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Presented herein is an atom- and step-economical method enabling the precise assembly of a heptacyclic scaffold containing both azocine and indoline units through the cascade reactions of indolin-1-yl(aryl)methanimines with diazo indanediones. The formation of products involves C-H bond activation and double carbene insertion followed by intramolecular condensation, retro-[2 + 2] cycloaddition, and recyclization. This cascade reaction not only provided a concise and straightforward strategy for the synthesis of the otherwise difficult to obtain heptacyclic compounds from readily available substrates but also disclosed an unprecedented reaction mode for indoline derivatives and diazo compounds. In general, this novel synthetic protocol has advantages, such as easily obtainable substrates, structurally sophisticated products, concise synthetic procedure, good compatibility with diverse functional groups, and ready scalability. Moreover, the products thus obtained showed decent antiproliferative activity against three human cancer cell lines.
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Introduction Heart Failure (HF) may induce bowel hypoperfusion, leading to hypoxia of the villa of the bowel wall and the occurrence of Clostridioides difficile infection (CDI). However, the risk factors for the development of CDI in HF patients have yet to be fully illustrated, especially because of a lack of evidence from real-world data. METHODS: Clinical data and survival situations of HF patients with CDI admitted to ICU were extracted from the Medical Information Mart for Intensive Care (MIMIC)-IV database. For developing a model that can predict 28-day all-cause mortality in HF patients with CDI, the Recursive Feature Elimination with Cross-Validation (RFE-CV) method was used for feature selection. And nine machine learning (ML) algorithms, including logistic regression (LR), decision tree (DT), bayesian, adaptive boosting (AdaBoost), random forest (RF), gradient boosting decision tree (GBDT), XGBoost, light gradient boosting machine (LightGBM), and categorical boosting (CatBoost) were applied for model construction. After training and hyperparameter optimization of the models through grid search 5-fold cross-validation, the performance of models was evaluated by the area under curve (AUC), accuracy, sensitivity, specificity, precision, negative predictive value, and F1 score. Furthermore, the SHapley Additive exPlanations (SHAP) method was used to interpret the optimal model. RESULTS: A total of 526 HF patients with CDI were included in the study, of whom 99 cases (18.8%) experienced death within 28 days. 18 of the 57 variables were selected for the model construction algorithm for model construction. Among the ML models considered, the RF model emerged as the optimal model achieving the accuracy, F1-score, and AUC values of 0.821, 0.596, and 0.864 respectively. The net benefit of the model surpassed other models at 16%~22% threshold probabilities based on decision curve analysis. According to the importance of features in the RF model, red blood cell distribution width, blood urea nitrogen, Simplified Acute Physiology Score II, Sequential Organ Failure Assessment, and white blood cell count were highlighted as the five most influential variables. CONCLUSIONS: We developed ML models to predict 28-day all-cause mortality in HF patients associated with CDI in the ICU, which are more effective than the conventional logistic regression model. The RF model has the best performance among all the ML models employed. It may be useful to help clinicians identify high-risk HF patients with CDI.
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The study embarked on a comprehensive examination of the evolution and diversity of microorganisms within long-term leachate pollution environments, with a focus on varying depths and levels of contamination, and its linkage to soil characteristics and the presence of heavy metals. It was observed that microbial diversity presented distinct cross-depth trend, where archaeal communities were found to be particularly sensitive to alterations in soil depth. Noteworthily, Euryarchaeota increased by 4.82 %, 7.64 % and 9.87 % compared with topsoil. The abundance of Tahumarchaeota was successively reduced by 5.79 %, 9.58 %, and 12.66 %. The bacterial community became more sensitive to leachate pollution, and the abundance of Protebacteria in contaminated soil decreased by 10.27 %, while the abundance of Firmicutes increased by 7.46 %. The bacterial genus Gemmobacter, Chitinophaga and Rheinheimera; the archaeal genus Methanomassiliicoccus and Nitrosopumilus; along with the fungal genus Goffeauzyma, Gibberella, and Setophaeosphaeria emerged as pivotal biological markers for their respective domains, underpinning the biogeochemical dynamics of these environments. Furthermore, the study highlighted that geochemical factors, specifically nitrate (NO3--N) levels and humic acid (HA) fractions, played crucial roles in modulating the composition and metabolic potential of these communities. Predictive analyses of functional potentials suggested that the N functional change of archaea was more pronounced, with anaerobic ammonia oxidation and nitrification decreased by 15.78 % and 14.62 %, respectively. Overall, soil characteristics alone explained 57.9 % of the total variation in the bacterial community structure. For fungal communities within contaminated soil, HMs were the primary contributors, explaining 46.9 % of the variability, while soil depth accounting for 6.4 % of the archaeal variation. This research enriches the understanding of the complex interrelations between heavy metal pollution, soil attributes, and microbial communities, paving the way for informed strategies in managing informal landfill sites effectively.
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Archaea , Microbiota , Microbiología del Suelo , Contaminantes del Suelo , Instalaciones de Eliminación de Residuos , Contaminantes del Suelo/análisis , Microbiota/efectos de los fármacos , Bacterias/clasificación , Suelo/química , Monitoreo del Ambiente , Metales Pesados/análisis , Hongos , Contaminantes Químicos del Agua/análisis , ChinaRESUMEN
Presented herein is a novel synthesis of indenone-fused pyran derivatives via the cascade reactions of aryl enaminones with cyclopropenones. The formation of products involves a one-pot cascade procedure consisting of aryl C-H bond and enamine C-H bond functionalization along with C-C bond cleavage of cyclopropenone and 1,3-rearrangement of the in situ-formed allylic alcohol moiety followed by intramolecular O-nucleophilic addition and Me2NH elimination. To our knowledge, this is the first synthesis of indenone-fused pyran derivatives via simultaneous formation of both indenone and pyran scaffolds through concurrent unsymmetrical relay C-H bond activation and double C-C/C-O bond formation. Moreover, the usefulness of this method is further showcased by its suitability for large-scale synthetic scenarios and diverse transformations of products.
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The impairment of the immune system by fluoride is a public health concern worldwide, yet the underlying mechanism is unclear. Both riboflavin and IL-17A are closely related to immune function and regulate the testicular toxicity of fluoride. However, whether riboflavin or IL-17A is involved in fluoride-induced immunotoxicity is unknown. Here, we first established a male ICR mouse model by treating mice with sodium fluoride (NaF) (100 mg/L) via the drinking water for 91 days. The results showed that fluoride increased the expression of the proinflammatory factors IL-1ß and IL-17A, which led to splenic inflammation and morphological injury. Moreover, the expression levels of the riboflavin transporters SLC52A2 and SLC52A3; the transformation-related enzymes RFK and FLAD1; and the key mitochondrial functional determinants SDH, COX, and ATP in the spleen were measured via real-time PCR, Western blotting, and ELISA. The results revealed that fluoride disrupted riboflavin transport, transformation, metabolism, and mitochondrial function. Furthermore, wild-type (WT) and IL-17A knockout (IL-17A-/-) C57BL/6 J male mice of the same age were treated with NaF (24 mg/kg·bw, equivalent to 100 mg/L) and/or riboflavin sodium phosphate (5 mg/kg·bw) via gavage for 91 days. Similar parameters were evaluated as above. The results confirmed that fluoride increased riboflavin metabolism through RFK but not through FLAD1. Fluoride also affected mitochondrial function and activated neutrophils (marked with Ly6g) and macrophages (marked with CD68) in the spleen. Interestingly, IL-17A partly mediated fluoride-induced riboflavin metabolism disorder and immunotoxicity in the spleen. This work not only reveals a novel toxic mechanism for fluoride but also provides new clues for exploring the physiological function of riboflavin and for diagnosing and treating the toxic effects of fluoride in the environment.
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Interleucina-17 , Ratones Endogámicos C57BL , Ratones Endogámicos ICR , Riboflavina , Fluoruro de Sodio , Bazo , Animales , Masculino , Interleucina-17/metabolismo , Bazo/efectos de los fármacos , Bazo/metabolismo , Fluoruro de Sodio/toxicidad , Ratones Noqueados , Ratones , Mitocondrias/efectos de los fármacos , Mitocondrias/metabolismo , Transporte BiológicoRESUMEN
Presented herein are novel syntheses of CF3-isoquinolinones and imidazole fused CF3-isoquinolinones based on the cascade reactions of 2-aryloxazolines with trifluoromethyl imidoyl sulfoxonium ylides. The formation of CF3-isoquinolinone involves an intriguing cascade process including oxazolinyl group-assisted aryl alkylation through C(sp2)-H bond metalation, carbene formation, migratory insertion, and proto-demetalation followed by intramolecular condensation and water-promoted oxazolinyl ring-scission. With this method, the isoquinolinone scaffold tethered with valuable functional groups was effectively constructed. By taking advantage of the functional groups embedded therein, the products thus obtained could be readily transformed into imidazole-fused CF3-isoquinolinones or coupled with some clinical drugs to furnish hybrid compounds with potential applications in drug development. In general, the developed protocols feature expeditious and convenient formation of valuable CF3-heterocyclic skeletons, broad substrate scope, and ready scalability. In addition, studies on the activity of selected products against some human cancer cell lines demonstrated their potential as lead compounds for the development of novel anticancer drugs.
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Chelator-assisted phytoremediation is an efficacious method for promoting the removal efficiency of heavy metals (HMs). The effects of N, N-bis(carboxymethyl)-L-glutamic acid (GLDA) and polyaspartic acid (PASP) on Cd uptake and pyrene removal by Solanum nigrum L. (S. nigrum) were compared in this study. Using GLDA or PASP, the removal efficiency of pyrene was over 98%. And PASP observably raised the accumulation and transport of Cd by S. nigrum compared with GLDA. Meanwhile, both GLDA and PASP markedly increased soil dehydrogenase activities (DHA) and microbial activities. DHA and microbial activities in the PASP treatment group were 1.05 and 1.06 folds of those in the GLDA treatment group, respectively. Transcriptome analysis revealed that 1206 and 1684 differentially expressed genes (DEGs) were recognized in the GLDA treatment group and PASP treatment group, respectively. Most of the DEGs found in the PASP treatment group were involved in the metabolism of carbohydrates, the biosynthesis of brassinosteroid and flavonoid, and they were up-regulated. The DEGs related to Cd transport were screened, and ABCG3, ABCC4, ABCG9 and Nramp5 were found to be relevant with the reduction of Cd stress in S. nigrum by PASP. Furthermore, with PASP treated, transcription factors (TFs) related to HMs such as WRKY, bHLH, AP2/ERF, MYB were down-regulated, while more MYB and bZIP TFs were up-regulated. These TFs associated with plant stress resistance would work together to induce oxidative stress. The above results indicated that PASP was more conducive for phytoremediation of Cd-pyrene co-contaminated soil than GLDA.
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Biodegradación Ambiental , Cadmio , Pirenos , Contaminantes del Suelo , Cadmio/metabolismo , Contaminantes del Suelo/metabolismo , Pirenos/metabolismo , Suelo/química , Péptidos/metabolismo , Perfilación de la Expresión Génica , Ácido Glutámico/metabolismoRESUMEN
Pichia pastoris, a methylotrophic yeast, can utilize methanol as a carbon source and energy source to synthesize high-value chemicals, and is an ideal host for biomanufacturing. Constructing the P. pastoris cell factory is somewhat impeded due to the absence of genetic tools for manipulating multi-gene biosynthetic pathways. To broaden its application in the field of metabolic engineering, this study identified and screened 15 novel integration sites in P. pastoris using CRISPR-Cpf1 genome editing technology, with EGFP serving the reporter protein. These integration sites have integration efficiencies of 10-100 % and varying expression strengths, which allow for selection based on the expression levels of genes as needed. Additionally, these integrated sites are applied in the heterologous biosynthesis of P. pastoris, such as the astaxanthin biosynthetic pathway and the carbon dioxide fixation pathway of the Calvin-Benson-Bassham (CBB) cycle. During the three-site integration process, the 8 genes of the CBB cycle were integrated into the genome of P. pastoris. This indicates the potential of these integration sites for integrating large fragments and suggests their successful application in metabolic engineering of P. pastoris. This may lead to improved efficiency of genetic engineering in P. pastoris.
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The storage ring of the high energy photon source will be driven by five 166.6 MHz ß = 1 quarter-wave superconducting cavities operating at 4 K. A higher-order-mode-damped superconducting cavity was designed with excellent rf and mechanical properties based on the successful development of the proof-of-principle cavity. The mechanical design of the dressed cavity was focused on addressing stress safety throughout the processes, tunability, frequency detuning due to pressure fluctuation, and Lorentz force, among other factors. A new liquid helium vessel was designed along with a comprehensive stiffening scheme to mitigate the surging peak stress on the cavity resulting from the significantly unequal beam pipe size. In the first batch, three cavities were manufactured, and surface preparations were carefully conducted to eliminate defects and etching traces while ensuring cleanliness. The cavity's Q0 at the design voltage of 1.5 MV reached 3.8 × 109 at 4 K, comfortably surpassing the design goal. Field emission onset was not observed during the entire test up to a peak electric field of 60 MV/m, thanks to the optimized processing procedures. Subsequently, one cavity was welded with the newly designed helium vessel and vertically tested at 2 K, achieving an rf performance comparable to the bare cavities, demonstrating the success of the jacketed cavity. This paper presents the design, fabrication, surface preparation, and cryogenic tests of the first higher-order-mode-damped 166.6 MHz ß = 1 superconducting cavity.
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What is already known about this topic?: Given the common modes of transmission, outbreaks of both human immunodeficiency virus (HIV) and syphilis are primarily observed in men who have sex with men (MSM). However, minimal research has been conducted to concurrently evaluate the rates and trends of HIV and syphilis incidence within this community in China. What is added by this report?: This manuscript presents the incidence rates and associated factors of HIV and syphilis in MSM in Tianjin based on data derived from a decade-long cohort study. Intriguingly, it depicts a decreasing trend in HIV incidence juxtaposed with an increasing incidence of syphilis among this population in Tianjin. What are the implications for public health practice?: The interconnected risk factors for HIV and syphilis pose significant hindrances to disease control. Our study underscores the urgent need for improved intervention strategies specifically aimed at MSM to mitigate the propagation of both infections.
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Callosobruchus maculatus is one of the most competitive stored grain pests, which causes a great loss to agricultural economy. However, due to an inadequacy of high-quality reference genome, the molecular mechanisms for olfactory and hypoxic adaptations to stored environments are unknown and require to be revealed urgently, which will contribute to the detection and prevention of the invasive pests C. maculatus. Here, we presented a high-quality chromosome-level genome of C. maculatus based on Illumina, Nanopore and Hi-C sequencing data. The total size was 1.2 Gb, and 65.17% (797.47 Mb) of it was identified to be repeat sequences. Among assembled chromosomes, chromosome 10 was considered the X chromosome according to the evidence of reads coverage and homologous genes among species. The current version of high-quality genome provides preferable data resources for the adaptive evolution research of C. maculatus.
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Escarabajos , Genoma de los Insectos , Animales , Escarabajos/genéticaRESUMEN
In this study, we examined the aging characteristics of polyethylene (PE) and polylactic acid (PLA) microplastics (MPs), examining the adsorption behaviors and mechanisms concerning Cd(II) and Cr(VI) under both single and binary systems. The results revealed that aging treatment changed the physicochemical properties of MPs. The aging mechanisms of PLA and PE MPs were shown to be similar by the 2D-FTIR-COS study. These mechanisms involve the formation of oxygen-containing functional groups through the combination of carbon chain breakdown and oxygen. Aged MPs had a greater ability to adsorb metal ions than pristine MPs, with PLA MPs outperforming PE MPs. After 30 days of aging, Cd(II) adsorption increased by 40.61 % and 25.49 % for PE and PLA MPs, respectively, while Cr(VI) adsorption increased by 37.50 % and 69.29 %, respectively. The adsorption ability of PE and PLA MPs with Cd(II) or Cr(VI) under binary systems was less than that under single systems, with Cd(II) exhibiting more adsorption competitiveness than Cr(VI). Humic acid (HA), ionic species and strength, solution pH, and adsorption of Cd(II) and Cr(VI) were found to be significantly correlated. Further investigation into the adsorption mechanisms of Cd(II) and Cr(VI) on PE and PLA MPs revealed that pore-filling, electrostatic interactions, complexation, and hydrogen bonding play important roles in the adsorption process. The study's conclusions are crucial for assessing the risk associated with concurrent contamination by metal ions and microplastics.
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Cadmio , Cromo , Microplásticos , Poliésteres , Polietileno , Contaminantes Químicos del Agua , Poliésteres/química , Adsorción , Cadmio/química , Polietileno/química , Contaminantes Químicos del Agua/química , Microplásticos/química , Cromo/química , Sustancias HúmicasRESUMEN
Leaf inclination angle (LIA) and tillering impact the winter wheat (Triticum aestivum L.) population canopy structure. Understanding their effects on water use (WU) parameters and yield can guide water-saving strategies through population control. In this study, six near-isogenic lines (NILs) and their parents were selected as materials. These special materials were characterized by varying tillering at the current sowing density, a similar genetic background, and, particularly, a gradient in mean flag leaf LIA. The investigation focused on the jointing to early grain-filling stage, the peak water requirement period of wheat crops. Population-scale transpiration (PT) and evaporation from the soil surface (E) were partitioned from total evapotranspiration (ET) by the means of micro-lysimeters. The results showed decreased PT, E, and ET with increased population density (PD) within a narrow density range derived from varying tillering across genotypes. Significant correlations existed between PD and ET, E, and PT, especially in the wettest 2017-2018 growing season. Within such narrow PD range, all the correlations between WU parameters and PD were negative, although some correlations were not statistically significant, thereby suggesting the population structure's predominant impact. No significant correlation existed between LIA and both ET and PT within the LIA range of 35°-65°. However, significant correlations occurred between LIA and E in two growing seasons. Genotypes with similar LIA but different PD produced varied ET; while with similar PD, the four pairs of genotypes with different LIA each consumed similar ET, thus highlighting PD's more crucial role in regulating ET. The yield increased with higher LIA, and showed a significant correlation, emphasizing the LIA's significant effect on yield. However, no correlation was observed with PD, indicating the minor effect of tillering at the current sowing density. Therefore these results might offer valuable insights for breeding water-saving cultivars and optimizing population structures for effective field water conservation.
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Hojas de la Planta , Transpiración de Plantas , Suelo , Triticum , Triticum/genética , Triticum/fisiología , Triticum/crecimiento & desarrollo , Hojas de la Planta/fisiología , Suelo/química , Estaciones del Año , Agua/metabolismo , GenotipoRESUMEN
BACKGROUND: Recent studies indicate that both prefrontal and visual regions play critical roles in visual working memory (VWM), with prefrontal regions mainly associated with executive functions, and visual cortices linked to representations of memory contents. VWM involves the selective filtering of irrelevant information, yet the specific contributions of the prefrontal regions and visual cortex in this process remain unclear. OBJECTIVE: To understand the dynamic causal roles of prefrontal and visual regions in VWM. METHODS: The differentiation of VWM components was achieved using a computational model that incorporated a swap rate for non-target stimuli. Single-pulse magnetic transcranial stimulation (spTMS) was delivered to the early visual cortex (EVC) and the inferior frontal junction (IFJ) across different phases of an orientation recall task that with or without distractors. RESULTS: Our results indicate that spTMS over the EVC and IFJ influences VWM particularly when distractors are present. VWM precision can be impacted by spTMS applied to either region during the early retention, while spTMS effect is especially prominent when EVC is stimulated during the late retention phase and when directed at the ipsilateral EVC. Conversely, the probability of accurately recalling the target exhibited comparable patterns when spTMS was administered to either the EVC or IFJ. CONCLUSIONS: We highlight the "sensory recruitment" of VWM characterized by critical involvement of EVC particularly in the information-filtering process within VWM. The maintenance of memory content representations necessitates ongoing communication between the EVC and IFJ throughout the entirety of the VWM process in a dynamic pattern.
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Memoria a Corto Plazo , Estimulación Magnética Transcraneal , Corteza Visual , Percepción Visual , Humanos , Memoria a Corto Plazo/fisiología , Estimulación Magnética Transcraneal/métodos , Corteza Visual/fisiología , Percepción Visual/fisiología , Masculino , Adulto , Femenino , Corteza Prefrontal/fisiología , Recuerdo Mental/fisiología , Adulto JovenRESUMEN
Presented herein is the synthesis of diversely functionalized pyrrolizines from the reaction of N-alkoxycarbamoyl pyrroles with CF3-ynones. The formation of the product is based on a C-H bond activation-initiated cascade process including N-alkoxycarbamoyl group-directed alkenylation of the pyrrole scaffold followed by simultaneous intramolecular nucleophilic addition along with cleavage and transfer of the directing group. By taking advantage of the rich chemistry of the transferred alkoxycarbamoyl moiety, the products could be transformed into a series of structurally and biologically interesting pyrrolizine derivatives. To our knowledge, this is the first example in which the N-alkoxycarbamoyl unit acted as a transferable and transformable directing group for the divergent synthesis of pyrrolizines.
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Escherichia coli (E. coli) can induce severe clinical bovine mastitis, which is to blame for large losses experienced by dairy farms. Macrophage polarization into various states is in response to pathogen infections. Lycopene, a naturally occurring hydrocarbon carotenoid, relieved inflammation by controlling M1/M2 status of macrophages. Thus, we wanted to explore the effect of lycopene on polarization states of macrophages in E. coli-induced mastitis. Macrophages were cultivated with lycopene for 24, before E. coli inoculation for 6 h. Lycopene (0.5 µmol/L) significantly enhanced cell viabilities and significantly reduced lactic dehydrogenase (LDH) levels in macrophages, whereas 2 and 3 µmol/L lycopene significantly enhanced LDH activities. Lycopene treatment significantly reduced the increase in LDH release, iNOS, CD86, TNF-α, IL-1ß and phosphatase and tensin homolog (PTEN) expressions in E. coli group. 0.5 µmol/L lycopene significantly increased E. coli-induced downregulation of CD206, arginase I (ARG1), indoleamine 2,3-dioxygenase (IDO), chitinase 3-like 3 (YM1), PI3K, AKT, p-AKT, mammalian target of rapamycin (mTOR), p-mTOR, jumonji domain-containing protein-3 (JMJD3) and interferon regulatory factor 4 (IRF4) levels. Moreover, Ginkgolic acid C17:1 (a specific PTEN inhibitor), 740YPDGFR (a specific PI3K activator), SC79 (a specific AKT activator) or CHPG sodium salt (a specific NF-κB activator) significantly decreased CD206, AGR1, IDO and YM1 expressions in lycopene and E. coli-treated macrophages. Therefore, lycopene increased M2 macrophages via inhibiting NOTCH1-PI3K-mTOR-NF-κB-JMJD3-IRF4 pathway in response to E. coli infection in macrophages. These results contribute to revealing the pathogenesis of E. coli-caused bovine mastitis, providing the new angle of the prevention and management of mastitis.
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Infecciones por Escherichia coli , Escherichia coli , Licopeno , Macrófagos , Transducción de Señal , Animales , Bovinos , Femenino , Ratones , Línea Celular , Infecciones por Escherichia coli/microbiología , Infecciones por Escherichia coli/inmunología , Factores Reguladores del Interferón/metabolismo , Factores Reguladores del Interferón/genética , Licopeno/farmacología , Macrófagos/efectos de los fármacos , Macrófagos/microbiología , Macrófagos/inmunología , Macrófagos/metabolismo , Mastitis Bovina/microbiología , FN-kappa B/metabolismo , Fosfatidilinositol 3-Quinasas/metabolismo , Fosfatidilinositol 3-Quinasas/genética , Receptor Notch1/metabolismo , Receptor Notch1/genética , Transducción de Señal/efectos de los fármacos , Serina-Treonina Quinasas TOR/metabolismoRESUMEN
The environmental burden due to industrial activities has been quite observable in the last few years, with heavy metals (HMs) like lead, cadmium, and arsenic inducing serious perturbations to the microbial ecosystem of groundwater. Studies carried out in North China, a region known for interconnection of industrial and groundwater systems, sought to explore the natural mechanisms of adaptation of microbes to groundwater contamination. The results showed that heavy metals permeate from surface increased the diversity and abundance of microbial communities in groundwater, producing an average decrease of 40.84% and 34.62% in the relative abundance of Bacteroidetes and Proteobacteria in groundwater, respectively. Meanwhile, the key environmental factors driving the evolution of microbial communities shift from groundwater nutrients to heavy metals, which explained 50.80% of the change in the microbial community composition. Microbial indicators are more sensitive to HMs pollution and could accurately identify industrial area where HMs permeation occurred and other extraneous pollutants. The phylum Bacteroidetes could act as appropriate indicators for the identification. Significant genera that were identified, being Mesorhizobium, Clostridium, Bacillus and Mucilaginibacter, were found to play important roles in the microbial network in terms of the potential to assist in groundwater clean-up. Notably, pollution from heavy metals has diminished the effectiveness and resilience of microbial communities in groundwater, thereby heightening the susceptibility of these normally stable microbial ecosystems. These findings offer new perspectives on how to monitor and detect groundwater pollution, and provide scientific guidance for developing suitable remediation methods for groundwater contaminated with heavy metals. Future research is essential explore the application of metal-tolerant or resistant bacteria in bioremediation strategies to rehabilitate groundwater systems contaminated by HMs.
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Monitoreo del Ambiente , Agua Subterránea , Metales Pesados , Contaminantes Químicos del Agua , Metales Pesados/análisis , Contaminantes Químicos del Agua/análisis , Contaminantes Químicos del Agua/metabolismo , Agua Subterránea/química , Agua Subterránea/microbiología , China , Monitoreo del Ambiente/métodos , Microbiota/efectos de los fármacos , Bacterias/metabolismo , Bacterias/efectos de los fármacos , Bacteroidetes , Industrias , EcosistemaRESUMEN
Presented herein is a novel synthesis of CF3-substituted pyrrolo[1,2-a]indole derivatives based on the cascade reactions of N-alkoxycarbamoyl indoles with CF3-ynones. Mechanistically, the formation of a product involves a tandem process initiated by Rh(III)-catalyzed and N-alkoxycarbamoyl group-directed regioselective C2-H alkenylation of the indole scaffold followed by in situ removal of the directing group and intramolecular N-nucleophilic addition/annulation under one set of reaction conditions. To our knowledge, this is the first example in which a N-alkoxycarbamoyl unit initially acts as a directing group for C2-H functionalization of the indole scaffold and is then removed to provide the required reactive NH-moiety for subsequent intramolecular condensation. Moreover, the products thus obtained could be conveniently transformed into structurally and biologically attractive cycloheptenone fused indole derivatives through an acid-promoted cascade transformation. In addition, studies on the activity of selected products against human cancer cell lines demonstrated their potential as lead compounds for the development of novel anticancer drugs.
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Presented herein is an effective and concise synthesis of acyl cyclopentaquinolinone derivatives via the cascade reactions of N-(o-ethynylaryl)acrylamides with α-diazo carbonyl compounds. The formation of product involves a visible light-induced radical formation from α-diazo carbonyl compound followed by its addition onto the acrylamide moiety to trigger double radical annulation, single-electron oxidation, and ß-elimination. To our knowledge, this is the first example in which the cyclopentaquinolinone scaffold was constructed along with the introduction of an acyl group under visible light irradiation conditions. Compared with literature methods for similar purpose, this newly developed protocol has advantages such as readily accessible substrates, mild reaction conditions, valuable products, concise synthetic procedure, and high sustainability. With all these merits, this method is expected to find wide applications in the construction of related acyl heterocyclic skeletons.
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Presented herein is a novel synthesis of pharmaceutically privileged spiroindoline derivatives via cascade reactions of N-methyl-N-nitrosoanilines with diazo homophthalimides. A group of mechanistic studies disclosed that the formation of product involves an unusual reaction mode of N-methyl-N-nitrosoaniline featuring an initial C(sp2)-H bond activation/alkylation followed by a C(sp3)-H bond activation/spiroannulation. To our knowledge, this is the first example in which N-methyl-N-nitrosoaniline acts as a C3N1 synthon to accomplish formal [4+1] spiroannulation with the participation of the N-methyl unit rather than the previously reported C2N1 synthon to undergo formal [3+2] annulation without the participation of the N-methyl unit. In general, this newly developed synthetic protocol features simple and readily accessible starting materials, valuable products, unique reaction mechanism, high efficiency and atom-economy, excellent compatibility with diverse functional groups, and ready scalability.