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1.
J Org Chem ; 87(7): 4649-4653, 2022 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-35200013

RESUMO

To improve the rigidity of spirobisindane, it was intramolecularly locked by forming eight-membered rings via sulfur and phosphorus atoms to produce an interlocked polycyclic structure under mild conditions in good yields. By carefully analyzing the crystal structures, we noticed that the angle between the two benzene rings in the locked version is significantly smaller than that of the typical spirobisindane structure. Molecular modeling indicated that locking the spiro center can remarkably enhance the rigidity.


Assuntos
Carbono , Fósforo , Cristalografia por Raios X , Modelos Moleculares , Fósforo/química , Enxofre
2.
Microbiome ; 10(1): 75, 2022 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-35538590

RESUMO

BACKGROUND: The deep sea harbors the majority of the microbial biomass in the ocean and is a key site for organic matter (OM) remineralization and storage in the biosphere. Microbial metabolism in the deep ocean is greatly controlled by the generally depleted but periodically fluctuating supply of OM. Currently, little is known about metabolic potentials of dominant deep-sea microbes to cope with the variable OM inputs, especially for those living in the hadal trenches-the deepest part of the ocean. RESULTS: In this study, we report the first extensive examination of the metabolic potentials of hadal sediment Chloroflexi, a dominant phylum in hadal trenches and the global deep ocean. In total, 62 metagenome-assembled-genomes (MAGs) were reconstructed from nine metagenomic datasets derived from sediments of the Mariana Trench. These MAGs represent six novel species, four novel genera, one novel family, and one novel order within the classes Anaerolineae and Dehalococcoidia. Fragment recruitment showed that these MAGs are globally distributed in deep-sea waters and surface sediments, and transcriptomic analysis indicated their in situ activities. Metabolic reconstruction showed that hadal Chloroflexi mainly had a heterotrophic lifestyle, with the potential to degrade a wide range of organic carbon, sulfur, and halogenated compounds. Our results revealed for the first time that hadal Chloroflexi harbor pathways for the complete hydrolytic or oxidative degradation of various recalcitrant OM, including aromatic compounds (e.g., benzoate), polyaromatic hydrocarbons (e.g., fluorene), polychlorobiphenyl (e.g., 4-chlorobiphenyl), and organochlorine compounds (e.g., chloroalkanes, chlorocyclohexane). Moreover, these organisms showed the potential to synthesize energy storage compounds (e.g., trehalose) and had regulatory modules to respond to changes in nutrient conditions. These metabolic traits suggest that Chloroflexi may follow a "feast-or-famine" metabolic strategy, i.e., preferentially consume labile OM and store the energy intracellularly under OM-rich conditions, and utilize the stored energy or degrade recalcitrant OM for survival under OM-limited condition. CONCLUSION: This study expands the current knowledge on metabolic strategies in deep-ocean Chlorolfexi and highlights their significance in deep-sea carbon, sulfur, and halogen cycles. The metabolic plasticity likely provides Chloroflexi with advantages for survival under variable and heterogenic OM inputs in the deep ocean. Video Abstract.


Assuntos
Chloroflexi , Carbono/metabolismo , Chloroflexi/genética , Ecossistema , Oceanos e Mares , Enxofre/metabolismo
3.
Zhongguo Zhong Yao Za Zhi ; 47(7): 1864-1870, 2022 Apr.
Artigo em Chinês | MEDLINE | ID: mdl-35534256

RESUMO

In order to realize the rapid and non-destructive detection of SO_2 content in sulphur-fumigated Achyranthis Bidentatae Radix, this paper first prepared the sulphur-fumigated Achyranthis Bidentatae Radix samples with the usage amount of sulphur being 0, 2.5%, and 5% of the mass of Achyranthis Bidentatae Radix pieces. The SO_2 content in different batches of sulphur-fumigated Achyranthis Bidentatae Radix was determined using the method in Chinese Pharmacopoeia, followed by the acquisition of their hyperspectral data within both visible-near infrared(435-1 042 nm) and short-wave infrared(898-1 751 nm) regions by hyperspectral imaging. Meanwhile, the first derivative, AUTO, multiplicative scatter correction, Savitzky-Golay(SG) smoothing, and standard normal variable transformation algorithms were used to pre-process the original hyperspectral data, which were then subjected to characteristic band extraction based on competitive adaptive reweighted sampling(CARS) and the partial least square regression analysis for building a quantitative model of SO_2 content in sulphur-fumigated Achyranthis Bidentatae Radix. It was found that the accuracy of the quantitative model built depending on the visible-near infrared spectra was high, with the determination coefficient of prediction set(R■) reaching 0.900 1. The established quantitative model has enabled the rapid and non-destructive detection of SO_2 content in sulphur-fumigated Achyranthis Bidentatae Radix, which can serve as an effective supplement to the method described in Chinese Pharmacopeia.


Assuntos
Imageamento Hiperespectral , Raízes de Plantas , Análise dos Mínimos Quadrados , Enxofre
4.
Ecotoxicol Environ Saf ; 236: 113479, 2022 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-35366561

RESUMO

Effects of iron and sulfur redox states in the soil caused by different growth seasons on Cd uptake by rice remain unclear. In this study, three early rice cultivars and three late rice cultivars were cultivated in a double-cropping system in Cd-contaminated paddy fields. The total Cd accumulation of early rice cultivars was 20.5-51.1 µg plant-1, and the Cd concentration in grains was 0.19-0.73 mg kg-1, significantly lower than those of late rice cultivars by 8-15 times and 3-9 times, respectively. The filling and mature stages were identified as the most crucial stages of Cd uptake by both early and late rice cultivars. The growth season of early rice cultivars was characterized by more abundant rainfall and lower soil Eh than that for late rice cultivars. Therefore, the abundances of Fe-reducing bacteria (FeRB, 36.9-39%) and S-reducing bacteria (SRB, 1.77-2.79%) were higher during the filling and mature stages of early rice. They primarily belonged to the Clostridium, Geobacter, and Desulfuromonadales genera. Stimulation of FeRB and SRB activity promoted Fe(III) and S reduction and increased the content of Fe2+ and S2- in rhizosphere soil. This promoted the binding of Cd to amorphous Fe oxides and sulfides or Fe sulfides, thereby decreasing the available Cd content. Moreover, the Cd in the iron plaque (IP) and Cd transfer from IP to roots were lower in early rice. These findings suggest that maintaining high moisture content in the soil during the filling and mature stages, especially for late rice cultivars, could efficiently reduce Cd uptake by rice planted in contaminated soil.


Assuntos
Oryza , Poluentes do Solo , Cádmio/metabolismo , Ferro/química , Oryza/metabolismo , Estações do Ano , Solo/química , Poluentes do Solo/análise , Sulfetos/metabolismo , Enxofre/metabolismo
5.
J Am Chem Soc ; 144(16): 7189-7197, 2022 Apr 27.
Artigo em Inglês | MEDLINE | ID: mdl-35436110

RESUMO

A multi-component approach to structurally complex organosulfur products is described via the nickel-catalyzed 1,2-carbosulfenylation of unactivated alkenes with organoboron nucleophiles and tailored organosulfur electrophiles. The key to the development of this transformation is the identification of a modular N-alkyl-N-(arylsulfenyl)arenesulfonamide family of sulfur electrophiles. Tuning the electronic and steric properties of the leaving group in these reagents controls pathway selectivity, favoring three-component coupling and suppressing side reactions, as examined via computational studies. The unique syn-stereoselectivity differs from traditional electrophilic sulfenyl transfer processes involving a thiiranium ion intermediate and arises from the directed arylnickel(I) migratory insertion mechanism, as elucidated through reaction kinetics and control experiments. Reactivity and regioselectivity are facilitated by a collection of monodentate, weakly coordinating native directing groups, including sulfonamides, alcohols, amines, amides, and azaheterocycles.


Assuntos
Alcenos , Níquel , Catálise , Indicadores e Reagentes , Enxofre
6.
Microbiol Spectr ; 10(2): e0026422, 2022 Apr 27.
Artigo em Inglês | MEDLINE | ID: mdl-35377234

RESUMO

Ralstonia solanacearum, which causes bacterial wilt disease of many crops, requires denitrifying respiration to survive in its plant host. In the hypoxic environment of plant xylem vessels, this pathogen confronts toxic oxidative radicals like nitric oxide (NO), which is generated by both bacterial denitrification and host defenses. R. solanacearum has multiple distinct mechanisms that could mitigate this stress, including putative NO-binding protein (NorA), nitric oxide reductase (NorB), and flavohaemoglobin (HmpX). During denitrification and tomato pathogenesis and in response to exogenous NO, R. solanacearum upregulated norA, norB, and hmpX. Single mutants lacking ΔnorB, ΔnorA, or ΔhmpX increased expression of many iron and sulfur metabolism genes, suggesting that the loss of even one NO detoxification system demands metabolic compensation. Single mutants suffered only moderate fitness reductions in host plants, possibly because they upregulated their remaining protective genes. However, ΔnorA/norB, ΔnorB/hmpX, and ΔnorA/hmpX double mutants grew poorly in denitrifying culture and in planta. It is likely that the loss of norA, norB, and hmpX is lethal, since the methods used to construct the double mutants could not generate a triple mutant. Functional aconitase activity assays showed that NorA, HmpX, and especially NorB are important for maintaining iron-sulfur cluster proteins. Additionally, plant defense genes were upregulated in tomatoes infected with the NO-overproducing ΔnorB mutant, suggesting that bacterial detoxification of NO reduces the ability of the plant host to perceive the presence of the pathogen. Thus, R. solanacearum's three NO detoxification systems each contribute to and are collectively essential for overcoming metabolic nitrosative stress during denitrification, for virulence and growth in the tomato, and for evading host plant defenses. IMPORTANCE The soilborne plant pathogen Ralstonia solanacearum (Rs) causes bacterial wilt, a serious and widespread threat to global food security. Rs is metabolically adapted to low-oxygen conditions, using denitrifying respiration to survive in the host and cause disease. However, bacterial denitrification and host defenses generate nitric oxide (NO), which is toxic and also alters signaling pathways in both the pathogen and its plant hosts. Rs mitigates NO with a trio of mechanistically distinct proteins: NO-reductase (NorB), predicted iron-binding (NorA), and oxidoreductase (HmpX). This redundancy, together with analysis of mutants and in-planta dual transcriptomes, indicates that maintaining low NO levels is integral to Rs fitness in tomatoes (because NO damages iron-cluster proteins) and to evading host recognition (because bacterially produced NO can trigger plant defenses).


Assuntos
Lycopersicon esculentum , Ralstonia solanacearum , Desnitrificação , Ferro/metabolismo , Ferro/toxicidade , Lycopersicon esculentum/metabolismo , Lycopersicon esculentum/microbiologia , Óxido Nítrico/metabolismo , Oxirredutases/metabolismo , Doenças das Plantas/microbiologia , Plantas/metabolismo , Ralstonia solanacearum/genética , Enxofre/metabolismo
7.
Inorg Chem ; 61(16): 5991-6007, 2022 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-35403427

RESUMO

Redox potentials have been calculated for 12 different iron-sulfur sites of 6 different types with 1-4 iron ions. Structures were optimized with combined quantum mechanical and molecular mechanical (QM/MM) methods, and the redox potentials were calculated using the QM/MM energies, single-point QM methods in a continuum solvent or by QM/MM thermodynamic cycle perturbations. We show that the best results are obtained with a large QM system (∼300 atoms, but a smaller QM system, ∼150 atoms, can be used for the QM/MM geometry optimization) and a large value of the dielectric constant (80). For absolute redox potentials, the B3LYP density functional method gives better results than TPSS, and the results are improved with a larger basis set. However, for relative redox potentials, the opposite is true. The results are insensitive to the force field (charges of the surroundings) used for the QM/MM calculations or whether the protein and solvent outside the QM system are relaxed or kept fixed at the crystal structure. With the best approach for relative potentials, mean absolute and maximum deviations of 0.17 and 0.44 V, respectively, are obtained after removing a systematic error of -0.55 V. Such an approach can be used to identify the correct oxidation states involved in a certain redox reaction.


Assuntos
Benchmarking , Ferro , Oxirredução , Proteínas/química , Teoria Quântica , Solventes , Enxofre
8.
Sensors (Basel) ; 22(7)2022 Mar 24.
Artigo em Inglês | MEDLINE | ID: mdl-35408102

RESUMO

In this study, nitrogen and sulfur co-doped carbon dots (NS-CDs) were investigated for the detection of heavy metals in water through absorption-based colorimetric response. NS-CDs were synthesized by a simple one-pot hydrothermal method and characterized by TEM, STEM-coupled with energy dispersive X-ray analysis, NMR, and IR spectroscopy. Addition of Cu(II) ions to NS-CD aqueous solutions gave origin to a distinct absorption band at 660 nm which was attributed to the formation of cuprammonium complexes through coordination with amino functional groups of NS-CDs. Absorbance increased linearly with Cu(II) concentration in the range 1-100 µM and enabled a limit of detection of 200 nM. No response was observed with the other tested metals, including Fe(III) which, however, appreciably decreased sensitivity to copper. Increase of pH of the NS-CD solution up to 9.5 greatly reduced this interference effect and enhanced the response to Cu(II), thus confirming the different nature of the two interactions. In addition, a concurrent response to Co(II) appeared in a different spectral region, thus suggesting the possibility of dual-species multiple sensitivity. The present method neither requires any other reagents nor any previous assay treatment and thus can be a promising candidate for low-cost monitoring of copper onsite and by unskilled personnel.


Assuntos
Carbono , Pontos Quânticos , Carbono/química , Cobalto , Colorimetria/métodos , Cobre/análise , Compostos Férricos , Nitrogênio/química , Pontos Quânticos/química , Enxofre , Água
9.
Proc Natl Acad Sci U S A ; 119(17): e2119032119, 2022 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-35439051

RESUMO

SignificanceIodine-induced cleavage is widely used for detecting bacterial DNA phosphorothioation in gel electrophoresis, deep sequencing, and single-molecule optical mapping. However, we lack quantitative understanding of the phosphorothioate DNA (PT-DNA) cleavage efficiency and the chemoselectivity of this method for determination of phosphorothioate vs. phosphate. Computational explorations now reveal why iodine selectively attacks at sulfur in phosphorothioate links but not at normal phosphates. The active role of Tris buffer in the PT-DNA cleavage, and the factors controlling cleavage efficiency, were also revealed. Cleavage efficiency is limited by competition between the desired DNA backbone cleavage and unwanted P-S/P-O conversion. These mechanistic studies will guide the development of new methods for iodine-induced specific PT-DNA cleavage.


Assuntos
Iodo , Clivagem do DNA , DNA Bacteriano/genética , Iodetos , Fosfatos/química , Enxofre
10.
Water Res ; 216: 118381, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-35381430

RESUMO

Dark carbon fixation (DCF) contributes approximately 0.77 Pg C y-1 to oceanic primary production and the global carbon budget. It is estimated that nearly half of the DCF in marine sediments occurs in estuarine and coastal regions, but the environmental factors controlling DCF and the microorganisms responsible for its production remain under exploration. In this study, we investigated DCF rates and the active chemoautotrophic microorganisms in intertidal sediments of the Yangtze Estuary, using 14C-labeling and DNA-stable isotope probing (DNA-SIP) techniques. The measured DCF rates ranged from 0.27 to 3.37 mmol C m-2 day-1 in intertidal surface sediments. The rates of DCF were closely related to sediment sulfide content, demonstrating that the availability of reductive substrates may be the dominant factor controlling DCF in the intertidal sediments. A significant positive correlation was also observed between the DCF rates and abundance of the cbbM gene. DNA-stable isotope probing (DNA-SIP) results further confirmed that cbbM-harboring bacteria, rather than cbbL-harboring bacteria, played a dominant role in DCF in intertidal sediments. Phylogenetic analysis showed that the predominant cbbM-harboring bacteria were affiliated with Burkholderia, including Sulfuricella denitrificans, Sulfuriferula, Acidihalobacter, Thiobacillus, and Sulfurivermis fontis. Moreover, metagenome analyses indicated that most of the potential dark-carbon-fixing bacteria detected in intertidal sediments also harbor genes for sulfur oxidation, denitrification, or dissimilatory nitrate reduction to ammonium (DNRA), indicating that these chemoautotrophic microorganisms may play important roles in coupled carbon, nitrogen, and sulfur cycles. These results shed light on the ecological importance and the underlying mechanisms of the DCF process driven by chemoautotrophic microorganisms in intertidal wetlands.


Assuntos
Bactérias , Ciclo do Carbono , Bactérias/genética , Carbono , DNA , Sedimentos Geológicos/química , Nitratos/análise , Nitrogênio , Filogenia , Enxofre
11.
Bioengineered ; 13(4): 10026-10037, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-35436415

RESUMO

Many dysregulated lncRNAs have been reported to perform an integral function in hepatocellular carcinoma (HCC). However, the role of long non-coding RNA (lncRNA) NRAV in HCC has not been elucidated. To address this issue, we investigated the function of NRAV in HCC in this research. Through bioinformatics prediction and real-time quantitative polymerase chain reaction validation, we found that NRAV plays an upmodulating role in HCC cells and tissues, and patients with high NRAV expression showed a poor prognosis. Cell viability was examined by conducting a Cell Counting Kit-8 analysis. Subsequently, the proliferation capacity of the cells was analyzed utilizing cell colony formation assay, and transwell invasion experiments were conducted to identify the cell invasion ability. To determine the association between NRAV and miR-199a-3p, and CDGSH iron-sulfur domain-containing protein 2 (CISD2), we conducted a dual luciferase assay. The protein and gene expressions were estimated utilizing Western blot. Findings illustrated that the overexpression of NRAV enhanced the HCC cell viability, proliferation and invasion, whereas they were inhibited significantly by down expression of NRAV. The dual-luciferase assay showed that miR-199a-3p is not only a target for NRAV but also interacts with the 3' UTR of CISD2 in HCC cells. MiR-199a-3p/CISD2 axis performs a function in NRAV-mediated cell behavior regulation. NRAV may trigger the Wnt/ß-catenin signaling via the modulation of the miR-199a-3p/CISD2 axis in HCC. The findings of this work can provide novel insights into clinical diagnosis and the treatment of HCC in the future.Abbreviations: HCC, hepatocellular carcinoma; LncRNA, long non-coding RNA; CISD2, CDGSH iron-sulfur domain-containing protein 2; CCK-8, Cell Counting Kit-8; cDNA, single-stranded complementary DNA; RT-qPCR, real-time quantitative polymerase chain reaction; BCA, bicinchoninic acid; ceRNA, competing endogenous RNAs.


Assuntos
Carcinoma Hepatocelular , Neoplasias Hepáticas , MicroRNAs , RNA Longo não Codificante , Regiões 3' não Traduzidas , Carcinoma Hepatocelular/metabolismo , Linhagem Celular Tumoral , Proliferação de Células/genética , Regulação Neoplásica da Expressão Gênica/genética , Humanos , Ferro/metabolismo , Neoplasias Hepáticas/genética , Neoplasias Hepáticas/patologia , MicroRNAs/genética , MicroRNAs/metabolismo , RNA Longo não Codificante/genética , RNA Longo não Codificante/metabolismo , Enxofre , Via de Sinalização Wnt/genética
12.
Phys Chem Chem Phys ; 24(16): 9176-9187, 2022 Apr 20.
Artigo em Inglês | MEDLINE | ID: mdl-35383346

RESUMO

Bacterial DNA phosphorothioation (PT) physiologically and stereo-specifically replaces a non-bridging oxygen in a phosphate link with a sulfur atom, which can be recognized by a highly conserved sulfur-binding domain (SBD). Here we conducted thermodynamic integration (TI), molecular dynamics simulation, and quantum chemical calculations to decipher the specific molecular interactions between PT-DNA and SBD in Streptomyces coelicolor type IV restriction enzyme ScoMcrA. The TI-calculated binding affinity of (5'-CCGRp-PSGCCGG-3')2 is larger than that of (5'-CCGGCCGG-3')2 by about 7.4-7.7 kcal mol-1. The binding difference dominantly stems from hydration energy of non-phosphorothioate DNA (9.8-10.6 kcal mol-1) in aqueous solution, despite the persistent preference of 2.6-3.2 kcal mol-1 in the DNA-SBD MD simulations. Furthermore, the quantum chemical calculations reveal an unusual non-covalent interaction in the phosphorothioate-binding scenario, where the PS⋯NP165 chalcogen bond prevails the PS⋯HCß vdW interactions from the adjacent residues H116-R117-Y164-P165-A168. Thus, the chalcogen-hydrophobic interaction pulls PT-DNA into the SBD binding pocket while the water cage pulls a normal DNA molecule out. The synergetic mechanism suggests the special roles of the proline pyrrolidine group in the SBD proteins, consistent with the experimental observations in the X-ray crystallography and structural bioinformatics analysis.


Assuntos
Enxofre , Água , DNA/química , DNA Bacteriano , Interações Hidrofóbicas e Hidrofílicas , Fosfatos/química , Enxofre/química
13.
PLoS One ; 17(4): e0266447, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35395053

RESUMO

Spinal deformity is a serious economic and animal welfare problem in intensive fish farming systems, which will be a significant unsolved problem for the fish sector. The aim of this study was to determine the relative expression of genes (Akt1 substrate 1, Calreticulin, Collagen type I alpha 2 chain, Corticotropin-releasing hormone, Chromodomain-Helicase DNA-binding, Growth hormone, Insulin like growth factor 1, Myostatin, Sine oculis-related homeobox 3, Toll-like receptor 2) in different tissues associated with spinal deformity and to determine the macroelement (calcium, magnesium, phosphorus, potassium, sodium, sulfur) and microelement (barium, copper, iron, manganese, strontium, zinc) content of spine in healthy and deformed common carps (Cyprinus carpio) in Hungary. The mRNA levels of the genes were measured in 7 different tissues (abdominal fat, blood, brain, dorsal muscle, genitals, heart, liver) by qRT-PCR. Correlations between gene expression and element content were analyzed by using linear regression and Spearman rank correlation. In a total of 15 cases, we found a statistically significant connection between gene expression in a tissue and the macro- or microelement content of the spine. In these contexts, the genes Akt1 substrate 1 (3), Collagen type I alpha 2 chain (2), Corticotropin-releasing hormone (4), Insulin-like growth factor 1 (4), and Myostatin (2), the tissue's blood (3), brain (6), heart (5), and liver (1), the macroelements sodium (4), magnesium (4), phosphorus (1) and sulfur (2) as well as the microelement iron (4) were involved. We also found statistically significant mRNA level differences between healthy and deformed common carps in tissues that were not directly affected by the deformation. Based on our results, genes regulating the nervous system and growth, elements, and tissues are the most associated components in the phenomenon of spinal deformity. With our study, we wish to give direction to and momentum for the exploration of these complex processes.


Assuntos
Carpas , Animais , Carpas/genética , Colágeno Tipo I , Hormônio Liberador da Corticotropina/genética , Ferro , Magnésio , Miostatina , Sistema Nervoso , Fósforo , RNA Mensageiro/genética , Sódio , Enxofre
14.
Mar Pollut Bull ; 178: 113603, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35390629

RESUMO

To assess the aquaculture-induced sediment conditions associated with sulfur cycles, shifts in bacterial communities across farming stages were investigated. The sulfate reduction rate (SRR), and concentrations of acid volatile sulfide (AVS) and H2S were significantly higher at the mid- and post-farming stages than at the early stage, indicating that the aquaculture effects persist even after harvest. Incomplete organic carbon-oxidizing sulfate-reducing bacteria (IO-SRB) affiliated with Desulfobulbaceae, and gammaproteobacterial sulfur oxidizing bacteria (SOB) (Thiohalobacter, Thioprofundum, and Thiohalomonas) were dominant during the early stage, whereas fermenting bacteria (Bacteroidetes and Firmicutes) and complete oxidizing SRB (CO-SRB) belonging to Desulfobacteraceae, and epsilonproteobacterial SOB (Sulfurovum) dominated during the mid- and post-stages. The shift in SRB and SOB communities well reflected the anoxic and sulfidic conditions of farm sediment. Especially, the Sulfurovum-like SOB correlated highly and positively with H2S, AVS, and SRR, suggesting that they could be relevant microbiological proxies to assess sulfidic conditions in farm sediment.


Assuntos
Bactérias , Pesqueiros , Sulfatos , Sulfetos , Enxofre
15.
Environ Sci Technol ; 56(9): 5960-5972, 2022 May 03.
Artigo em Inglês | MEDLINE | ID: mdl-35416037

RESUMO

Increasing global deoxygenation has widely formed oxygen-limited biotopes, altering the metabolic pathways of numerous microbes and causing a large greenhouse effect of nitrous oxide (N2O). Although there are many sources of N2O, denitrification is the sole sink that removes N2O from the biosphere, and the low-level oxygen in waters has been classically thought to be the key factor regulating N2O emissions from incomplete denitrification. However, through microcosm incubations with sandy sediment, we demonstrate here for the first time that the stress from oxygenated environments does not suppress, but rather boosts the complete denitrification process when the sulfur cycle is actively ongoing. This study highlights the potential of reducing N2O-driven greenhouse warming and fills a gap in pre-cognitions on the nitrogen cycle, which may impact our current understanding of greenhouse gas sinks. Combining molecular techniques and kinetic verification, we reveal that dominant inhibitions in oxygen-limited environments can interestingly undergo triple detoxification by cryptic sulfur and oxygen cycling, which may extensively occur in nature but have been long neglected by researchers. Furthermore, reviewing the present data and observations from natural and artificial ecosystems leads to the necessary revision needs of the global nitrogen cycle.


Assuntos
Desnitrificação , Oxigênio , Ecossistema , Ciclo do Nitrogênio , Enxofre
16.
Environ Sci Technol ; 56(9): 5808-5819, 2022 May 03.
Artigo em Inglês | MEDLINE | ID: mdl-35442653

RESUMO

Sulfidized nanoscale zerovalent iron (SNZVI) with desirable properties and reactivity has recently emerged as a promising groundwater remediation agent. However, little information is available on how the molecular structure of chlorinated ethenes (CEs) affects their dechlorination by SNZVI or whether the sulfur content of SNZVI can alter their dechlorination pathway and reactivity. Here, we show that the reactivity (up to 30-fold) and selectivity (up to 70-fold) improvements of SNZVI (compared to NZVI) toward CEs depended on the chlorine number, chlorine position, and sulfur content. Low CEs (i.e., vinyl chloride and cis-1,2-dichloroethene) and high CEs (perchloroethene) tended to be dechlorinated by SNZVI primarily via atomic H and direct electron transfer, respectively, while SNZVI could efficiently and selectively dechlorinate trichloroethene and trans-1,2-dichloroethene via both pathways. Increasing the sulfidation degree of SNZVI suppressed its ability to produce atomic H but promoted electron transfer and thus altered the relative contributions of atomic H and electron transfer to the CE dechlorination, resulting in different reactivities and selectivities. These were indicated by the correlations of CE dechlorination rates and improvements with CE molecular descriptors, H2 evolution rates, and electron transfer indicators of SNZVI. These mechanistic insights indicate the importance of determining the structure-specific properties and reactivity of both SNZVI materials and their target contaminants and can lead to a more rational design of SNZVI for in situ groundwater remediation of various CEs.


Assuntos
Ferro , Poluentes Químicos da Água , Cloro , Etilenos , Estrutura Molecular , Enxofre
17.
Appl Environ Microbiol ; 88(9): e0021622, 2022 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-35404072

RESUMO

Oxygen minimum zones (OMZs) are hot spots for redox-sensitive nitrogen transformations fueled by sinking organic matter. In comparison, the regulating role of sulfur-cycling microbes in marine OMZs, their impact on carbon cycling in pelagic and benthic habitats, and activities below the seafloor remain poorly understood. Using 13C DNA stable isotope probing (SIP) and metatranscriptomics, we explored microbial guilds involved in sulfur and carbon cycling from the ocean surface to the subseafloor on the Namibian shelf. There was a clear separation in microbial community structure across the seawater-seafloor boundary, which coincided with a 100-fold-increased concentration of microbial biomass and unique gene expression profiles of the benthic communities. 13C-labeled 16S rRNA genes in SIP experiments revealed carbon-assimilating taxa and their distribution across the sediment-water interface. Most of the transcriptionally active taxa among water column communities that assimilated 13C from diatom exopolysaccharides (mostly Bacteroidetes, Actinobacteria, Alphaproteobacteria, and Planctomycetes) also assimilated 13C-bicarbonate under anoxic conditions in sediment incubations. Moreover, many transcriptionally active taxa from the seafloor community (mostly sulfate-reducing Deltaproteobacteria and sulfide-oxidizing Gammaproteobacteria) that assimilated 13C-bicarbonate under sediment anoxic conditions also assimilated 13C from diatom exopolysaccharides in the surface ocean and OMZ waters. Despite strong selection at the sediment-water interface, many taxa related to either planktonic or benthic communities were found to be present at low abundance and actively assimilating carbon under both sediment and water column conditions. In austral winter, mixing of shelf waters reduces stratification and suspends sediments from the seafloor into the water column, potentially spreading metabolically versatile microbes across niches. IMPORTANCE Microbial activities in oxygen minimum zones (OMZs) transform inorganic fixed nitrogen into greenhouse gases, impacting the Earth's climate and nutrient equilibrium. Coastal OMZs are predicted to expand with global change and increase carbon sedimentation to the seafloor. However, the role of sulfur-cycling microbes in assimilating carbon in marine OMZs and related seabed habitats remain poorly understood. Using 13C DNA stable isotope probing and metatranscriptomics, we explore microbial guilds involved in sulfur and carbon cycling from ocean surface to subseafloor on the Namibian shelf. Despite strong selection and differential activities across the sediment-water interface, many active taxa were identified in both planktonic and benthic communities, either fixing inorganic carbon or assimilating organic carbon from algal biomass. Our data show that many planktonic and benthic microbes linked to the sulfur cycle can cross redox boundaries when mixing of the shelf waters reduces stratification and suspends seafloor sediment particles into the water column.


Assuntos
Bicarbonatos , Microbiota , Carbono/metabolismo , DNA , Isótopos , Nitrogênio/metabolismo , Oceanos e Mares , Oxigênio/metabolismo , RNA Ribossômico 16S , Água do Mar/microbiologia , Enxofre/metabolismo , Água/química
18.
Environ Pollut ; 305: 119286, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35439601

RESUMO

Airborne fine particles can affect climate change and human health; moreover, they can be transported over significant distances. However, studies on characteristics of individual particles and their morphology, elemental composition, aging processes, and spatial distribution after long-range transport over the Yellow Sea are limited. Therefore, in this study, we conducted shipborne measurements of fine particulate matter of less than 2.5 µm in diameter (PM2.5) over the Yellow Sea and classified the individual particles into seven types based on their morphology and composition. Overall, the percentage of organic-rich particles was the highest, followed by that of sea spray, sulfur-rich, dust, metals, fly ash, soot, and other particles. Near Shandong, China, the percentage of fly ash and sulfur-rich particles increased, while an increased percentage of only sulfur-rich particles was observed near the Korean Peninsula. In the open sea, the PM2.5 concentrations were the lowest, and sea spray particles predominated. During the cruises, three types (Types 1, 2, and 3) of events with substantially increased PM2.5 concentrations occurred, each with different dominant particles. Type 1 events frequently featured air masses from northern China and Mongolia with high wind speeds and increased dust particles. Type 2 events involved air masses from China with high wind speeds; fly ash, soot, organic-rich particles, and the sulfate percentage in PM2.5 increased. Type 3 events displayed stagnant conditions and local transport (from Korea); soot, dust particles, and the secondary sulfate and nitrate percentages in PM2.5 increased. Thus, different types of transport affected concentrations and dominant types of fine particles over the Yellow Sea during spring.


Assuntos
Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , China , Cinza de Carvão , Poeira/análise , Monitoramento Ambiental , Material Particulado/análise , Fuligem , Sulfatos , Enxofre
19.
Environ Pollut ; 305: 119322, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35447253

RESUMO

The fate of nitrogen is controlled by the competition between nitrate reduction pathways. Denitrification removes nitrogen in the system to the atmosphere, whereas dissimilatory nitrate reduction to ammonia (DNRA) retains nitrate in the form of ammonia. Different microbes specialize in the oxidation of different electron donors, thus electron donors might influence the outcomes of the competition. Here, we investigated the fate of nitrate with five forms of sulfur as electron donors. Chemoautotrophic nitrate reduction did not continue after the passages of the enrichments with sulfide, sulfite and pyrite. Nitrate reduction rate was the highest in the enrichment with thiosulfate. Denitrification was stimulated and no DNRA was observed with thiosulfate, while both denitrification and DNRA were stimulated with elemental sulfur. Metagenomes of the enrichments were assembled and binned into ten genomes. The enriched populations with thiosulfate included Thiobacillus, Lentimicrobium, Sulfurovum and Hydrogenophaga, all of which contained genes involved in sulfur oxidation. Elemental sulfur-based DNRA was performed by Thiobacillus (with NrfA and NirB) and Nocardioides (with only NirB). Our study established a link between sulfur sources, nitrate reduction pathways and microbial populations.


Assuntos
Compostos de Amônio , Nitratos , Amônia , Compostos de Amônio/metabolismo , Desnitrificação , Nitratos/metabolismo , Nitrogênio , Óxidos de Nitrogênio , Oxirredução , Enxofre , Tiossulfatos
20.
Bioresour Technol ; 354: 127194, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35452827

RESUMO

In this study, two short-cut sulfur autotrophic denitrification (SSADN) reactors were initiated using different reduced sulfur forms as electron donors and their effects on the start-up speed of the SSADN process, NO2--N accumulation characteristics, and microbial community were investigated. Results revealed that during the same period, due to the relatively slow S0 dissolution rate, the NO2--N production rate realized by microorganisms in S0-SSADN (NO2--N production rate (NPR), 174 mg/(L·d)) was significantly slower than S2--SSADN (NPR, 679 mg/(L·d)). The NO2--N accumulation efficiency (NAE) was maintained > 80%, which was significantly higher than S2--SSADN. In the SSADN system using different reduced sulfur forms, the microbial community structure and abundance considerably differed. The main sulfur-oxidizing bacteria (SOB) in S0-SSADN were Sulfurimonas (6.5%) and Thiobacillus (5.3%). The main SOB species in S2--SSADN was Thiomonas (13.6%). Thermomonas played an important role in the two reactors as an important NO3--N denitrifying bacteria species.


Assuntos
Reatores Biológicos , Desnitrificação , Processos Autotróficos , Bactérias , Elétrons , Nitratos , Nitrogênio/química , Dióxido de Nitrogênio , Enxofre/química
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