RESUMO
Soil constituents may play an important role in peroxydisulfate (PDS)-based oxidation of organic contaminants in soil. Iron-containing minerals (Fe-minerals) have been found to promote PDS activation for organics degradation. Our study found that ascorbic acid (H2A) could enhance PDS activation by soil Fe-minerals for triphenyl phosphate (TPHP) degradation. Determination and characterization analyses of Fe fractions showed that H2A could induce the reductive dissolution of solid Fe-minerals and the increasing of oxygen vacancies/hydroxyl groups content on Fe-minerals surface. The increasing of divalent Fe (Fe(II)) accelerated PDS activation to generate reactive oxygen species (ROS). Electron paramagnetic resonance (EPR) and quenching studies showed that sulfate radicals (SO4â¢-) and hydroxyl radicals (HOâ¢) contributed significantly to TPHP degradation. The composition and content of Fe-minerals and soil organic matter (SOM) markedly influenced ROS transformations. Surface-bond and structural Fe played the main role in the production of Fe(II) in reaction system. The high-concentration SOM could result in ROS consumption and degradation inhibition. Density functional theory (DFT) studies revealed that H2A is preferentially adsorbed at α-Fe2O3(012) surface through Fe-O-C bridges rather than hydrogen bonds. After absorption, H atoms on H2A may further be migrated to adjacent O atoms on the α-Fe2O3(012) surface. With the transformation of H atoms to the α-Fe2O3(012) surface, the Fe-O-C bridge is broken and one electron is transferred from the O to Fe atom, inducing the reduction of trivalent Fe (Fe(III)) atom. MS/MS2 analysis, HPLC analysis, and toxicity assessment demonstrated that TPHP was transformed to less toxic 4-hydroxyphenyl diphenyl phosphate (OH-TPHP), diphenyl hydrogen phosphate (DPHP), and phenyl phosphate (PHP) through phenol-cleavage and hydroxylation processes, and even be mineralized in reaction system.
Assuntos
Compostos de Bifenilo , Retardadores de Chama , Ferro , Ferro/química , Espécies Reativas de Oxigênio , Ácido Ascórbico , Espectrometria de Massas em Tandem , Compostos Organofosforados , Minerais , Oxirredução , Compostos Ferrosos , Solo , FosfatosRESUMO
Numerous application of pyrethroid insecticides has led to their accumulation in the environment, threatening ecological environment and human health. Its fate in the presence of iron-bearing minerals and natural organic matter under light irradiation is still unknown. We found that goethite (Gt) and humic acid (HA) could improve the photodegradation of bifenthrin (BF) in proper concentration under light irradiation. The interaction between Gt and HA may further enhance BF degradation. On one hand, the adsorption of HA on Gt may decrease the photocatalytic activity of HA through decreasing HA content in solution and sequestering the functional groups related with the production of reactive species. On the other hand, HA could improve the photocatalytic activity of Gt through extending light absorption, lowing of bandgap energy, hindering the recombination of photo-generated charges, and promoting the oxidation and reduction reaction on Gt surface. The increased oxygen vacancies on Gt surface along with the reduction of trivalent iron and the nucleophilic attack of hole to surface hydroxyl group contributed to the increasing photocatalytic activity of Gt. Electron paramagnetic resonance and quenching studies demonstrated that both oxidation species, such as hydroxyl radical (â¢OH) and singlet oxygen (1O2), and reducing species, such as hydrogen atoms (Hâ¢) and superoxide anion radical (O2â¢-), contributed to BF degradation in UV-Gt-HA system. Mass spectrometry, ion chromatography, and toxicity assessment indicated that less toxic C23H22ClF3O3 (OH-BF), C9H10ClF3O (TFP), C14H14O2 (OH-MBP), C14H12O2 (MBP acid), C14H12O3 (OH-MBP acid), and chloride ions were the main degradation products. The production of OH-BF, MPB, and TFP acid through oxidation and the production of MPB and TFP via reduction were the two primary pathways of BF degradation.
Assuntos
Substâncias Húmicas , Compostos de Ferro , Minerais , Oxirredução , Piretrinas , Substâncias Húmicas/análise , Minerais/química , Compostos de Ferro/química , Piretrinas/química , Fotólise , Inseticidas/químicaRESUMO
The phytohormone ethylene (ET) is a crucial signaling molecule that induces the biosynthesis of shikonin and its derivatives in Lithospermum erythrorhizon shoot cultures. However, the molecular mechanism and the positive regulators involved in this physiological process are largely unknown. In this study, the function of LeACS-1, a key gene encoding the 1-aminocyclopropane-1-carboxylic acid synthase for ET biosynthesis in L. erythrorhizon hairy roots, was characterized by using overexpression and RNA interference (RNAi) strategies. The results showed that overexpression of LeACS-1 significantly increased endogenous ET concentration and shikonin production, consistent with the up-regulated genes involved in ET biosynthesis and transduction, as well as the genes related to shikonin biosynthesis. Conversely, RNAi of LeACS-1 effectively decreased endogenous ET concentration and shikonin production and down-regulated the expression level of above genes. Correlation analysis showed a significant positive linear relationship between ET concentration and shikonin production. All these results suggest that LeACS-1 acts as a positive regulator of ethylene-induced shikonin biosynthesis in L. erythrorhizon hairy roots. Our work not only gives new insights into the understanding of the relationship between ET and shikonin biosynthesis, but also provides an efficient genetic engineering target gene for secondary metabolite production in non-model plant L. erythrorhizon.
Assuntos
Etilenos/farmacologia , Regulação da Expressão Gênica de Plantas/fisiologia , Lithospermum/metabolismo , Liases/metabolismo , Naftoquinonas/metabolismo , Raízes de Plantas/metabolismo , Clonagem Molecular , Biologia Computacional , DNA Complementar/genética , DNA Complementar/metabolismo , Liases/genética , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Raízes de Plantas/efeitos dos fármacos , Plantas Geneticamente Modificadas , Transdução de Sinais/fisiologiaRESUMO
Energy recovery from low-strength wastewater through anaerobic methanogenesis is constrained by limited substrate availability. The development of efficient methanogenic communities is critical but challenging. Here we develop a strategy to acclimate methanogenic communities using conductive carrier (CC), electrical stress (ES), and Acid Orange 7 (AO7) in a modified biofilter. The synergistic integration of CC, ES, and AO7 precipitated a remarkable 72-fold surge in methane production rate compared to the baseline. This increase was attributed to an altered methanogenic community function, independent of the continuous presence of AO7 and ES. AO7 acted as an external electron acceptor, accelerating acetogenesis from fermentation intermediates, restructuring the bacterial community, and enriching electroactive bacteria (EAB). Meanwhile, CC and ES orchestrated the assembly of the archaeal community and promoted electrotrophic methanogens, enhancing acetotrophic methanogenesis electron flow via a mechanism distinct from direct electrochemical interactions. The collective application of CC, ES, and AO7 effectively mitigated electron flow impediments in low-strength wastewater methanogenesis, achieving an additional 34% electron recovery from the substrate. This study proposes a new method of amending anaerobic digestion systems with conductive materials to advance wastewater treatment, sustainability, and energy self-sufficiency.
RESUMO
Heterotrophic nitrification-aerobic denitrification (HN-AD) process was achieved in a moving bed biofilm reactor after 180-days acclimation using PCL as carbon source for low C/N wastewater treatment. A novel HN-AD strain, JQ-H3, with ability of PCL degradation was augmented to improve nitrogen removal. TN removal efficiencies of 82.31%, 90.05%, and 93.16% were achieved in the augmented reactor (R2), at different HRTs of 24 h, 20 h, and 16 h, while in the control reactor (R1), the TN removal efficiencies were 59.24%, 74.61%, and 76.68%. The effluent COD in R2 was 10.17 mg/L, much lower than that of 42.45 mg/L in R1. Microbial community analysis revealed that JQ-H3 has successfully proliferated with a relative abundance of 4.79%. Relative abundances of functional enzymes of nitrogen cycling remarkably increased due to bioaugmentation based on the analysis of PICRUSt2. This study provides a new approach for enhancing nitrogen removal in low C/N sewage treatment via the HN-AD process.
Assuntos
Desnitrificação , Águas Residuárias , Pseudomonas , Nitrogênio/análise , Carbono , Reatores Biológicos , Nitrificação , Biofilmes , AceleraçãoRESUMO
Persistent heavy metal (HM) contaminated soil provides special habitat for microorganisms, HM stress and complex abiotic factors bring great uncertainty for the development of bacteria and eukaryotic microbes. Despite numerous studies about HMs' effect on soil microorganisms, the key factors affecting microbial communities in severe HM contaminated soil and their interactions are still not definite. In this study, the effect of HM fractions and soil properties on the interaction between bacterial communities and eukaryotic microorganisms was studied by high-throughput Illumina sequencing and simplified continuous extraction of HM in severe HM contaminated soil. Based on amplification and sequencing of the 18S rRNA gene, this study revealed that protists and algae were the most predominant eukaryotic microorganisms, and the dominant phyla were SAR, Opisthokonta and Archaeplastida in HM seriously polluted soil. These results also showed that exchangeable As was negatively correlated with bacterial Shannon and Simpson indexes, while exchangeable Zn was positively correlated with Shannon and Simpson indexes of eukaryotic microbes. Moreover, the structural equation model illustrated that pH, moisture content, available potassium and phosphorus, and exchangeable Cd, As and Zn were the dominant factors shaping bacterial communities, while total organic carbon and exchangeable Zn made the predominant contributions to variations in eukaryotic microbes. In addition, eukaryotic microbes were intensely affected by the bacterial communities, with a standardized regression weight of 0.53, which exceeded the influence of other abiotic factors. It was suggested that community-level adaptions through cooperative interactions under serious HM stress in soil.
Assuntos
Metais Pesados , Microbiota , Poluentes do Solo , Bactérias/genética , Carvão Mineral , Eucariotos , Metais Pesados/análise , Centrais Elétricas , Solo/química , Microbiologia do Solo , Poluentes do Solo/análiseRESUMO
Silicon suboxide (SiO x ) is one of the most promising anodes for the next-generation high-power lithium-ion batteries because of its higher lithium storage capacity than current commercial graphite, relatively smaller volume variations than pure silicon, and appropriate working potential. However, the high cost, poor cycling stability, and rate capability hampered its industrial applications due to its complex production process, volume changes during Li+ insertion/extraction, and low conductivity. Herein, a low-cost and high-capacity SiO x /C@graphite (SCG) hybrid was designed and synthesized by a facile one-pot carbonization/hydrogen reduction process of the rice husk and graphite. As an advanced anode for lithium-ion batteries, the SiO x /C@graphite hybrid delivers a high reversible capacity with significantly enhanced cycling stability (842 mAh g-1 after 300 cycles at 0.5 A g-1) and rate capability (562 mAh g-1 after 300 cycles at 1 A g-1). The great improvement in performances could be attributed to the positive synergistic effect of SiO x nanoparticles as lithium storage active materials, the in situ-formed carbon matrix network derived from biomass functioning as an efficient three-dimensional conductive network and spacer to improve the rate capability and buffer the volume changes, and graphite as a conductor to further improve the rate capabilities and cycling stability by increasing the conductivity. The low-cost and high-capacity SCG derived from rice husk synthesized by a facile, scalable synthetic method turns out to be a promising anode for the next-generation high-power lithium-ion batteries.
RESUMO
Porous multicomponent Mn-Sn-Co oxide microspheres (MnSnO3-MC400 and MnSnO3-MC500) have been fabricated using CoSn(OH)6 nanocubes as templates via controlling pyrolysis of a CoSn(OH)6/Mn0.5Co0.5CO3 precursor at different temperatures in N2. During the pyrolysis process of CoSn(OH)6/Mn0.5Co0.5CO3 from 400 to 500 °C, the part of (Co,Mn)(Co,Mn)2O4 converts into MnCo2O4 accompanied with structural transformation. The MnSnO3-MC400 and MnSnO3-MC500 microspheres as secondary nanomaterials consist of MnSnO3, MnCo2O4, and (Co,Mn)(Co,Mn)2O4. Benefiting from the advantages of multicomponent synergy and porous secondary nanomaterials, the MnSnO3-MC400 and MnSnO3-MC500 microspheres as anodes exhibit the specific capacities of 1030 and 750 mA h g-1 until 1000 cycles at 1 A g-1 without an obvious capacity decay, respectively.
RESUMO
A new non-enzyme method based on hybridization chain reaction (HCR) and colorimetric reaction catalyzed by magnetic Ni/Fe layered double hydroxide (LDH) nanosheets was developed for detection of microRNA (miRNA), let-7b. The DNA hairpins from HCR were separated and adsorbed by Ni/Fe LDH. The peroxidase-like activity of Ni/Fe LDH was found to be enhanced by the DNA hairpins on the surface. The factors, such as ratio of Ni/Fe and concentration of DNA hairpins, related to the catalytic activity were evaluated and the mechanism was discussed. The results of this new detection method for let-7b provided low limit of detection (0.36â¯fM), wide linear range (0.01â¯pM to 200â¯pM) with good linearity (r2 =â¯0.9968). The optimized method was applied to analyze let-7b in real samples, lung cancer cells. This work demonstrated a new and cost-effective approach for efficient detection of miRNA.
Assuntos
DNA/química , Hidróxidos/química , Ferro/química , Neoplasias Pulmonares/química , MicroRNAs/análise , Nanoestruturas/química , Níquel/química , Catálise , Colorimetria , Humanos , Limite de Detecção , Neoplasias Pulmonares/patologia , Fenômenos Magnéticos , Hibridização de Ácido Nucleico , Tamanho da PartículaRESUMO
Glyphosate is a non-selective organophosphate herbicide that is widely used in agriculture, but its effects on soil microbial communities are highly variable and often contradictory, especially for high dose applications. We applied glyphosate at two rates: the recommended rate of 50 mg active ingredient kg-1 soil and 10-fold this rate to simulate multiple glyphosate applications during a growing season. After 6 months, we investigated the effects on the composition of soil microbial community, the catabolic activity and the genetic diversity of the bacterial community using phospholipid fatty acids (PLFAs), community level catabolic profiles (CLCPs), and 16S rRNA denaturing gradient gel electrophoresis (DGGE). Microbial biomass carbon (Cmic) was reduced by 45%, and the numbers of the cultivable bacteria and fungi were decreased by 84 and 63%, respectively, under the higher glyphosate application rate. According to the PLFA analysis, the fungal biomass was reduced by 29% under both application rates. However, the CLCPs showed that the catabolic activity of the gram-negative (G-) bacterial community was significantly increased under the high glyphosate application rate. Furthermore, the DGGE analysis indicated that the bacterial community in the soil that had received the high glyphosate application rate was dominated by G- bacteria. Real-time PCR results suggested that copies of the glyphosate tolerance gene (EPSPS) increased significantly in the treatment with the high glyphosate application rate. Our results indicated that fungi were impaired through glyphosate while G- bacteria played an important role in the tolerance of microbiota to glyphosate applications.
Assuntos
Bactérias/efeitos dos fármacos , Glicina/análogos & derivados , Bactérias Gram-Negativas/efeitos dos fármacos , Herbicidas/farmacologia , Micobioma/efeitos dos fármacos , Organofosfatos/farmacologia , Microbiologia do Solo , Agricultura , Bactérias/metabolismo , Biomassa , Carbono/metabolismo , Ácidos Graxos/análise , Glicina/farmacologia , Bactérias Gram-Negativas/genética , Fosfolipídeos/metabolismo , RNA Ribossômico 16S/genética , Solo/química , Poluentes do Solo/farmacologia , GlifosatoRESUMO
The response mechanism of aerobic granular sludge (AGS) systems to salt stress in high-salinity wastewater treatment processes has not been fully elucidated in current studies. The aim of this study was to reveal the comprehensive effects of salinity on AGS characteristics using microbial community and metaproteomics analyses. The results showed that the removal efficiency of COD, TN and TP decreased significantly with increasing salinity. Under salt stress, the Na+ content in AGS decreased, while the K+ and Ca2+ contents increased. This was because the salt-tolerant mechanism of the microorganisms was dependent on the uptake of K+ and ejection of Na+via K+/Na+ pumps, Na+/H+ reversed transport proteins, and K+ channels. Compared with the salt-free condition, 14 of 25 different protein spots were identified successfully by metaproteomic analysis, including porin, periplasmic-binding protein, and ATP-binding cassette-type for phosphonate transporter, which were expressed mainly by members of γ-Proteobacteria and α-Proteobacteria. The variations in functional proteins and microbial community revealed that α- and γ-Proteobacteria had disproportionally active and the metabolic activity of ß-Proteobacteria was inhibited by increasing salinity. Additionally, Psychrobacter sp. was confirmed to be a predominant bacterium at 15 g/L NaCl, as the porin was strongly expressed.