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The lattice parameter of platinum-based intermetallic compounds (IMCs), which correlates with the intrinsic activity of the oxygen reduction reaction (ORR), can be modulated by crystal phase engineering. However, the controlled preparation of IMCs with unconventional crystal structures remains highly challenging. Here, we demonstrate the synthesis of carbon-supported PtCu-based IMC catalysts with an unconventional L10 structure by a composition-regulated strategy. Experiment and machine learning reveal that the thermodynamically favorable structure changes from L11 to L10 when slight Cu atoms are substituted with Co. Benefiting from crystal-phase-induced strain enhancement, the prepared L10-type PtCu0.8Co0.2 catalyst exhibits much-enhanced mass and specific activities of 1.82 A mgPt-1 and 3.27 mA cmPt-2, which are 1.91 and 1.73 times higher than those of the L11-type PtCu catalyst, respectively. Our work highlights the important role of crystal phase in determining the surface strain of IMCs, and opens a promising avenue for the rational preparation of IMCs with different crystal phases by doping.
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Improving the interconnected structure and bioregulatory function of natural chitosan is beneficial for optimizing its performance in bone regeneration. Here, a facile immunoregulatory constructional design is proposed for developing instructive chitosan by directional freezing and alkaline salting out. The molecular dynamics simulation confirmed the assembly kinetics and structural features of various polyphenols and chitosan molecules. Along with the in vitro anti-inflammatory, antioxidative, promoting bone mesenchymal stem cell (BMSC) adhesion and proliferation performance, proanthocyanidin optimizing chitosan (ChiO) scaffold presented an optimal immunoregulatory structure with the directional microchannel. Transcriptome analysis in vitro further revealed the cytoskeleton- and immune-regulation effect of ChiO are the key mechanism of action on BMSC. The rabbit cranial defect model (Φ = 10 mm) after 12 weeks of implantation confirmed the significantly enhanced bone reconstitution. This facile immunoregulatory directional microchannel design provides effective guidance for developing inducible chitosan scaffolds.
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Quitosano , Células Madre Mesenquimatosas , Proantocianidinas , Quitosano/química , Proantocianidinas/química , Proantocianidinas/farmacología , Animales , Conejos , Células Madre Mesenquimatosas/citología , Células Madre Mesenquimatosas/efectos de los fármacos , Andamios del Tejido/química , Proliferación Celular/efectos de los fármacos , Adhesión Celular/efectos de los fármacos , Simulación de Dinámica MolecularRESUMEN
This review explores the growing interest in 2D layered materials, such as graphene, h-BN, transition metal dichalcogenides (TMDs), and black phosphorus (BP), with a specific focus on recent advances in strain engineering. Both experimental and theoretical results are delved into, highlighting the potential of strain to modulate physical properties, thereby enhancing device performance. Various strain engineering methods are summarized, and the impact of strain on the electrical, optical, magnetic, thermal, and valleytronic properties of 2D materials is thoroughly examined. Finally, the review concludes by addressing potential applications and challenges in utilizing strain engineering for functional devices, offering valuable insights for further research and applications in optoelectronics, thermionics, and spintronics.
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In recent years, the coastal area in East China has experienced elevated volatile organic compounds (VOCs) levels during specific periods. VOCs have become one of the major atmospheric pollutants in these areas. In this study, 64 compounds including alkanes, alkenes, halohydrocarbons, aromatics, and oxygenated VOCs (OVOCs) were obtained by the TO-15 method through a 12-month campaign in industrial, urban and suburban areas in the Yangtze River Delta of China. The overall trends of total VOC (TVOC) concentrations at eight sampling sites were as follows: winter > autumn > spring > summer. The proportion of VOC categories was various at industrial sites, while OVOCs and halohydrocarbons had high proportions at urban sites and suburban sites, respectively. Coating, vehicle emission, petrochemical source, industrial source, and gasoline volatilization were identified as the major VOC emission sources by the positive matrix factorization model. Petrochemical and coating sources were the prime VOC sources at industrial sites. Aromatics contributed the most ozone formation potential at industrial sites, while OVOCs provided the main contributions at both urban and suburban sites during four seasons. According to the health risk assessment, a high probability of non-carcinogenic risk existed at three industrial sites. Special attention should be given to certain VOCs, such as acrolein and 1,2-dibromoethane in industrial areas.
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Contaminantes Atmosféricos , Monitoreo del Ambiente , Compuestos Orgánicos Volátiles , Compuestos Orgánicos Volátiles/análisis , China , Contaminantes Atmosféricos/análisis , Ríos/química , Estaciones del Año , IndustriasRESUMEN
In recent years, remotely controlling an unmanned aerial vehicle (UAV) to perform coverage search missions has become increasingly popular due to the advantages of the UAV, such as small size, high maneuverability, and low cost. However, due to the distance limitations of the remote control and endurance of a UAV, a single UAV cannot effectively perform a search mission in various and complex regions. Thus, using a group of UAVs to deal with coverage search missions has become a research hotspot in the last decade. In this paper, a differential evolution (DE)-based multi-UAV cooperative coverage algorithm is proposed to deal with the coverage tasks in different regions. In the proposed algorithm, named DECSMU, the entire coverage process is divided into many coverage stages. Before each coverage stage, every UAV automatically plans its flight path based on DE. To obtain a promising flight trajectory for a UAV, a dynamic reward function is designed to evaluate the quality of the planned path in terms of the coverage rate and the energy consumption of the UAV. In each coverage stage, an information interaction between different UAVs is carried out through a communication network, and a distributed model predictive control is used to realize the collaborative coverage of multiple UAVs. The experimental results show that the strategy can achieve high coverage and a low energy consumption index under the constraints of collision avoidance. The favorable performance in DECSMU on different regions also demonstrate that it has outstanding stability and generality.
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The quantity of sensor nodes within current computing systems is rapidly increasing in tandem with the sensing data. The presence of a bottleneck in data transmission between the sensors, computing, and memory units obstructs the system's efficiency and speed. To minimize the latency of data transmission between units, novel in-memory and in-sensor computing architectures are proposed as alternatives to the conventional von Neumann architecture, aiming for data-intensive sensing and computing applications. The integration of 2D materials and 2D ferroelectric materials has been expected to build these novel sensing and computing architectures due to the dangling-bond-free surface, ultra-fast polarization flipping, and ultra-low power consumption of the 2D ferroelectrics. Here, the recent progress of 2D ferroelectric devices for in-sensing and in-memory neuromorphic computing is reviewed. Experimental and theoretical progresses on 2D ferroelectric devices, including passive ferroelectrics-integrated 2D devices and active ferroelectrics-integrated 2D devices, are reviewed followed by the integration of perception, memory, and computing application. Notably, 2D ferroelectric devices have been used to simulate synaptic weights, neuronal model functions, and neural networks for image processing. As an emerging device configuration, 2D ferroelectric devices have the potential to expand into the sensor-memory and computing integration application field, leading to new possibilities for modern electronics.
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Groundwater contamination resulting from petroleum development poses a significant threat to drinking water sources, especially in developing countries. In situ natural remediation methods, including microbiological processes, have gained popularity for the reduction of groundwater contaminants. However, assessing the stage of remediation in deep contaminated groundwater is challenging and costly due to the complexity of diverse geological conditions and unknown initial concentrations of contaminants. This research proposes that redox zonation may be a more convenient and comprehensive indicator than the concentration of contaminants for determining the stage of natural remediation in deep groundwater. The combination of sequencing microbial composition using the high-throughput 16S rRNA gene and function predicted by FAPROTAX is a useful approach to determining the redox conditions of different contaminated groundwater. The sulfate-reducing environment, represented by Desulfobacteraceae, Peptococcaceae, Desulfovibrionaceae, and Desulfohalobiaceae could be used as characteristic early stages of remediation for produced water contamination in wells with high concentrations of SO42-, benzene, and salinity. The nitrate-reducing environment, enriched with microorganisms related to denitrification, sulfur-oxidizing, and methanophilic microorganisms could be indicative of the mid stages of in situ bioremediation. The oxygen reduction environment, enriched with oligotrophic and pathogenic Sphingomonadaceae, Caulobacteraceae, Syntrophaceae, Legionellales, Moraxellaceae, and Coxiellaceae, could be indicative of the late stages of remediation. This comprehensive approach could provide valuable insights into the process of natural remediation and facilitate improved environmental management in areas of deep contaminated groundwater.
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Biodegradación Ambiental , Agua Subterránea , Oxidación-Reducción , Contaminantes Químicos del Agua , Agua Subterránea/química , Agua Subterránea/microbiología , Contaminantes Químicos del Agua/análisis , ARN Ribosómico 16S , Monitoreo del Ambiente/métodos , Restauración y Remediación Ambiental/métodos , Microbiología del AguaRESUMEN
Fine-tuning pre-trained language models (LMs) may not always be the most practical approach for downstream tasks. While adaptation fine-tuning methods have shown promising results, a clearer explanation of their mechanisms and further inhibition of the transmission of information is needed. To address this, we propose an Inhibition Adaptation (InA) fine-tuning method that aims to reduce the number of added tunable weights and appropriately reweight knowledge derived from pre-trained LMs. The InA method involves (1) inserting a small trainable vector into each Transformer attention architecture and (2) setting a threshold to directly eliminate irrelevant knowledge. This approach draws inspiration from the shunting inhibition, which allows the inhibition of specific neurons to gate other functional neurons. With the inhibition mechanism, InA achieves competitive or even superior performance compared to other fine-tuning methods on BERT-large, RoBERTa-large, and DeBERTa-large for text classification and question-answering tasks.
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Lenguaje , Humanos , Redes Neurales de la Computación , Inhibición Neural/fisiología , Neuronas/fisiologíaRESUMEN
Cell line authentication plays a crucial role in the biomedical field, ensuring researchers work with accurately identified cells. Supervised deep learning has made remarkable strides in cell line identification by studying cell morphological features through cell imaging. However, biological batch (bio-batch) effects, a significant issue stemming from the different times at which data is generated, lead to substantial shifts in the underlying data distribution, thus complicating reliable differentiation between cell lines from distinct batch cultures. To address this challenge, we introduce CLANet, a pioneering framework for cross-batch cell line identification using brightfield images, specifically designed to tackle three distinct bio-batch effects. We propose a cell cluster-level selection method to efficiently capture cell density variations, and a self-supervised learning strategy to manage image quality variations, thus producing reliable patch representations. Additionally, we adopt multiple instance learning(MIL) for effective aggregation of instance-level features for cell line identification. Our innovative time-series segment sampling module further enhances MIL's feature-learning capabilities, mitigating biases from varying incubation times across batches. We validate CLANet using data from 32 cell lines across 93 experimental bio-batches from the AstraZeneca Global Cell Bank. Our results show that CLANet outperforms related approaches (e.g. domain adaptation, MIL), demonstrating its effectiveness in addressing bio-batch effects in cell line identification.
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Autenticación de Línea Celular , Humanos , Páncreas , Factores de TiempoRESUMEN
Most current research focusing on the health risk assessments of particulate polycyclic aromatic hydrocarbons (PAHs) have not analyzed the size distributions and human respiratory deposition rates. In the present study, size-separated particulate matter (PM) was collected in the coastal area of Ningbo using an Anderson eight-stage air sampler over a 1-year period (2014-2015). The 16 US Environmental Protection Agency priority PAHs associated with PM were pretreated with rapid solvent extraction and analyzed by gas chromatography-mass spectrometry. The respiratory exposure assessment was determined using the multiple-path particle dosimetry (MPPD) model. The results show that all PAHs exhibited bimodal distribution with one mode peak in accumulation mode (0.43-0.65 µm) and another mode peak in coarse mode (4.7-5.8 µm). In addition, a low coefficient of divergence of PAHs between PM2.1 and PM2.1-10 indicated a high spatial heterogeneity in source factor contribution and formation mechanism. The deposition fluxes (tracheobronchial + pulmonary) of PM were highest for children in the size range of 3.3 µm < particle diameter (Dp) < 9 µm, while for males and females the highest fluxes occurred in the size range of 1.1 µm < Dp < 2.1 µm. The depositions of coarse PM in children were significantly higher than those in adults. The benzo[a]pyrene equivalent (BaPeq) depositions of dibenz[a,h]anthracene ranged from 1.4e-04 to 0.015 ng h-1, which were highest among the PAHs. The PAHs on particles with Dp >4.7 µm contributed approximately three times more to children than to males and females. Therefore, the toxicity of coarse PM to children needed attention. The incremental lifetime cancer risks (ILCR) for children, males, and females were estimated to be 2.92 × 10-7, 1.82 × 10-7, and 2.38 × 10-7, respectively, which were below the cancer risk guideline value (10-6). These ILCR values were much lower than the risks calculated without considering particle size distributions and respiratory depositions. The combination of the size-segregated sampling technique and the MPPD model can effectively avoid the overestimation of human respiratory exposure. Environ Toxicol Chem 2024;43:1364-1377. © 2024 SETAC.
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Contaminantes Atmosféricos , Tamaño de la Partícula , Material Particulado , Hidrocarburos Policíclicos Aromáticos , Hidrocarburos Policíclicos Aromáticos/análisis , Hidrocarburos Policíclicos Aromáticos/toxicidad , China , Material Particulado/análisis , Humanos , Contaminantes Atmosféricos/análisis , Contaminantes Atmosféricos/toxicidad , Medición de Riesgo , Femenino , Masculino , Niño , Adulto , Monitoreo del Ambiente , Adolescente , Adulto Joven , Exposición por Inhalación/análisis , Preescolar , Persona de Mediana EdadRESUMEN
Mollisols rich in natural organic matter are a significant sink of carbon (C) and selenium (Se). Climate warming and agricultural expansion to the cold Mollisol regions may enhance soil respiration and biogeochemical cycles, posing a growing risk of soil C and Se loss. Through field-mimicking incubation experiments with uncultivated and cultivated soils from the Mollisol regions of northeastern China, this research shows that soil respiration remained significant even during cold seasons and caused co-emission of greenhouse gases (CO2 and CH4) and methylated Se. Such stimulus effects were generally stronger in the cultivated soils, with maximum emission rates of 7.45 g/m2/d C and 1.42 µg/m2/d Se. For all soil types, the greatest co-emission of CO2 and dimethyl selenide occurred at 25 % soil moisture, whereas measurable CH4 emission was observed at 40 % soil moisture with higher percentages of dimethyl diselenide volatilization. Molecular characterization with three-dimensional fluorescence and ultra-high resolution mass spectrometry suggests that CO2 emission is sensitive to the availability of microbial protein-like substances and free energy from organic carbon biodegradation under variable moisture conditions. Predominant Se binding to biodegradable organic matter resulted in high dependence of Se volatilization on rates of greenhouse gas emissions. These findings together highlight the importance of dynamic organic carbon quality for soil respiration and consequent Mollisol Se loss risk, with implications for science-based management of C and Se resources in agricultural lands to combat with Se deficiency.
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Dióxido de Carbono , Gases de Efecto Invernadero , Metano , Selenio , Suelo , Suelo/química , Selenio/análisis , Selenio/metabolismo , Gases de Efecto Invernadero/análisis , Metano/metabolismo , China , Dióxido de Carbono/análisis , Microbiología del Suelo , MetilaciónRESUMEN
Antibiotics easily remain in sediments after migrating from the surface to the subsurface due to water-rock interactions, posing a risk of secondary release to groundwater. To investigate the vertical distribution characteristics and environmental impact factors of antibiotics, five 30 m quaternary sediment columns were drilled and stratified near the hospital, and five major classes of antibiotics and sulfonamide metabolites were tested and analyzed. The results showed that:â the antibiotic content in the sediments ranged from 3.05 to 107.03 µg·kg-1, and all of the target antibiotics were detected except lomefloxacin, of which ofloxacin and oxytetracycline were the most important antibiotics in the study area. â¡ The antibiotics did not show a strict downward trend in the vertical direction but varied with the lithological stratification. ⢠Antibiotics were primarily deposited in the clay layer and varied with the fluctuation of the groundwater level. ⣠The results of redundancy analysis between antibiotics and environmental factors suggested that pH and TOC controlled the fate and transformation of antibiotics through influencing the adsorption of antibiotics by sediments. The risk of antibiotic contamination from hospital wastewater seepage into the subsurface environment should be taken seriously.
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Agua Subterránea , Contaminantes Químicos del Agua , Antibacterianos/análisis , Contaminantes Químicos del Agua/análisis , Monitoreo del Ambiente , Sedimentos Geológicos/química , ChinaRESUMEN
We introduce a straightforward, yet effective strategy to combat the performance decline of proton-exchange membrane fuel cells in low-humidity environments. Our method centers on air-oxidizing carbon supports, significantly improving proton and oxygen transport within the cathode catalyst layer.
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Bone regenerative scaffolds with a bionic natural bone hierarchical porous structure provide a suitable microenvironment for cell migration and proliferation. Here, a bionic scaffold (DP-PLGA/HAp) with directional microchannels is prepared by combining 3D printing and directional freezing technology. The 3D printed framework provides structural support for new bone tissue growth, while the directional pore embedded in the scaffolds provides an express lane for cell migration and nutrition transport, facilitating cell growth and differentiation. The hierarchical porous scaffolds achieve rapid infiltration and adhesion of bone marrow mesenchymal stem cells (BMSCs) and improve the expression of osteogenesis-related genes. The rabbit cranial defect experiment presents significant new bone formation, demonstrating that DP-PLGA/HAp offers an effective means to guide cranial bone regeneration. The combination of 3D printing and directional freezing technology might be a promising strategy for developing bone regenerative biomaterials.
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Regeneración Ósea , Células Madre Mesenquimatosas , Osteogénesis , Impresión Tridimensional , Andamios del Tejido , Regeneración Ósea/fisiología , Animales , Conejos , Andamios del Tejido/química , Células Madre Mesenquimatosas/citología , Células Madre Mesenquimatosas/metabolismo , Osteogénesis/efectos de los fármacos , Osteogénesis/fisiología , Porosidad , Diferenciación Celular , Copolímero de Ácido Poliláctico-Ácido Poliglicólico/química , Ingeniería de Tejidos/métodos , Proliferación Celular , Materiales Biocompatibles/química , Materiales Biocompatibles/farmacología , Durapatita/químicaRESUMEN
Urban groundwater, serving as a critical reservoir for potable water, faces susceptibility to contamination from discrete sources such as hospital wastewater. This study investigates the distribution and plausible origins of antibiotics and antibiotic resistance genes (ARGs) in urban groundwater, drawing comparisons between areas proximal to hospitals and non-hospital areas. Ofloxacin and oxytetracycline emerged as the prevalent antibiotics across all samples, with a discernibly richer array of antibiotic types observed in groundwater sourced from hospital-adjacent regions. Employing a suite of multi-indicator tracers encompassing indicator drugs, Enterococci, ammonia, and Cl/Br mass ratio, discernible pollution from hospital or domestic sewage leakage was identified in specific wells, correlating with an escalating trajectory in antibiotic contamination. Redundancy analysis underscored temperature and dissolved organic carbon as principal environmental factors influencing antibiotics distribution in groundwater. Network analysis elucidated the facilitating role of mobile genetic elements, such as int1 and tnpA-02 in propagating ARGs. Furthermore, ARGs abundance exhibited positive correlations with temperature, pH and metallic constituents (e.g., Cu, Pb, Mn and Fe) (p < 0.05). Notably, no conspicuous correlation manifested between antibiotics and ARGs. These findings accentuate the imperative of recognizing the peril posed by antibiotic contamination in groundwater proximal to hospitals and advocate for the formulation of robust prevention and control strategies to mitigate the dissemination of antibiotics and ARGs.
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Antibacterianos , Agua Subterránea , Antibacterianos/farmacología , Genes Bacterianos , Farmacorresistencia Microbiana/genética , Hospitales UrbanosRESUMEN
Nanohydroxyapatite (nHAp) has attracted significant attention for its tumor suppression and tumor microenvironment modulation capabilities. However, a strong tendency to aggregate greatly affects its anti-tumor efficiency. To address this issue, a hydrogel platform consisting of thiolated hyaluronic acid (HA-SH) modified nanohydroxyapatite (nHAp-HA) and HA-SH was developed for sustained delivery of nHAp for melanoma therapy. The hydrophilic and negatively charged HA-SH significantly improved the size dispersion and stability of nHAp in aqueous media while conferring nHAp targeting effects. Covalent sulfhydryl self-cross-linking between HA-SH and nHAp-HA groups ensured homogeneous dispersion of nHAp in the matrix material. Meanwhile, the modification of HA-SH conferred the targeting properties of nHAp and enhanced cellular uptake through the HA/CD44 receptor. The hydrogel platform could effectively reduce the aggregation of nHAp and release nHAp in a sustained and orderly manner. Antitumor experiments showed that the modified nHAp-HA retained the tumor cytotoxicity of nHAp in vitro and inhibited the growth of highly malignant melanomas up to 78.6% while being able to induce the differentiation of macrophages to the M1 pro-inflammatory and antitumor phenotype. This study will broaden the application of nanohydroxyapatite in tumor therapy.
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Durapatita , Ácido Hialurónico , Hidrogeles , Melanoma , Durapatita/química , Durapatita/farmacología , Ácido Hialurónico/química , Ácido Hialurónico/farmacología , Hidrogeles/química , Hidrogeles/farmacología , Animales , Ratones , Melanoma/tratamiento farmacológico , Melanoma/patología , Melanoma/metabolismo , Línea Celular Tumoral , Humanos , Receptores de Hialuranos/metabolismo , Antineoplásicos/química , Antineoplásicos/farmacología , Nanopartículas/química , Células RAW 264.7RESUMEN
Proline 4-hydroxylase 2 (P4HA2) is known for its hydroxylase activity, primarily involved in hydroxylating collagen precursors and promoting collagen cross-linking under physiological conditions. Although its overexpression influences a wide variety of malignant tumors' occurrence and development, its specific effects and mechanisms in oral squamous cell carcinoma (OSCC) remain unclear. This study focused on investigating the expression patterns, carcinogenic functions, and underlying mechanisms of P4HA2 in OSCC cells. Various databases, including TCGA, TIMER, UALCAN, GEPIA, and K-M plotter, along with paraffin-embedded samples, were used to ascertain P4HA2 expression in cancer and its correlation with clinicopathological features. P4HA2 knockdown and overexpression cell models were developed to assess its oncogenic roles and mechanisms. The results indicated that P4HA2 was overexpressed in OSCC and inversely correlated with patient survival. Knockdown of P4HA2 suppressed invasion, migration, and proliferation of OSCC cells both in vitro and in vivo, whereas overexpression of P4HA2 had the opposite effects. Mechanistically, the phosphorylation levels of the PI3K/AKT pathway were reduced following P4HA2 silencing. The study reveals that P4HA2 acts as a promising biomarker for predicting prognosis in OSCC and significantly affects metastasis, invasion, and proliferation of OSCC cells through the regulation of the PI3K/AKT signaling pathway.
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Carcinoma de Células Escamosas , Movimiento Celular , Proliferación Celular , Neoplasias de la Boca , Invasividad Neoplásica , Fosfatidilinositol 3-Quinasas , Procolágeno-Prolina Dioxigenasa , Proteínas Proto-Oncogénicas c-akt , Transducción de Señal , Animales , Femenino , Humanos , Masculino , Ratones , Persona de Mediana Edad , Carcinoma de Células Escamosas/patología , Carcinoma de Células Escamosas/metabolismo , Carcinoma de Células Escamosas/genética , Línea Celular Tumoral , Movimiento Celular/genética , Regulación Neoplásica de la Expresión Génica , Ratones Desnudos , Neoplasias de la Boca/patología , Neoplasias de la Boca/metabolismo , Neoplasias de la Boca/genética , Metástasis de la Neoplasia , Fosfatidilinositol 3-Quinasas/metabolismo , Procolágeno-Prolina Dioxigenasa/metabolismo , Procolágeno-Prolina Dioxigenasa/genética , Proteínas Proto-Oncogénicas c-akt/metabolismoRESUMEN
Intermetallic compounds (IMCs) with ordered atomic structure have gained great attention as nanocatalysts for its enhanced activity and stability. Although the reliance of IMC preparation on high-temperature annealing is well known, a comprehensive understanding of the formation mechanisms of IMCs in this process is currently lacking. Here, we employ aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM) to track the formation process of IMCs on carbon supports during in-situ annealing, by taking PtFe as a case study within an industry-relevant impregnation synthesis framework. We directly discern five different stages at the atomic level: initial atomic precursors; Pt cluster formation; Pt-Fe disordered alloying; structurally ordered Pt3Fe formation, and final Pt3Fe-PtFe IMC conversion. In particular, we find that the crucial role of high-temperature annealing resides in facilitating the diffusion of Fe towards Pt, enabling the creation of alloys with the targeted stoichiometric ratio, which in turn provides the thermodynamic driving force for the disorder-to-order transition.
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Inversion symmetry broken 3R phase transition metal dichalcogenides (TMDs) show fascinating prospects in spintronics, valleytronics, and nonlinear optics. However, the controlled synthesis of 3R phase TMDs is still a great challenge. In this work, two-dimensional 3R-NbSe2 single crystals up to 0.2 mm were synthesized for the first time through chemical vapor deposition method by designing a space-confined system. The crystal size and morphology can be controlled by the location of the stacked substrates and the amount of the Nb2O5 precursor. Scanning transmission electron microscopy and Raman measurements reveal the NbSe2 exhibits a pure 3R stacking mode with relatively weak interlayer van der Waals interactions. Importantly, 3R-NbSe2 shows obvious second harmonic generation signal which intensity intensified as thickness increases. Density functional theory calculations and optical absorption demonstrate the coexistence of metallic and semiconducting optical properties of 3R-NbSe2. We designed a NbSe2/WS2/NbSe2 photodetector utilizing the metallicity of 3R-NbSe2, which shows good performance especially an ultrafast response (6-7 µs, 0.5 ms - 7.9 s for Au electrodes in literature). The proposed strategy and findings are of great significance for the growth of many other 3R-TMDs and applications of nonlinear optical and ultrafast devices.
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Due to the significance of atmospheric HONO as a reservoir for radicals and the presence of substantial unknown sources of HONO, there is a pressing need for accurate and consistent measurement of its concentration. In this study, we compared the measurements obtained from the monitor for aerosols and gases in ambient air (MARGA) based on wet chemical method with those from the incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) based on optical method to assess the suitability of the MARGA instrument for accurate HONO detection. The diurnal patterns obtained by the two instruments are similar, with peaks at 8 a.m. and lows at 5 p.m. Over the course of the observation period, it was often observed that HONO concentrations recorded by the MARGA instrument consistently exceeded those obtained through the IBBCEAS technique, accounting for approximately 91.33% of the total observation time. Throughout the entire observation period, the R2 value between the two instruments was 0.49, indicating relatively good correlation. However, with a slope of only 0.27, it suggests poor agreement between the two instruments. Furthermore, the R2 and slopes between the two instruments vary with the seasons and day-night. The larger the quartile values of NO2, NH3, and BC, the greater the slopes of both MARGA and IBBCEAS instruments, and the higher the concentrations of NO2, NH3, and BC (indicator of semivolatile oxidizable hydrocarbons), the greater the differences between the two instruments, all indicating that NH3 may promote the reaction of NO2 with semivolatile oxidizable hydrocarbons to produce HONO. The O3 with its strong oxidizing properties may cause underestimation in the MARGA instrument by oxidizing NO2- to NO3- in the absorbing solution. It is challenging to derive a universal correction formula due to the interference of various chemical substances. Hence, MARGA should not be used for HONO research in the future.