RESUMO
Perilipin 2 (Plin2) is known to be dysregulated in several human malignancies, which facilitates cancer progression. Recent studies have found that the abnormal expression of Plin2 is associated with poor prognosis of non-small cell lung cancer (NSCLC). However, the specific role of Plin2 and its underlying mechanism remain unclear. This study revealed that Plin2 expression was low in NSCLC tissues, and its relatively higher expression indicated larger tumor size and poorer prognosis. In vitro experiments proved that Plin2 promoted NSCLC cellular proliferation and inhibited autophagy by activating the AKT/mTOR pathway. Meanwhile, treatment with the AKT phosphorylation promoter or inhibitor neutralized the influence of Plin2 depletion or over-expression on proliferation and autophagy, respectively. In vivo study showed that Plin2 stimulated subcutaneous tumorigenesis of NSCLC cells in nude mice. Collectively, this study clarified the carcinogenic role of Plin2 and its molecular mechanism in NSCLC progression, which may facilitate a targeted therapy in the future.
Assuntos
Carcinoma Pulmonar de Células não Pequenas , Neoplasias Pulmonares , Animais , Camundongos , Humanos , Carcinoma Pulmonar de Células não Pequenas/patologia , Proteínas Proto-Oncogênicas c-akt/genética , Proteínas Proto-Oncogênicas c-akt/metabolismo , Neoplasias Pulmonares/patologia , Perilipina-2/metabolismo , Transdução de Sinais , Camundongos Nus , Linhagem Celular Tumoral , Serina-Treonina Quinases TOR/genética , Serina-Treonina Quinases TOR/metabolismo , Autofagia/genética , Proliferação de CélulasRESUMO
Contact electrification between water and a solid surface is crucial for physicochemical processes at water-solid interfaces. However, the nature of the involved processes remains poorly understood, especially in the initial stage of the interface formation. Here we report that H2O2 is spontaneously produced from the hydroxyl groups on the solid surface when contact occurred. The density of hydroxyl groups affects the H2O2 yield. The participation of hydroxyl groups in H2O2 generation is confirmed by mass spectrometric detection of 18O in the product of the reaction between 4-carboxyphenylboronic acid and 18O-labeled H2O2 resulting from 18O2 plasma treatment of the surface. We propose a model for H2O2 generation based on recombination of the hydroxyl radicals produced from the surface hydroxyl groups in the water-solid contact process. Our observations show that the spontaneous generation of H2O2 is universal on the surfaces of soil and atmospheric fine particles in a humid environment.
Assuntos
Eletricidade , Peróxido de Hidrogênio , Radical Hidroxila , Água , Atmosfera/química , Umidade , Peróxido de Hidrogênio/síntese química , Peróxido de Hidrogênio/química , Radical Hidroxila/química , Espectrometria de Massas , Isótopos de Oxigênio/análise , Isótopos de Oxigênio/química , Tamanho da Partícula , Solo/química , Água/químicaRESUMO
The detection of virus RNA in wastewater has been established as a valuable method for monitoring Coronavirus disease 2019. Carbon nanomaterials hold potential application in separating virus RNA owing to their effective adsorption and extraction capabilities. However, carbon nanomaterials have limited separability under homogeneous aqueous conditions. Due to the stabilities in their nanostructure, it is a challenge to efficiently immobilize them onto magnetic beads for separation. Here, we develop a porous agarose layered magnetic graphene oxide (GO) nanocomposite that is prepared by agglutinating ferroferric oxide (Fe3O4) beads and GO with agarose into a cohesive whole. With an average porous size of approximately 500 nm, the porous structure enables the unhindered entry of virus RNA, facilitating its interaction with the surface of GO. Upon the application of a magnetic field, the nucleic acid can be separated from the solution within a few minutes, achieving adsorption efficiency and recovery rate exceeding 90% under optimized conditions. The adsorbed nucleic acid can then be preserved against complex sample matrix for 3 days, and quantitatively released for subsequent quantitative reverse transcription polymerase chain reaction (RT-qPCR) detection. The developed method was successfully utilized to analyze wastewater samples obtained from a wastewater treatment plant, detecting as few as 10 copies of RNA molecules per sample. The developed aMGO-RT-qPCR provides an efficient approach for monitoring viruses and will contribute to wastewater-based surveillance of community infections.
Assuntos
Grafite , Nanocompostos , RNA Viral , Sefarose , Águas Residuárias , Grafite/química , Águas Residuárias/virologia , Águas Residuárias/química , RNA Viral/análise , RNA Viral/isolamento & purificação , Sefarose/química , Nanocompostos/química , Porosidade , AdsorçãoRESUMO
Low-cost fabric-based top-emitting polymer light-emitting devices (Fa-TPLEDs) have aroused increasing attention due to their remarkable potential applications in wearable displays. However, it is still challenging to realize efficient all-solution-processed devices from bottom electrodes to top electrodes with large-scale fabrication. Here, a smooth reflective Ag cathode integrated on fabric by one-step silver mirror reaction and a composite transparent anode of polydimethylsiloxane/silver nanowires/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) via a water-assisted peeling method are presented, both of which possess excellent optoelectrical properties and robust mechanical flexibility. The Fa-TPLEDs are constructed by spin-coating functional layers on the bottom reflective cathodes and laminating the top transparent anodes. The Fa-TPLEDs show a current efficiency of 16.3 cd A-1 , an external quantum efficiency of 4.9% and angle-independent electroluminescence spectra. In addition, the Fa-TPLEDs possess excellent mechanical stability, maintaining a current efficiency of 14.3 cd A-1 after 200 bending cycles at a radius of 4 mm. The results demonstrate that the integration of solution-processed reflective cathodes and transparent anodes sheds light on a new avenue to construct low-cost and efficient fabric-based devices, showing great potential applications in emerging smart flexible/wearable electronics.
RESUMO
Self-powered vibration sensor is highly desired for distributed and continuous monitoring requirements of Industry 4.0. Herein, a flexible fiber-shaped triboelectric nanogenerator (F-TENG) with a coaxial core-shell structure is proposed for the vibration monitoring. The F-TENG exhibits higher adaptability to the complex surfaces, which has an outstanding application prospect due to vital compensation for the existing rigid sensors. Initially, the contact characteristics between the dielectric layers, that related to the perceiving performance of the TENG, are theoretically analyzed. Such a TENG with 1D structure endows high sensitivity, allowing for accurately responding to a wide range of vibration frequencies (0.1 to 100 Hz). Even applying to the real diesel engine, the error in detecting the vibration frequencies is only 0.32% compared with the commercial vibration sensor, highlighting its potential in practical application. Further, assisted by deep learning, the recognition accuracy in monitoring nine operating conditions of the system achieves 97.87%. Overall, the newly designed F-TENG with the merits of high-adaptability, cost-efficiency, and self-powered, has offered a promising solution to fulfill an extensive range of vibration sensing applications in the future.
RESUMO
A computational framework based on placental gene networks was proposed in this work to improve the accuracy of the placental exposure risk assessment of environmental compounds. The framework quantitatively characterizes the ability of compounds to cross the placental barrier by systematically considering the interaction and pathway-level information on multiple placental transporters. As a result, probability scores were generated for 307 compounds crossing the placental barrier based on this framework. These scores were then used to categorize the compounds into different levels of transplacental transport range, creating a gradient partition. These probability scores not only facilitated a more intuitive understanding of a compound's ability to cross the placental barrier but also provided valuable information for predicting potential placental disruptors. Compounds with probability scores greater than 90% were considered to have significant transplacental transport potential, whereas those with probability scores less than 80% were classified as unlikely to cross the placental barrier. Furthermore, external validation set results showed that the probability score could accurately predict the compounds known to cross the placental barrier. In conclusion, the computational framework proposed in this study enhances the intuitive understanding of the ability of compounds to cross the placental barrier and opens up new avenues for assessing the placental exposure risk of compounds.
Assuntos
Poluentes Ambientais , Placenta , Gravidez , Feminino , Placenta/metabolismo , Humanos , Medição de Risco , Exposição AmbientalRESUMO
Cohorts of pregnant women in 2018 and 2020 were selected to explore prenatal exposure to perfluoroalkyl and polyfluoroalkyl substances (PFAS). Maternal serum during the whole pregnancy (first to third trimesters) and matched cord serum were collected for the analysis of 50 PFAS. Perfluorooctanoic acid (PFOA), perfluorooctanesulfonic acid (PFOS), and 6:2 fluorotelomer sulfonic acid (6:2 FTS) were the dominant PFAS in both the maternal and cord serum. The median ∑PFAS concentration was 14.18 ng/mL, and the ∑PFAS concentration was observed to decline from the first trimester to the third trimester. The transplacental transfer efficiencies (TTE) of 29 PFAS were comprehensively assessed, and a "U"-shaped trend in TTE values with increasing molecular chain length of perfluoroalkyl carboxylic acid (PFCA) was observed in this study. Moreover, the maternal concentrations of 9-chlorohexadecafluoro-3-oxanonane-1-sulfonic acid (6:2 Cl-PFESA), perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA), perfluoroundecanoic acid (PFUdA), perfluorododecanoic acid (PFDoA), PFOS, and hexafluoropropylene oxide dimer acid (HFPO-DA) in the 2020 cohort were significantly lower than those in the 2018 cohort, declining by about 23.85-43.2% from 2018 to 2020 (p < 0.05). Higher proportions of emerging PFAS were observed in fetuses born in 2020. This birth cohort was collected during the COVID-19 epidemic period. The change in the PFAS exposure scene might be in response to the different exposure profiles of the 2018 and 2020 cohorts, which are attributed to the impact of COVID-19 on the social activities and environment of pregnant women. Finally, by application of a multiple informant model, the third trimester was identified as the critical window of vulnerability to PFAS exposure that affects birth weight and birth length.
Assuntos
Fluorocarbonos , Humanos , Feminino , Gravidez , Adulto , COVID-19/epidemiologia , Ácidos Alcanossulfônicos , Estudos de Coortes , Exposição Materna , Poluentes Ambientais , CaprilatosRESUMO
Multiple pieces of evidence have shown that prenatal exposure to perfluoroalkyl and polyfluoroalkyl substances (PFASs) is closely related to adverse birth outcomes for infants. However, difficult access to human samples limits our understanding of PFASs transport and metabolism across the human placental barrier, as well as the accurate assessment of fetal PFASs exposure. Herein, we assess fetal exposure to 28 PFASs based on paired serum, placenta, and meconium samples. Overall, 21 PFASs were identified first to be exposed to the fetus prenatally and to be metabolized and excreted by the fetus. In meconium samples, 25 PFASs were detected, with perfluorooctane sulfonate and perfluorohexane sulfonic acid being the dominant congeners, suggesting the metabolism and excretion of PFASs through meconium. Perfluoroalkyl sulfonic acids might be more easily eliminated through the meconium than perfluorinated carboxylic acids. Importantly, based on molecular docking, MRP1, OATP2B1, ASCT1, and P-gp were identified as crucial transporters in the dynamic placental transfer of PFASs between the mother and the fetus. ATSC5p and PubchemFP679 were recognized as critical structural features that affect the metabolism and secretion of PFASs through meconium. With increasing carbon chain length, both the transplacental transfer efficiency and meconium excretion efficiency of PFASs showed a structure-dependent manner. This study reports, for the first time, that meconium, which is a noninvasive and stable biological matrix, can be strong evidence of prenatal PFASs exposure.
Assuntos
Ácidos Alcanossulfônicos , Fluorocarbonos , Recém-Nascido , Gravidez , Humanos , Feminino , Placenta , Mecônio/metabolismo , Simulação de Acoplamento Molecular , Ácidos Alcanossulfônicos/metabolismo , Ácidos Carboxílicos/metabolismoRESUMO
Persistent organic pollutants (POPs) tend to accumulate in cold regions by cold condensation and global distillation. Soil organic matter is the main storage compartment for POPs in terrestrial ecosystems due to deposition and repeated air-surface exchange processes. Here, physicochemical properties and environmental factors were investigated for their role in influencing POPs accumulation in soils of the Tibetan Plateau and Antarctic and Arctic regions. The results showed that the soil burden of most POPs was closely coupled to stable mineral-associated organic carbon (MAOC). Combining the proportion of MAOC and physicochemical properties can explain much of the soil distribution characteristics of the POPs. The background levels of POPs were estimated in conjunction with the global soil database. It led to the proposition that the stable soil carbon pools are key controlling factors affecting the ultimate global distribution of POPs, so that the dynamic cycling of soil carbon acts to counteract the cold-trapping effects. In the future, soil carbon pool composition should be fully considered in a multimedia environmental model of POPs, and the risk of secondary release of POPs in soils under conditions such as climate change can be further assessed with soil organic carbon models.
Assuntos
Carbono , Poluentes do Solo , Solo , Solo/química , Poluentes Orgânicos Persistentes , Monitoramento Ambiental , Regiões Árticas , EcossistemaRESUMO
PURPOSE: Pringle maneuver (PM) is a double-edged sword in liver resection, which is beneficial in reducing blood loss but also causes ischemia-reperfusion injury which may stimulate the outgrowth of micrometastases. The impact of PM on tumor recurrence remains controversial. This study aimed to assess whether PM has effect on the prognosis of colorectal cancer liver metastases (CRLM) after hepatectomy. METHODS: PubMed and the Cochrane Library databases were searched. The PM is defined as the portal triad clamping for several minutes, followed by several minutes of reperfusion, repeated as needed. Prolonged PM was defined as continuous clamping ≥ 20 min or ≥ 3 cycles for maximally 15-min intermittent ischemia. RESULTS: Eleven studies encompassing 4054 patients were included in this meta-analysis. The pooled hazard ratio (HR) did not show significant differences between PM and non-PM groups for disease-free survival (DFS) (HR = 0.91, 95% confidence interval (CI) 0.76-1.11, P = 0.36) and overall survival (HR = 1.03, 95% CI 0.76-1.39, P = 0.87). Subgroup analysis revealed that prolonged PM has adverse impact on DFS (HR 1.75, 95% CI = 1.28-2.40, P = 0.0005). However, non-prolonged PM is a protective factor for DFS (HR 0.82, 95% CI = 0.73-0.92, P = 0.001). CONCLUSION: These findings suggested that prolonged PM may have an adverse impact on the DFS of patients with CRLM and non-prolonged PM is a protective factor for DFS. Further prospective multicenter studies are warranted.
Assuntos
Neoplasias Colorretais , Hepatectomia , Neoplasias Hepáticas , Humanos , Neoplasias Colorretais/patologia , Neoplasias Colorretais/cirurgia , Neoplasias Colorretais/mortalidade , Neoplasias Hepáticas/secundário , Neoplasias Hepáticas/cirurgia , Neoplasias Hepáticas/mortalidade , Prognóstico , Intervalo Livre de Doença , Recidiva Local de Neoplasia , Perda Sanguínea Cirúrgica/estatística & dados numéricosRESUMO
As a typical organophosphorus flame retardant, tris(2-chloroethyl) phosphate (TCEP) is refractory in aqueous environment. The application of TAP is a promising method for removing pollutants. Herein, the removal of TCEP using TAP was rigorously investigated, and the effects of some key variables were optimized by the one-factor-at-a-time approach. To further evaluate the interactions among variables, the response surface methodology (RSM) based on central composite design was employed. Under optimized conditions (pH 5, [PS]0: [TCEP]0 = 500:1), the maximum removal efficiency (RE) of TCEP reached up to 90.6%. In real-world waters, the RE of TCEP spanned the range of 56%- 65% in river water, pond water, lake water and sanitary sewage. The low-concentration Cl- (0.1 mM) promoted TCEP degradation, but the contrary case occurred when the high-concentration Cl-, NO3-, CO32-, HCO3-, HPO42-, H2PO4-, NH4+ and humic acid were present owing to their prominently quenching effects on SO4â¢-. Both EPR and scavenger experiments revealed that the main radicals in the TAP system were SO4â¢- and â¢OH, in which SO4â¢- played the most crucial role in TCEP degradation. GC-MS/MS analysis disclosed that two degradation products appeared, sourcing from the replacement, oxidation, hydroxylation and water-molecule elimination reactions. The other two products were inferred from the comprehensive literature. As for acute toxicity to fish, daphnid and green algae, product A displayed the slightly higher toxicity, whereas other three products exhibited the declining toxicity as compared to their parent molecule. These findings offer a theoretical/practical reference for high-efficiency removal of TCEP and its ecotoxicological risk evaluation.
Assuntos
Retardadores de Chama , Fosfinas , Poluentes Químicos da Água , Retardadores de Chama/toxicidade , Espectrometria de Massas em Tandem , Compostos Organofosforados , Organofosfatos/toxicidade , Organofosfatos/química , Oxirredução , Água , Fosfatos , Poluentes Químicos da Água/toxicidade , Poluentes Químicos da Água/químicaRESUMO
The nanoscale zinc oxide (n-ZnO) was used in food packages due to its superior antibacterial activity, resulting in potential intake of n-ZnO through the digestive system, wherein n-ZnO interacted with saliva. In recent, facet engineering, a technique for controlling the exposed facets, was applied to n-ZnO, whereas risk of n-ZnO with specific exposed facets in saliva was ignored. ZnO nanoflakes (ZnO-0001) and nanoneedles (ZnO-1010) with the primary exposed facets of {0001} and {1010} respectively were prepared in this study, investigating stability and toxicity of ZnO-0001 and ZnO-1010 in synthetic saliva. Both ZnO-0001 and ZnO-1010 partially transformed into amorphous Zn3(PO4)2 within 1 hr in the saliva even containing orgnaic components, forming a ZnO-Zn3(PO4)2 core-shell structure. Nevertheless, ZnO-1010 relative to ZnO-0001 would likely transform into Zn3(PO4)2, being attributed to superior dissolution of {1010} facet due to its lower vacancy formation energy (1.15 eV) than {0001} facet (3.90 eV). The toxicity of n-ZnO to Caco-2 cells was also dependent on the primary exposed facet; ZnO-0001 caused cell toxicity through oxidative stress, whereas ZnO-1010 resulted in lower cells viability than ZnO-0001 through oxidative stress and membrane damage. Density functional theory calculations illustrated that ·O2- was formed and released on {1010} facet, yet O22- instead of ·O2- was generated on {0001} facet, leading to low oxidative stress from ZnO-0001. All findings demonstrated that stability and toxicity of n-ZnO were dependent on the primary exposed facet, improving our understanding of health risk of nanomaterials.
Assuntos
Óxido de Zinco , Humanos , Óxido de Zinco/toxicidade , Óxido de Zinco/química , Células CACO-2 , Saliva , Estresse OxidativoRESUMO
MOTIVATION: RNA-binding proteins (RBPs) are a group of proteins associated with RNA regulation and metabolism, and play an essential role in mediating the maturation, transport, localization and translation of RNA. Recently, Genome-wide RNA-binding event detection methods have been developed to predict RBPs. Unfortunately, the existing computational methods usually suffer some limitations, such as high-dimensionality, data sparsity and low model performance. RESULTS: Deep convolution neural network has a useful advantage for solving high-dimensional and sparse data. To improve further the performance of deep convolution neural network, we propose evolutionary deep convolutional neural network (EDCNN) to identify protein-RNA interactions by synergizing evolutionary optimization with gradient descent to enhance deep conventional neural network. In particular, EDCNN combines evolutionary algorithms and different gradient descent models in a complementary algorithm, where the gradient descent and evolution steps can alternately optimize the RNA-binding event search. To validate the performance of EDCNN, an experiment is conducted on two large-scale CLIP-seq datasets, and results reveal that EDCNN provides superior performance to other state-of-the-art methods. Furthermore, time complexity analysis, parameter analysis and motif analysis are conducted to demonstrate the effectiveness of our proposed algorithm from several perspectives. AVAILABILITY AND IMPLEMENTATION: The EDCNN algorithm is available at GitHub: https://github.com/yaweiwang1232/EDCNN. Both the software and the supporting data can be downloaded from: https://figshare.com/articles/software/EDCNN/16803217. SUPPLEMENTARY INFORMATION: Supplementary data are available at Bioinformatics online.
Assuntos
Algoritmos , Redes Neurais de Computação , Software , Proteínas de Ligação a RNA/metabolismo , RNA/metabolismoRESUMO
Human adenovirus (HAdV) is a highly virulent respiratory pathogen that poses clinical challenges in terms of diagnostics and treatment. Currently, no effective therapeutic drugs or prophylactic vaccines are available for HAdV infections. One factor contributing to this deficiency is that existing animal models, including wild-type and single-receptor transgenic mice, are unsuitable for HAdV proliferation and pathology testing. In this study, a tri-receptor transgenic mouse model expressing the three best-characterized human cellular receptors for HAdV (hCAR, hCD46, and hDSG2) was generated and validated via analysis of transgene insertion, receptor mRNA expression, and protein abundance distribution. Following HAdV-7 infection, the tri-receptor mice exhibited high transcription levels at the early and late stages of the HAdV gene, as well as viral protein expression. Furthermore, the tri-receptor mice infected with HAdV exhibited dysregulated cytokine responses and multiple tissue lesions. This transgenic mouse model represents human HAdV infection and pathogenesis with more accuracy than any other reported animal model. As such, this model facilitates the comprehensive investigation of HAdV pathogenesis as well as the evaluation of potential vaccines and therapeutic modalities for HAdV.
Assuntos
Infecções por Adenoviridae , Infecções por Adenovirus Humanos , Adenovírus Humanos , Camundongos , Animais , Humanos , Camundongos Transgênicos , Processamento de Proteína Pós-Traducional , Expressão Gênica , Modelos Animais de Doenças , Adenovírus Humanos/fisiologiaRESUMO
Two Gram-stain-negative, strictly aerobic, chemoheterotrophic, short-rod-shaped and non-motile strains, forming yellow colonies and designated F47161T and F64183T, were isolated from marine sediment of Xiaoshi Island, Wei Hai, PR China. Strain F47161T grew at 15-37 °C (optimally at 30 °C) and pH 6.0-9.0 (optimally at pH 7.5) and in the presence of 1-9â% (w/v) NaCl (optimally at 3â%). Strain F64183T grew at 10-37 °C (optimally at 30 °C) and pH 6.0-8.5 (optimally at pH 7.0) and in the presence of 1-8â% (w/v) NaCl (optimally at 3â%). The results of phylogenetic analysis based on 16S rRNA gene sequences indicated that F47161T and F64183T were related to members of the genus Aequorivita. The strains shared 97.4â% 16S rRNA gene sequence similarity to each other. F47161T and F64183T shared highest 16S rRNA gene sequence similarity to Aequorivita sinensis JCM 19789T, and the values were 97.5â% and 98.4 %, respectively. The predominant cellular fatty acids of both F64183T and F47161T were iso-C15â:â0 and iso-C17â:â0 3-OH, but the predominant fatty acids of F47161T also included anteiso-C15â:â0. The sole respiratory quinone of F47161T and F64183T was menaquinone 6 (MK-6), consistent with that observed for all related strains. Between F47161T and F64183T, the average nucleotide identity (ANI) and digital DNA-DNA hybridisation (dDDH) values were 75.8â% and 20.5â%, respectively, and between the novel isolates (F47161T and F64183T) and A. sinensis JCM 19789T they were 76.0â% and 94.2â% and 20.6â% and 57.1â%, respectively. The genomic DNA G+C contents of F47161T and F64183T was 37.3â% and 34.5â%, respectively. The polar lipid profiles of F47161T and F64183T contained phosphatidylethanolamine, two aminolipids, one glycolipid, one phosphoglycolipid and two unidentified polar lipids. Differential phenotypic and genotypic characteristics of the two strains indicated that the two strains should be classified as representing two novel species of the genus Aequorivita, for which the names Aequorivita vitellina sp. nov. and Aequorivita xiaoshiensis sp. nov. are proposed. The type strains are F47161T (=MCCC 1H00509T=KCTC 92017T) and F64183T (=MCCC 1H00507T=KCTC 92016T), respectively.
Assuntos
Ácidos Graxos , Flavobacteriaceae , Ácidos Graxos/química , Água do Mar , Filogenia , RNA Ribossômico 16S/genética , Cloreto de Sódio , DNA Bacteriano/genética , Composição de Bases , Técnicas de Tipagem Bacteriana , Análise de Sequência de DNA , Sedimentos Geológicos , Vitamina K 2/químicaRESUMO
Glacier-retreated areas are ideal areas to study soil biogeochemical processes during vegetation succession, because of the limited effect of other environmental and climatic factors. In this study, the changes of soil dissolved organic matter (DOM) and its relationship with microbial communities along the Hailuogou Glacier forefield chronosequence were investigated. Both microbial diversity and DOM molecular chemodiversity recovered rapidly at the initial stage, indicating the pioneering role of microorganisms in soil formation and development. The chemical stability of soil organic matter enhanced with vegetation succession due to the retaining of compounds with high oxidation state and aromaticity. The molecular composition of DOM affected microbial communities, while microorganisms tended to utilize labile components to form refractory components. This complex relationship network between microorganisms and DOM components played an important role in the development of soil organic matter as well as the formation of stable soil carbon pool in glacier-retreated areas.
Assuntos
Microbiota , Solo , Solo/química , Matéria Orgânica Dissolvida , Camada de Gelo , Microbiologia do SoloRESUMO
Per- and polyfluoroalkyl substances (PFASs), including perfluorohexanesulfonic acid (PFHxS), as emerging persistent organic pollutants widely detected in drinking water, have drawn increasing concern. The PFHxS contamination of drinking water always results from direct and indirect sources, especially the secondary generations through environmental transformations of precursors. However, the mechanism of the transformation of precursors to PFHXS during the drinking water treatment processes remains unclear. Herein, the potential precursors and formation mechanisms of PFHxS were explored during drinking water disinfection. Simultaneously, the factors affecting PFHxS generation were also examined. This study found PFHxS could be generated from polyfluoroalkyl sulfonamide derivatives during chlorination and chloramination. The fate and yield of PFHxS varied from different precursors and disinfection processes. In particular, monochloramine more favorably formed PFHxS. Several perfluoroalkyl oxidation products and decarboxylation intermediates were detected and identified in the chloraminated samples using Fourier-transform ion cyclotron resonance mass spectrometry. Combined with density functional theory calculations, the results indicated that the indirect oxidation via the attack of the nitrogen atom in sulfonamide groups might be the dominant pathway for generating PFHxS during chloramination, and the process could be highly affected by the monochloramine dose, pH, and temperature. This study provides important evidence of the secondary formation of PFHxS during drinking water disinfection and scientific support for chemical management of PFHxS and PFHxS-related compounds.
Assuntos
Desinfetantes , Água Potável , Poluentes Químicos da Água , Purificação da Água , Água Potável/análise , Poluentes Químicos da Água/análise , Desinfecção , Sulfonamidas/análise , Halogenação , Purificação da Água/métodos , Sulfanilamida/análise , Desinfetantes/análiseRESUMO
Brown carbon (BrC) is one of the most mysterious aerosol components responsible for global warming and air pollution. Iron (Fe)-induced catalytic oxidation of ubiquitous phenolic compounds has been considered as a potential pathway for BrC formation in the dark. However, the reaction mechanism and product composition are still poorly understood. Herein, 13 phenolic precursors were employed to react with Fe under environmentally relevant conditions. Using Fourier transform ion cyclotron resonance mass spectrometry, a total of 764 unique molecular formulas were identified, and over 85% of them can be found in atmospheric aerosols. In particular, products derived from precursors with catechol-, guaiacol-, and syringol-like-based structures can be distinguished by their optical and molecular characteristics, indicating the structure-dependent formation of BrC from phenolic precursors. Multiple pieces of evidence indicate that under acidic conditions, the contribution of either autoxidation or oxygen-induced free radical oxidation to BrC formation is extremely limited. Ligand-to-Fe charge transfer and subsequent phenoxy radical coupling reactions were the main mechanism for the formation of polymerization products with high molecular diversity, and the efficiency of BrC generation was linearly correlated with the ionization potential of phenolic precursors. The present study uncovered how chemically diverse BrC products were formed by the Fe-phenolic compound reactions at the molecular level and also provide a new paradigm for the study of the atmospheric aerosol formation mechanism.
Assuntos
Poluentes Atmosféricos , Compostos de Ferro , Carbono , Aerossóis/análise , Compostos de Ferro/análise , Ferro , Guaiacol/análise , Poluentes Atmosféricos/análiseRESUMO
Per- and polyfluoroalkyl substances (PFAS) receive significant research attention due to their potential adverse effects on human health. Evidence shows that the kidney is one of the target organs of PFAS. In occupational exposure scenarios, high PFAS concentrations may adversely affect kidney metabolism, but whether this effect is reflected in the small metabolic molecules contained in urine remains unknown. In this study, 72 matched serum and urine samples from occupational workers of a fluorochemical manufactory as well as 153 urine samples from local residents were collected, and 23 PFAS levels were quantified. The concentrations of Σ23PFAS in the serum and urine samples of workers were 5.43 ± 1.02 µg/mL and 201 ± 46.9 ng/mL, respectively, while the Σ23PFAS concentration in the urine of the residents was 6.18 ± 0.76 ng/mL. For workers, high levels of urinary PFAS were strongly correlated with levels in serum (r = 0.57-0.93), indicating that urinary PFAS can be a good indicator for serum PFAS levels. Further, a urine nontargeted metabolomics study was conducted. The results of association models, including Bayesian kernel machine regression, demonstrated positive correlations between urinary PFAS levels and key small kidney molecules. A total of eight potential biomarkers associated with PFAS exposure were identified, and all of them showed significant positive correlations with markers of kidney function. These findings provide the first evidence that urine can serve as a matrix to indicate the adverse health effects of high levels of exposure to PFAS on the kidneys.
Assuntos
Ácidos Alcanossulfônicos , Poluentes Ambientais , Fluorocarbonos , Exposição Ocupacional , Humanos , Teorema de Bayes , Fluorocarbonos/análise , Metabolômica , Rim/química , Ácidos Alcanossulfônicos/análise , Poluentes Ambientais/análiseRESUMO
Semiconductor photocatalysis has become an increasing area of interest for use in water treatment methods. This review systematically presents the recent developments of emerging semiconductor photocatalysis system and their application in the removal of water pollutants. A brief overview of the semiconductor photocatalysis mechanism involved with the generation of reactive oxygen species (ROS) is provided first. Then a detailed explanation of the development of TiO2-based, g-C3N4-based, and bismuth-based semiconductor materials and their applications in the degradation of water pollutants are highlighted with recent illustrative examples. Furthermore, the future prospects of semiconductor photocatalysis for water treatment are critically analyzed.