absence or presence of Hg (500 nm). Altogether, these results suggest an apparent link between HgcAB, one-carbon metabolism, and metal homeostasis, thereby providing insights for further exploration of biochemical mechanisms and biological functions of microbial Hg methylation.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2018

Mercury in Water

Mercury (Hg) is a global pollutant threatening our water resources and human health. Every one of us contains some levels of Hg or methylmercury (MeHg) in our body due to consumption of contaminated food such as fish and rice. Our understanding of the behavior of Hg in natural aquatic environments is limited as the major factors controlling microbial uptake and conversion of inorganic Hg to neurotoxic MeHg remain obscure. MeHg concentrations in water can bioaccumulate up to eight orders of magnitude in the food chain. Metallic or elemental Hg can evaporate and transport around the globe, and also readily undergoes chemical, photochemical and biological transformations (i.e., oxidation, reduction, methylation and demethylation) in water and sediments. Natural dissolved organic matter (DOM) plays a critical role in mediating these transformations because of its exceptionally strong binding affinity for Hg and its dual functional roles in reducing and oxidizing Hg. While the discovery of Hg-methylation genes significantly advanced our understanding of MeHg biosynthesis, the simultaneous degradation of MeHg at low concentrations (i.e., picomolar to nanomolar) by a range of methanotrophic and anaerobic bacteria has recently been recognized possibly as an important process for controlling net MeHg production, a key factor that determines Hg concentrations and bioaccumulation in biota. Although treatment technologies for Hg removal from water are available, they are mostly applicable to industrial waste streams and at localized contamination sites with high Hg concentrations (i.e., micromolar to millimolar). Reductions in Hg human exposure may be achievable by decreasing anthropogenic releases, such as coal combustion, over the long-term since Hg methylation responds to Hg inputs, particularly freshly deposited Hg in natural aquatic systems.

Gu, Baohua↗
DOE OSTI2018

Nanomolar Copper Enhances Mercury Methylation by Desulfovibrio desulfuricans ND132

Methylmercury (MeHg) is produced by certain anaerobic microorganisms, such as the sulfate-reducing bacterium Desulfovibrio desulfuricans ND132, but environmental factors affecting inorganic mercury [Hg(II)] uptake and methylation remain unclear. We report that the presence of a small amount of copper ions [Cu(II), <100 nM] enhances Hg(II) uptake and methylation by washed cells of ND132, while Hg(II) methylation is inhibited at higher Cu(II) concentrations because of the toxicity of copper to the microorganism. The enhancement or inhibitory effect of Cu(II) is dependent on both time and concentration. The presence of nanomolar concentrations of Cu(II) facilitates rapid uptake of Hg(II) (within minutes) and doubles MeHg production within a 24 h period, but micromolar concentrations of Cu(II) completely inhibit Hg(II) methylation. Metal ions such as zinc [Zn(II)] and nickel [Ni(II)] also inhibit but do not enhance Hg(II) methylation under the same experimental conditions. Furthermore, these observations suggest a synergistic effect of Cu(II) on Hg(II) uptake and methylation, possibly facilitated by copper transporters or metallochaperones in this organism, and highlight the fact that complex environmental factors affect MeHg production in the environment.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Methylmercury Uptake and Degradation by Methanotrophs

Methylmercury (CH 3 Hg + ) is a potent neurotoxin produced by certain anaerobic microorganisms in natural environments. While numerous studies have characterized the basis of mercury methylation, no studies have examined CH 3 Hg + degradation by methanotrophs, despite their ubiquitous presence in the environment. We report that some methanotrophs (e.g., Methylosinus trichosporium OB3b) can take up and degrade CH 3 Hg + rapidly, whereas others (e.g., Methylococcus capsulatus Bath) can take up but not degrade CH 3 Hg + . Demethylation by M. trichosporium OB3b increases with increasing CH 3 Hg + concentrations but is abolished in mutants deficient in methanobactin biosynthesis. Further, addition of methanol as a competing C1 substrate inhibits demethylation, suggesting that CH3Hg+ degradation by methanotrophs may involve an initial bonding of CH 3 Hg + by methanobactin followed by cleavage of the C-Hg bond in CH 3 Hg + by the methanol dehydrogenase. This new demethylation pathway by methanotrophs indicates possible broader involvement of C1-metabolizing aerobes in the environmental degradation of toxic CH3Hg+.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗