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ß-1,3-glucanases can degrade ß-1,3-glucoside bonds in ß-glucan which is the main cell-wall component of most of fungi, and have the crucial application potential in plant protection and food processing. Herein, a ß-1,3-glucanase FlGluA from Flavobacterium sp. NAU1659 composed of 333 amino acids with a predicted molecular mass of 36.6 kDa was expressed in Escherichia coli BL21, purified and characterized. The deduced amino acid sequence of FlGluA showed the high identity with the ß-1,3-glucanase belonging to glycoside hydrolase (GH) family 16. Enzymological characterization indicated FlGluA had the highest activity on zymosan A, with a specific activity of 3.87 U/mg, followed by curdlan (1.16 U/mg) and pachymaran (0.88 U/mg). It exhibited optimal catalytic activity at the pH 5.0 and 40 °C, and was stable when placed at 4 °C for 12 h in the range of pH 3.0-8.0 or at a temperature below 50 °C for 3 h. Its catalytic activity was enhanced by approximately 36 % in the presence of 1 mM Cr3+. The detection of thin-layer chromatography and mass spectrometry showed FlGluA hydrolyzed zymosan A mainly to glucose and disaccharide, and trace amounts of tetrasaccharide and pentasaccharide, however, it had no action on laminaribiose, indicating its endo-ß-1,3-glucanase activity. The mycelium growth of F. oxysporum treated by FlGluA was inhibited, with approximately 37 % of inhibition rate, revealing the potential antifungal activity of the enzyme. These results revealed the hydrolytic properties and biocontrol activity of FlGluA, laying a crucial foundation for its potential application in agriculture and industry.
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We analyzed the clinical characteristics of outpatients with influenza-B-associated pneumonia during the 2021-2022 influenza season and analyzed the molecular epidemiology and evolution of influenza B virus. The presence of influenza B virus was confirmed by reverse transcription polymerase chain reaction (RT-PCR). Electronic medical records were used to collect and analyze data of outpatients. The HA and NA genes were phylogenetically analyzed using ClustalW 2.10 and MEGA 11.0. Out of 1569 outpatients who tested positive for influenza B virus, 11.7% (184/1569) developed pneumonia, and of these, 19.0% (35/184) had underlying diseases. Fever, cough, and sore throat were the most common symptoms. Among the complications, acute respiratory distress syndrome (ARDS), acute kidney injury (AKI), and shock accounted for 2.7% (5/184), 4.9% (9/184), and 1.6% (3/184), respectively. Of the outpatients, 2.7% (5/184) were admitted to the hospital, and 0.5% (1/184) of them died. All of the strains from Beijing were identified as belonging to the B/Victoria lineage. The HA and NA gene sequences of 41 influenza B viruses showed high similarity to each other, and all of them belonged to clade 1A.3. Compared with the vaccine strain B/Washington/02/2019, all of the isolates contained N150K, G181E, and S194D mutations. S194D, E195K, and K200R mutations were detected in the 190 helix of the receptor binding region of HA. Co-mutations of H122Q, A127T, P144L, N150K, G181E, S194D, and K200R in HA and D53N, N59S, and G233E in NA were detected in 78.0% (32/41) of the isolates, and 56.3% (18/32) of these were from outpatients with influenza-B-associated pneumonia. Influenza outpatients with underlying diseases were more likely to develop pneumonia. No significant differences were observed in clinical symptoms or laboratory results between outpatients with and without pneumonia, so testing for influenza virus seems to be a good choice. The observed amino acid variations suggest that current vaccines might not provide effective protection.
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Influenza Humana , Humanos , Influenza Humana/epidemiologia , Vírus da Influenza B , Pequim , Estações do Ano , Pacientes Ambulatoriais , Evolução Molecular , Filogenia , Glicoproteínas de Hemaglutininação de Vírus da Influenza/genéticaRESUMO
The fate of antimony (Sb) is strongly affected by adsorption, yet Sb isotope fractionation and the associated mechanism have not been widely reported. Here we experimentally investigated the process of Sb(V) adsorption on iron (oxyhydr)oxides and the associated isotope effects. Sb isotope fractionation occurs during adsorption (Δ123Sbsolution-mineral = 1.20 ± 0.02 for ferrihydrite and 2.35 ± 0.04 for goethite). Extended X-ray absorption fine structure (EXAFS) analysis shows that Sb(V) adsorption on iron (oxyhydr)oxides occurs via inner-sphere surface complexation, including mononuclear bidentate edge-sharing (2E) and binuclear bidentate corner-sharing (2C) complexes. A longer atom distance of Sb-Fe in ferrihydrite leads to less Sb isotope fractionation during Sb adsorption than in goethite. The Gibbs free energy and Mayer bond order were calculated based on density functional theory (DFT) and suggested that the strength of the bonding environment can be summarized as Sb(OH)6- > 2E > 2C. In turn, the bonding environment indicates the mechanism of Sb isotope fractionation during the process. This study reveals that Sb isotope fractionation occurs during Sb(V) adsorption onto iron (oxyhydr)oxides, providing a basis for the future study of Sb isotopes and further understanding of the fractionation mechanism.
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Ferro , Óxidos , Ferro/química , Antimônio/química , Adsorção , Compostos Férricos/química , IsótoposRESUMO
Accumulation of geogenic phosphorus (P) in groundwater is an emerging environmental concern, which is closely linked to coupled processes involving FeOOH and organic matter under methanogenic conditions. However, it remains unclear how P enrichment is associated with methane cycling, particularly the anaerobic methane oxidation (AMO). This study conducted a comprehensive investigation of carbon isotopes in dissolved inorganic carbon (DIC), CO2, and CH4, alongside Fe isotopes, microbial communities, and functions in quaternary aquifers of the central Yangtze River plain. The study found that P concentrations tended to increase with Fe(II) concentrations, δ56Fe, and δ13C-DIC, suggesting P accumulation due to the reductive dissolution of FeOOH under methanogenic conditions. The positive correlations of pmoA gene abundance versus δ13C-CH4 and Fe concentrations versus δ13C-CH4, and the prevalent presence of Candidatus_Methanoperedens, jointly demonstrated the potential significance of Fe(III)-mediated AMO process (Fe-AMO) alongside traditional methanogenesis. The increase of P concentration with δ13C-CH4 value, pmoA gene abundance, and Fe concentration suggested that the Fe-AMO process facilitated P enrichment in groundwater. Redundancy analysis confirmed this assertion, identifying P concentration as the primary determinant and the cooperative influence of Fe-AMO microorganisms such as Candidatus_Methanoperedens and Geobacter on P enrichment. Our work provided new insights into P dynamics in subsurface environments.
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Água Subterrânea , Metano , Oxirredução , Fósforo , Água Subterrânea/química , Metano/metabolismo , Fósforo/metabolismo , Anaerobiose , Compostos Férricos/metabolismoRESUMO
Massive soil erosion occurs in the world's Mollisol regions due to land use change and climate warming. The migration of Mollisol organic matter to river systems and subsequent changes in carbon biogeochemical flow and greenhouse gas fluxes are of global importance but little understood. By employing comparative mesocosm experiments simulating varying erosion intensity in Mollisol regions of northeastern China, this research highlights that erosion-driven export and biomineralization of terrestrial organic matter facilitates CO2 and CH4 emission from receiving rivers. Stronger Mollisol erosion, as represented by a higher soil-to-water ratio in suspensions, increased CO2 efflux, particularly for the paddy Mollisols. This is mechanistically attributable to increased bioavailability of soluble organic carbon in river water that is sourced back to destabilized organic matter, especially from the cultivated Mollisols. Concurrent changes in microbial community structure have enhanced both aerobic and anaerobic processes as reflected by the coemission of CO2 and CH4. Higher greenhouse gas effluxes from paddy Mollisol suspensions suggest that agricultural land use by supplying more nitrogen-containing, higher-free-energy organic components may have enhanced microbial respiration. These new findings highlight that Mollisol erosion is a hidden significant contributor to greenhouse gas emissions from river water, given that the world's four major Mollisol belts are all experiencing intensive cultivation.
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Carbono , Gases de Efeito Estufa , Rios , Rios/química , Solo/química , China , Dióxido de Carbono , Metano/metabolismoRESUMO
The biogeochemical processes of iodine are typically coupled with organic matter (OM) and the dynamic transformation of iron (Fe) minerals in aquifer systems, which are further regulated by the association of OM with Fe minerals. However, the roles of OM in the mobility of iodine on Fe-OM associations remain poorly understood. Based on batch adsorption experiments and subsequent solid-phase characterization, we delved into the immobilization and transformation of iodate and iodide on Fe-OM associations with different C/Fe ratios under anaerobic conditions. The results indicated that the Fe-OM associations with a higher C/Fe ratio (=1) exhibited greater capacity for immobilizing iodine (â¼60-80% for iodate), which was attributed to the higher affinity of iodine to OM and the significantly decreased extent of Fe(II)-catalyzed transformation caused by associated OM. The organic compounds abundant in oxygen with high unsaturation were more preferentially associated with ferrihydrite than those with poor oxygen and low unsaturation; thus, the associated OM was capable of binding with 28.1-45.4% of reactive iodine. At comparable C/Fe ratios, the mobilization of iodine and aromatic organic compounds was more susceptible in the adsorption complexes compared to the coprecipitates. These new findings contribute to a deeper understanding of iodine cycling that is controlled by Fe-OM associations in anaerobic environments.
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Iodo , Ferro , Iodo/química , Ferro/química , Adsorção , Água Subterrânea/química , Minerais/químicaRESUMO
Organoiodine compounds (OICs) are the dominant iodine species in groundwater systems. However, molecular mechanisms underlying the geochemical formation of geogenic OICs-contaminated groundwater remain unclear. Based upon multitarget field monitoring in combination with ultrahigh-resolution molecular characterization of organic components for alluvial-lacustrine aquifers, we identified a total of 939 OICs in groundwater under reducing and circumneutral pH conditions. In comparison to those in water-soluble organic matter (WSOM) in sediments, the OICs in dissolved organic matter (DOM) in groundwater typically contain fewer polycyclic aromatics and polyphenol compounds but more highly unsaturated compounds. Consequently, there were two major sources of geogenic OICs in groundwater: the migration of the OICs from aquifer sediments and abiotic reduction of iodate coupled with DOM iodination under reducing conditions. DOM iodination occurs primarily through the incorporation of reactive iodine that is generated by iodate reduction into highly unsaturated compounds, preferably containing hydrophilic functional groups as binding sites. It leads to elevation of the concentration of the OICs up to 183 µg/L in groundwater. This research provides new insights into the constraints of DOM molecular composition on the mobilization and enrichment of OICs in alluvial-lacustrine aquifers and thus improves our understanding of the genesis of geogenic iodine-contaminated groundwater systems.
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Água Subterrânea , Iodo , Poluentes Químicos da Água , Iodatos , Poluentes Químicos da Água/análise , Água Subterrânea/química , Água , Monitoramento AmbientalRESUMO
To better understand the impact of long-term irrigation practices on arsenic (As) accumulation in agricultural soils, 100 soil samples from depths of 0-20â¯cm were collected from the Datong basin, where the As-contaminated groundwater has been used for irrigation for several decades. Soil samples were analyzed for major elements, trace elements, and As, Fe speciation. Results reveal As content ranging from 4.00 to 14.5â¯mg/kg, an average of 10.2 ± 2.05â¯mg/kg, consistent with surveys conducted in 1998 and 2007. Arsenic speciation ranked in descending order as follows: As associated with silicate minerals (AsSi, 29.70 ± 7.53â¯%) > amorphous Fe-minerals associated As (AsFeox1, 26.40 ± 3.27â¯%) > crystalline Fe-minerals associated As (AsFeox2, 24.02 ± 4.60â¯%) > strongly adsorbed As (AsSorb, 14.29 ± 2.81â¯%) > As combined with carbonates and Fe-carbonates (AsCar, 2.30 ± 0.44â¯%) > weakly adsorbed As (AsDiss, 2.59 ± 1.00â¯%). The anomalous negative correlation between As and Fe content reflects the primary influence of soil provenance. Evidence from major element compositions and rare earth element patterns indicates that total As and Fe contents in soils are controlled by parent materials, exhibiting distinct north-south differences (As: higher levels in the north, lower levels in the south; Fe: higher levels in the south, lower levels in the north). Evidence from the Chemical Index of Alteration (CIA) and As/Ti ratio suggests that chemical weathering has led to As enrichment in the central basin. Notably, relationships such as AsDiss/Ti, AsSorb/Ti with CIA and total Fe content indicate significant influences of irrigation practices on adsorbed As (both weakly and strongly adsorbed) contents, showing a pattern of higher levels in the central basin and lower levels in the Piedmont. However, total As content remained stable after long-term irrigation, potentially due to the re-release of accumulated As via geochemical pathways during non-irrigated periods. These findings demonstrate that the soil systems can naturally remediate exogenous As contamination induced by irrigation practices. Quantitative assessment of the balance between As enrichment and re-release in soil systems is crucial for preventing soil As contamination, highlighting strategies like water-saving techniques and fallow periods to manage As contamination in agricultural areas using As-contaminated groundwater for irrigation.
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The spatial heterogeneity of arsenic (As) concentration exceeding the 10 µg/L WHO limit at the field scale poses significant challenges for groundwater utilization, but it remains poorly understood. To address this knowledge gap, the Daying site was selected as a representative case (As concentration ranged from 1.55 to 2237 µg/L within a 250 × 150 m field), and a total of 28 groundwater samples were collected and analyzed for hydrochemistry, As speciation, and stable hydrogen and oxygen isotope. Principal component analysis was employed to identify the primary factors controlling groundwater hydrochemistry. Results indicate that the spatial heterogeneity of groundwater As concentration is primarily attributed to vertical recharge and competitive adsorption. Low vertical recharge introduces reductive substances, such as dissolved organic matter, which enhances the reductive environment and facilitates microbial-induced reduction and mobilization of As. Conversely, areas with high vertical recharge introduce oxidizing agents like SO42- and DO, which act as preferred electron acceptors over Fe(III), thus inhibiting the reductive dissolution of Fe(III) oxides and the mobilization of As. PCA and hydrochemistry jointly indicate that spatial variability of P and its competitive adsorption with As are important factors leading to spatial heterogeneity of groundwater As concentration. However, the impacts of pH, Si, HCO3-, and F- on As adsorption are insignificant. Specifically, low vertical recharge can increase the proportion of As(III) and promote P release through organic matter mineralization. This process further leads to the desorption of As, indicating a synergistic effect between low vertical recharge and competitive adsorption. This field-scale spatial heterogeneity underscores the critical role of hydrogeological conditions. Sites with close hydraulic connections to surface water often exhibit low As concentrations in groundwater. Therefore, when establishing wells in areas with widespread high-As groundwater, selecting sites with open hydrogeological conditions can prove beneficial.
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Arsênio , Água Subterrânea , Poluentes Químicos da Água , Arsênio/análise , Compostos Férricos , Poluentes Químicos da Água/análise , Monitoramento Ambiental , Água Subterrânea/química , OxidantesRESUMO
OBJECTIVE: To analyze the clinical phenotype and genetic characteristics for a child with Canavan disease. METHODS: A child who was admitted to the Children's Hospital Affiliated to Shandong University on April 9, 2021 for inability to uphold his head for 2 months and increased muscle tone for one week was subjected to whole exome sequencing, and candidate variants were verified by Sanger sequencing. RESULTS: Genetic testing revealed that the child has harbored compound heterozygous variants of the ASPA gene, including a paternally derived c.556_559dupGTTC (p. L187Rfs*5) and a maternally derived c.919delA (p. S307Vfs*24). Based on the guidelines from the American College of Medical Genetics and Genomics, both variants were predicted to be pathogenic (PVS1+PM2_Supporting+PM3). CONCLUSION: The c.556_559dupGTTC (p.L187Rfs*5) and c.919delA (p.S307Vfs*24) compound heterozygous variants of the ASPA gene probably underlay the pathogenesis of Canavan disease in this child.
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Doença de Canavan , Criança , Humanos , Doença de Canavan/genética , Testes Genéticos , Genômica , Mutação , FenótipoRESUMO
BACKGROUND: Influenza A viruses have undergone rapid evolution with virulent; however, complete and comprehensive data on gene evolution and amino acid variation of HA and NA in immunosuppressed patients was few. In this study, we analysed molecular epidemiology and evolution of influenza A viruses in immunosuppressed population, and immunocompetent population were used as controls. METHODS: Full sequences of HA and NA of A(H1N1)pdm09 and A(H3N2) were acquired through reverse transcription-polymerase chain reaction (RT-PCR). HA and NA genes were sequenced using the Sanger method and phylogenetically analysed using ClustalW 2.10 and MEGA software version 11.0. RESULTS: During the 2018-2020 influenza seasons, 54 immunosuppressed and 46 immunocompetent inpatients screened positive for influenza A viruses by using the quantitative real-time PCR (qRT-PCR) were enrolled. 27 immunosuppressed and 23 immunocompetent nasal swab or bronchoalveolar lavage fluid samples were randomly selected and sequenced using the Sanger method. A(H1N1)pdm09 were detected in 15 samples and the remaining 35 samples were A(H3N2) positive. By analyzing the HA and NA gene sequences of these virus strains, we found that all A(H1N1)pdm09 viruses shared high similarities to each other and the HA and NA genes of these viruses exclusively belonged to subclade 6B.1A.1. Some NA genes of A(H3N2) viruses were not in the same clade as those of A/Singapore/INFIMH-16-0019/2016 and A/Kansas/14/2017, which may have led to A(H3N2) being the dominant strain in the 2019-2020 influenza season. Both A(H1N1)pdm09 and A(H3N2) viruses showed similar evolutionary lineages patterns of HA and NA between immunosuppressed and immunocompetent patients. Compared with the vaccine strains, there were no statistically significant of HA and NA genes and amino acid sequences of influenza A viruses in immunosuppressed and immunocompetent patients. However, the oseltamivir resistance substitution of NA-H275Y and R292K have been observed in immunosuppressed patients. CONCLUSIONS: A(H1N1)pdm09 and A(H3N2) viruses showed similar evolutionary lineages patterns of HA and NA between immunosuppressed and immunocompetent patients. Both immunocompetent and immunosuppressed patients have some key substitutions, which should be of note monitored, especially those with potential to affect the viral antigen.
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Vírus da Influenza A Subtipo H1N1 , Vírus da Influenza A , Influenza Humana , Humanos , Vírus da Influenza A/genética , Influenza Humana/epidemiologia , Vírus da Influenza A Subtipo H1N1/genética , Vírus da Influenza A Subtipo H3N2/genética , Filogenia , Estações do Ano , Pacientes Internados , Pequim , Glicoproteínas de Hemaglutininação de Vírus da Influenza/genética , Neuraminidase/genéticaRESUMO
Chitosanases hydrolyze chitosan into chitooligosaccharides (COSs) with various biological activities, which are widely employed in many areas including plant disease management. In this study, the novel chitosanase AqCsn1 belonging to the glycoside hydrolase family 46 (GH46) was cloned from Aquabacterium sp. A7-Y and heterologously expressed in Escherichia coli BL21 (DE3). AqCsn1 displayed the highest hydrolytic activity towards chitosan with 95% degree of deacetylation at 40 °C and pH 5.0, with a specific activity of 13.18 U/mg. Product analysis showed that AqCsn1 hydrolyzed chitosan into (GlcN)2 and (GlcN)3 as the main products, demonstrating an endo-type cleavage pattern. Evaluation of antagonistic activity showed that the hydrolysis products of AqCsn1 suppress the mycelial growth of Magnaporthe oryzae and Phytophthora sojae in a concentration-dependent manner, and the inhibition rate of P. sojae reached 39.82% at a concentration of 8 g/L. Our study demonstrates that AqCsn1 and hydrolysis products with a low degree of polymerization might have potential applications in the biological control of agricultural diseases.
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Quitosana , Quitosana/farmacologia , Polimerização , Quitina , Oligossacarídeos/farmacologia , Glicosídeo Hidrolases/genética , Glicosídeo Hidrolases/química , Hidrólise , Escherichia coli/genéticaRESUMO
Mollisols are critical agricultural resources for securing global food supply. Due to its health importance, selenium (Se) fate in the Mollisols attracts growing concerns. Land use change from conventional drylands to paddy wetlands impacts Se bioavailability in the vulnerable Mollisol agroecosystems. The underlying processes and mechanisms however remain elusive. Here, results of flow-through reactor experiments with paddy Mollisols from northern cold-region sites indicate that continuous flooding with surface water for 48 d induced redox zonation that facilitated the loss of Mollisol Se by up to 51%. Further process-based biogeochemical modeling suggests largest degradation rates of dissolved organic matter (DOM) in 30 cm deep Mollisols that contained the highest-level labile DOM and organic-bound Se. Electron shunting from degradation of Se-bearing DOM coupled to reductive dissolution of Se-adsorbed Fe oxides accounts mainly for Se(IV) release into the pore water. Consequent changes in DOM molecular composition make the reservoir of organic-bound Se vulnerable to flooding-induced redox zonation and likely enhance Se loss through destruction of thiolated Se and emission of gaseous Se from the Mollisol layer. This study highlights a neglected scenario where the speciation-driven loss of bioavailable Se from the paddy wetlands can be a significant consequence in the cold-region Mollisol agroecosystems.
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Selênio , Selênio/química , Solo/química , Áreas Alagadas , Agricultura , ÁguaRESUMO
Microorganisms play crucial roles in the global iodine cycling through iodine oxidation, reduction, volatilization, and deiodination. In contrast to iodate formation in radionuclide-contaminated groundwater by the iodine-oxidizing bacteria, microbial contribution to the formation of high level of iodide in geogenic high iodine groundwater is poorly understood. In this study, our results of comparative metagenomic analyses of deep groundwater with typical high iodide concentrations in the North China Plain revealed the existence of putative dissimilatory iodate-reducing idrABP1P2 gene clusters in groundwater. Heterologous expression and characterization of an identified idrABP1P2 gene cluster confirmed its functional role in iodate reduction. Thus, microbial dissimilatory iodate reduction could contribute to iodide formation in geogenic high iodine groundwater. In addition, the identified iron-reducing, sulfur-reducing, sulfur-oxidizing, and dehalogenating bacteria in the groundwater could contribute to the release and production of iodide through the reductive dissolution of iron minerals, abiotic iodate reduction of derived ferrous iron and sulfide, and dehalogenation of organic iodine, respectively. These microbially mediated iodate reduction and organic iodine dehalogenation processes may also result in the transformation among iodine species and iodide enrichment in other geogenic iodine-rich groundwater systems worldwide.
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Água Subterrânea , Iodo , Poluentes Químicos da Água , Iodetos/análise , Iodatos/análise , Iodo/análise , Ferro , Bactérias/genética , Bactérias/metabolismo , Oxirredução , China , Enxofre/análise , Poluentes Químicos da Água/análiseRESUMO
The genesis of geogenic iodine (I)-contaminated groundwater poses a significant threat to long-term water exploitation. Safe and sustainable water supply, particularly in the northern arid basins, demands a quantitative prediction of the high variability of I distribution over hydrogeological timescales. Here, bioenergetics-informed reactive transport modeling was combined with high-resolution molecular characterization of fueling organic matter to decipher the time-controlled interactions between vertical flow and (bio)geochemical processes in I transport within the Datong aquifers. The declining reactivities of I-bearing organic matter and Fe oxides in the 15-40 m depth decreased the rate of I release, while a growing number of pore volumes flushed through the aquifers to leach out I- and organic I. This removal effect is compensated by the desorption of I- from Fe oxides and secondary FeS generated from the concurrent reduction of Fe oxides and SO42-. Consequently, peak concentrations of groundwater I- may have appeared, depending upon the vertical recharge rate, at the first several pore volumes flushed through the aquifers. The current vertical distributions of the various I species likely represent a quasi-steady state between I mobilization and leaching. These new mechanistic insights into the dynamic hydrogeological-(bio)geochemical processes support secure groundwater use in the I-affected northern arid basins.
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Arsênio , Água Subterrânea , Iodo , Poluentes Químicos da Água , Poluentes Químicos da Água/análise , Monitoramento Ambiental , Água Subterrânea/química , Abastecimento de Água , ÓxidosRESUMO
Mollisols support the most productive agroecosystems in the world. Despite their critical links to food quality and human health, the varying distributions of selenium (Se) species and factors governing Se mobility in the mollisol vadose zone remain elusive. This research reveals that, in northern mollisol agroecosystems, Se hotspots (≥0.32 mg/kg) prevail along the regional river systems draining the Lesser Khingan Mountains, where piedmont Se-rich oil shales are the most probable source of regional Se. While selenate and selenite dominate Se species in the water-soluble and absorbed pools, mollisol organic matter is the major host for Se. Poorly crystalline and crystalline Fe oxides are subordinate in Se retention, hosting inorganic and organic Se at levels comparable to those in the adsorbed pool. The depth-dependent distributions of mollisol Se species for the non-cropland and cropland sites imply a predominance of reduced forms of Se under the mildly acidic and reducing conditions that, in turn, are variably impacted by agricultural land use. These findings therefore highlight that fluvial deposition and land use change together are the main drivers of the spatial variability and speciation of mollisol Se.
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Compostos de Selênio , Selênio , Humanos , Ácido Selenioso , Agricultura , Ácido Selênico , ÁguaRESUMO
Bacterial sulfate reduction plays a crucial role in the mobilization of toxic substances in aquifers. However, the role of bacterial sulfate reduction on iodine mobilization in geogenic high-iodine groundwater systems has been unexplored. In this study, the enrichment of groundwater δ34SSO4 (15.56 to 69.31) and its significantly positive correlation with iodide and total iodine concentrations in deep groundwater samples of the North China Plain suggested that bacterial sulfate reduction participates in the mobilization of groundwater iodine. Similar significantly positive correlations were further observed between the concentrations of iodide and total iodine and the relative abundance of the dsrB gene by qPCR, as well as the composition and abundance of sulfate-reducing bacteria (SRB) predicted from 16S rRNA gene high-throughput sequencing data. Subsequent batch culture experiments by the SRB Desulfovibrio sp. B304 demonstrated that SRB could facilitate iodine mobilization through the enzyme-driven biotic and sulfide-driven abiotic reduction of iodate to iodide. In addition, the dehalogenation of organoiodine compounds by SRB and the reductive dissolution of iodine-bearing iron minerals by biogenic sulfide could liberate bound or adsorbed iodine into groundwater. The role of bacterial sulfate reduction in iodine mobilization revealed in this study provides new insights into our understanding of iodide enrichment in iodine-rich aquifers worldwide.
Assuntos
Arsênio , Água Subterrânea , Iodo , Poluentes Químicos da Água , Iodo/análise , Iodetos/análise , RNA Ribossômico 16S/genética , Bactérias/metabolismo , Sulfetos , Sulfatos/análise , China , Poluentes Químicos da Água/análiseRESUMO
The enrichment of geogenic phosphorus (P) in groundwater systems threatens environmental and public health worldwide. Two significant factors affecting geogenic P enrichment include organic matter (OM) and Fe (oxyhydr)oxide (FeOOH). However, due to variable reactivities of OM and FeOOH, variable strategies of their coupled influence controlling P enrichment in groundwater systems remain elusive. This research reveals that when the depositional environment is enriched in more labile aliphatic OM, its fermentation is coupled with the reductive dissolution of both amorphous and crystalline FeOOHs. When the depositional environment is enriched in more recalcitrant aromatic OM, it largely relies on crystalline FeOOH acting concurrently as electron acceptors while serving as "conduits" to help itself stimulate degradation and methanogenesis. The main source of geogenic P enriched by these two different coupled processes is different: the former is P-containing OM, which mainly contained unsaturated aliphatic compounds and highly unsaturated-low O compounds, and the latter is P associated with crystalline FeOOH. In addition, geological setting affects the deposition rate of sediments, which can alter OM degradation/preservation, and subsequently affects geochemical conditions of geogenic P occurrence. These findings provide new evidence and perspectives for understanding the hydro(bio)geochemical processes controlling geogenic P enrichment in alluvial-lacustrine aquifer systems.
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Arsênio , Água Subterrânea , Poluentes Químicos da Água , Fósforo , Poluentes Químicos da Água/análise , Água Subterrânea/química , Óxidos , Monitoramento Ambiental , Sedimentos Geológicos/químicaRESUMO
Iodate (IO3-) can be abiotically reduced by Fe(II) or biotically reduced by the dissimilatory Fe(III)-reducing bacterium Shewanella oneidensis (MR-1) via its DmsEFAB and MtrCAB. However, the intermediates and stoichiometry between the Fe(II) and IO3- reaction and the relative contribution of abiotic and biotic IO3- reduction by biogenic Fe(II) and MR-1 in the presence of Fe(III) remain unclear. In this study, we found that abiotic reduction of IO3- by Fe(II) produced intermediates HIO and I- at a ratio of 1:2, followed by HIO disproportionation to I- and IO3-. Comparative analyses of IO3- reduction by MR-1 wild type (WT), MR-1 mutants deficient in DmsEFAB or MtrCAB, and Shewanella sp. ANA-3 in the presence of Fe(III)-citrate, Fe(III) oxides, or clay minerals showed that abiotic IO3- reduction by biogenic Fe(II) predominated under iron-rich conditions, while biotic IO3- reduction by DmsEFAB played a more dominant role under iron-poor conditions. Compared to that in the presence of Fe(III)-citrate, MR-1 WT reduced more IO3- in the presence of Fe(III) oxides and clay minerals. The observed abiotic and biotic IO3- reduction by MR-1 under Fe-rich and Fe-limited conditions suggests that Fe(III)-reducing bacteria could contribute to the transformation of iodine species and I- enrichment in natural iodine-rich environments.
Assuntos
Iodo , Shewanella , Compostos Férricos , Oxirredução , Iodatos , Argila , Óxidos , Ferro , Compostos Ferrosos , Minerais , CitratosRESUMO
Naturally occurring (i.e., geogenic) ammonium in groundwater has been widely detected globally, but the major controls on its regional distribution have been poorly characterized. Here, we identified the dominant role of paleo-geomorphology driven by paleo-climate in controlling the spatial variability of geogenic ammonium in groundwater using random forest algorithm and revealed the underlying mechanisms based on borehole sediment analysis of data obtained from the Dongting Lake Plain of the central Yangtze River basins in China. In the paleo-channel (PC) area, the aquifer depth-matched sediments were deposited during the last deglaciation when warm climate resulted in rapid filling into incised valleys, and terrestrial organic matter (OM) mainly as lignin experienced less degradation prior to sedimentation and had lower humification, higher N abundance, and nominal oxidation state of carbon (NOSC). In the paleo-interfluve (PI) area, the depth-matched sediments were deposited during the last glaciation, followed by intensive erosion in the surface during the last glacial maximum, and terrestrial OM mainly as lignin had been partly degraded into aliphatics prior to sedimentation and had higher humification, lower N abundance, and NOSC. As a result, under the present anaerobic conditions, less-humic and N-rich OM with more oxidized C tends to be more intensively mineralized into ammonium in the PC area than those in the PI area. These findings highlight the importance of paleo-geomorphology with paleo-climate in controlling the enrichment of geogenic ammonium in groundwater, which has a universal significance for understanding the genesis and distribution of high N loads in the aquatic environment worldwide.