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Diamond is considered the most promising next-generation semiconductor material due to its excellent physical characteristics. It has been more than three decades since the discovery of a special structure named n-diamond. However, despite extensive efforts, its crystallographic structure and properties are still unclear. Here, we show that subdisordered structures in diamond provide an explanation for the structural feature of n-diamond. Monocrystalline diamond with subdisordered structures is synthesized via the chemical vapor deposition method. Atomic-resolution scanning transmission electron microscopy characterizations combined with the picometer-precision peak finder technology and diffraction simulations reveal that picometer-scale shifts of atoms within cells of diamond govern the subdisordered structures. First-principles calculations indicate that the bandgap of diamond decreases rapidly with increasing shifting distance, in accordance with experimental results. These findings clarify the crystallographic structure and electronic properties of n-diamond and provide new insights into the bandgap adjustment in diamond.
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Electrophoretic displays (EPDs) utilize the electrophoretic particles in electronic ink (e-ink) to display different color states with bistability. Bistability of EPDs is achieved by placing colloidal particles in a highly viscous solvent to keep the distribution of colloidal particles stable without sustaining the external field, so it only consumes power when updating the image. The feature of low power consumption makes it suitable for applications such as advertising boards, price tags, etc. Apart from these applications, recent research on lateral-driving EPDs extends its applications to smart windows, privacy control, and so on. However, achieving bistability by simply increasing the viscosity of solvent is inefficient in the case of lateral driving operation. Therefore, it is deserving to have intensive study on the mechanism of bistability from other aspects. Herein, we propose a mechanism to investigate the charge adsorption behavior on the electrode to affect the bistability of particles, which is based on the "Stern layer adsorption/desorption" model. Based on the above mechanism, we further fabricated a hexadecyl trimethylammonium bromide (CTAB)/poly(vinyl alcohol) (PVA) composite film on the electrode to improve the bistability of lateral-driving EPD by reducing the diffusion current caused by unabsorbed charges. This developed lateral-driving EPD can significantly improve the bistability, which is enhanced from 40 s to 7 min, an increase by a factor of approximately 10. This work gives a way to consider the bistability of colloidal particles in nonpolar solvent.
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To address the problem that complex bearing faults are coupled to each other, and the difficulty of diagnosis increases, an improved envelope spectrum-maximum second-order cyclostationary blind deconvolution (IES-CYCBD) method is proposed to realize the separation of vibration signal fault features. The improved envelope spectrum (IES) is obtained by integrating the part of the frequency axis containing resonance bands in the cyclic spectral coherence function. The resonant bands corresponding to different fault types are accurately located, and the IES with more prominent target characteristic frequency components are separated. Then, a simulation is carried out to prove the ability of this method, which can accurately separate and diagnose fault types under high noise and compound fault conditions. Finally, a compound bearing fault experiment with inner and outer ring faults is designed, and the inner and outer ring fault characteristics are successfully separated by the proposed IES-CYCBD method. Therefore, simulation and experiments demonstrate the strong capability of the proposed method for complex fault separation and diagnosis.
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As an ultra-wide bandgap semiconductor, hexagonal boron nitride (h-BN) has drawn great attention in solar-blind photodetection owing to its wide bandgap and high thermal conductivity. In this work, a metal-semiconductor-metal structural two-dimensional h-BN photodetector was fabricated by using mechanically exfoliated h-BN flakes. The device achieved an ultra-low dark current (16.4 fA), high rejection ratio (R205nm/R280nm= 235) and high detectivity up to 1.28 × 1011Jones at room temperature. Moreover, due to the wide bandgap and high thermal conductivity, the h-BN photodetector showed good thermal stability up to 300 °C, which is hard to realize for common semiconductor materials. The high detectivity and thermal stability of h-BN photodetector in this work showed the potential applications of h-BN photodetectors working in solar-blind region at high temperature.
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Manipulating catalytic active sites and reaction kinetics in alkaline media is crucial for rationally designing mighty water-splitting electrocatalysts with high efficiency. Herein, the coupling between oxygen vacancies and interface engineering is highlighted to fabricate a novel amorphous/crystalline CrOx -Ni3 N heterostructure grown on Ni foam for accelerating the alkaline hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Density functional theory (DFT) calculations reveal that the electron transfer from amorphous CrOx to Ni3 N at the interfaces, and the optimized Gibbs free energies of H2 O dissociation (ΔGH-OH ) and H adsorption (ΔGH ) in the amorphous/crystalline CrOx -Ni3 N heterostructure are conducive to the superior and stable HER activity. Experimental data confirm that numerous oxygen vacancies and amorphous/crystalline interfaces in the CrOx -Ni3 N catalysts are favorable for abundant accessible active sites and enhanced intrinsic activity, resulting in excellent catalytic performances for HER and OER. Additionally, the in situ reconstruction of CrOx -Ni3 N into highly active Ni3 N/Ni(OH)2 is responsible for the optimized OER performance in a long-term stability test. Eventually, an alkaline electrolyzer using CrOx -Ni3 N as both cathode and anode has a low cell voltage of 1.53 V at 10 mA cm-2 , together with extraordinary durability for 500 h, revealing its potential in industrial applications.
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It was interesting to experimentally find that the thermal insulation of silica aerogels was improved by doping graphene sheets with high heat conductivity. The underlying mechanism is investigated in the present work from the perspective of gas-solid interaction using a comprehensive analysis of molecular dynamics (MD) simulations, theoretical modeling, and experimental data. The MD-modeled small pores are demonstrated to effectively represent big pores in silica aerogels because of similar heat conduction physics, because it is found that adsorption does not contribute to gas heat conduction. Meanwhile, based on the experimentally measured density, the porous structures are schematically re-engineered using molecular modeling for the first time. The evaluated pore size distributions numerically present a consistency with available experimental data. Inspired by the visualization of the 3D pore structure, we proposed a graphene/silica/nitrogen model to evaluate the role of graphene in heat conduction: it can not only reduce effective gas collision (impede heat transport) but also enhance the gas-solid coupling effect. The former is dominant because of the high porosity, leading to an improvement in thermal insulation. The competition between them can be the reason for the "trade-off" phenomenon in the graphene doping effect in the available experiment.
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An efficient visible light photoredox catalyzed aerobic deprotection of 1,3-oxathiolanes using organic dye Eosin Y as a photocatalyst is disclosed. The deprotection procedure features the use of a metal-free catalyst, mild conditions, a broad range of substrate scope, and good functional group tolerance. 35 examples were tested under the standard conditions and most of them afforded the deprotected products in modest to high yields.
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The development of accurate, reliable devices for glucose detection has drawn much attention from the scientific community over the past few years. Here, we report a single-step method to fabricate Ni nanoparticle-modified graphene-diamond hybrid electrodes via a catalytic thermal treatment, by which the graphene layers are directly grown on the diamond surface using Ni thin film as a catalyst, meanwhile, Ni nanoparticles are formed in situ on the graphene surface due to dewetting behavior. The good interface between the Ni nanoparticles and the graphene guarantees efficient charge transfer during electrochemical detection. The fabricated electrodes exhibit good glucose sensing performance with a low detection limit of 2 µM and a linear detection range between 2 µM-1 mM. In addition, this sensor shows great selectivity, suggesting potential applications for sensitive and accurate monitoring of glucose in human blood.
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Técnicas Eletroquímicas/instrumentação , Eletrodos , Glucose/análise , Nanopartículas Metálicas/química , Níquel/química , Catálise , Diamante/química , Técnicas Eletroquímicas/métodos , Grafite/química , Limite de Detecção , Oxirredução , Espectroscopia Fotoeletrônica , Sensibilidade e Especificidade , Análise Espectral RamanRESUMO
Described herein is an organocatalytic enantioselective desymmetrizing cycloisomerization of arylsulfonyl-protected ynamide cyclohexanones, representing the first metal-free asymmetric Conia-ene-type carbocyclization. This method allows the highly efficient and atom-economical construction of a range of valuable morphans with wide substrate scope and excellent enantioselectivity (up to 97 % ee). In addition, such a cycloisomerization of alkylsulfonyl-protected ynamide cyclohexanones can lead to the divergent synthesis of normorphans as the main products with high enantioselectivity (up to 90 % ee). Moreover, theoretical calculations are employed to elucidate the origins of regioselectivity and enantioselectivity.
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The second near-infrared window emission (1.0-1.7 µm, NIR-II) has received extensive attention with the advantages of negligible tissue scattering, reduced autofluorescence, and less background noise. Here a novel analysis platform based on quantum dots (QDs) for highly selective detection of Zn2+ and Cd2+ with an enhanced NIR-II fluorescence is reported for the first time. We have developed a facile two-step route to synthesize the water-soluble Ag2S QDs, constituting of a green hydrothermal process and followed surface ligands exchange. Surface passivation was proposed to be the mechanism for the enhanced fluorescence. The added Zn2+ or Cd2+ could react with the surface thioglycollic acid to form Zn-thiol or Cd-thiol complex passivation shell, which restored surface defects and suppressed nonradiative recombination pathway. The detection platform exhibited a linear relationship between the ion concentrations and enhanced fluorescence and had a detection limit as low as 760 nM for Zn2+ and 546 nM for Cd2+ at pH = 7.4. Furthermore, the as-synthesized Ag2S QDs showed good robustness in real sample matrix and were demonstrated to be able to detect exogenous Zn(II) in cells. These properties suggest potential applications of detection of Zn2+ in biology and Cd2+ in environment via the NIR-II fluorescent Ag2S QDs.
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UNLABELLED: Hepatocellular carcinoma (HCC) is one of the most lethal cancers worldwide because of metastasis. Epithelial-mesenchymal transition (EMT) is widely considered to be crucial to the invasion-metastasis cascade during cancer progression. Actin-like 6A (ACTL6A) is initially verified important for cell proliferation, differentiation, and migration. In this study, we find that ACTL6A plays an essential role in metastasis and EMT of HCC. ACTL6A expression is up-regulated in HCC cells and tissues. A high level of ACTL6A in HCCs is correlated with aggressive clinicopathological features and is an independent poor prognostic factor for overall and disease-free survival of HCC patients. Ectopic expression of ACTL6A markedly promotes HCC cells migration, invasion, as well as EMT in vitro and promotes tumor growth and metastasis in the mouse xenograft model. Opposite results are observed when ACTL6A is knocked down. Mechanistically, ACTL6A promotes metastasis and EMT through activating Notch signaling. ACTL6A knockdown has the equal blockage effect as the Notch signaling inhibitor, N-[N-(3,5-difluorophenacetyl)-L-alanyl]-S-phenylglycine t-butylester, in HCC cells. Further studies indicate that ACTL6A might manipulate SRY (sex determining region Y)-box 2 (SOX2) expression and then activate Notch1 signaling. CONCLUSIONS: ACTL6A promotes metastasis and EMT by SOX2/Notch1 signaling, indicating a prognostic biomarker candidate and a potential therapeutic target for HCC.
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Actinas/genética , Carcinoma Hepatocelular/genética , Proteínas Cromossômicas não Histona/genética , Proteínas de Ligação a DNA/genética , Transição Epitelial-Mesenquimal/genética , Regulação Neoplásica da Expressão Gênica , Neoplasias Hepáticas/genética , Adulto , Idoso , Análise de Variância , Animais , Biópsia por Agulha , Carcinoma Hepatocelular/mortalidade , Carcinoma Hepatocelular/patologia , Modelos Animais de Doenças , Feminino , Humanos , Imuno-Histoquímica , Neoplasias Hepáticas/mortalidade , Neoplasias Hepáticas/patologia , Masculino , Camundongos , Pessoa de Meia-Idade , Análise Multivariada , Invasividade Neoplásica/patologia , Metástase Neoplásica/genética , Valor Preditivo dos Testes , Prognóstico , Distribuição Aleatória , Análise de Sobrevida , Ativação Transcricional , Células Tumorais Cultivadas , Regulação para CimaRESUMO
The expression level of tumor-related mRNA can reveal significant information about tumor progression and prognosis, so specific mRNA in cells provides an important approach for biological and disease studies. Here, fluorescence lifetime imaging of nanoflares in living cells was first employed to detect specific intracellular mRNA. We characterized the lifetime changes of the prepared nanoflares before and after the treatment of target mRNA and also compared the results with those of fluorescence intensity-based measurements both intracellularly and extracellularly. The nanoflares released the cy5-modified oligonucleotides and bound to the targets, resulting in a fluorescence lifetime lengthening. This work puts forward another dimension of detecting specific mRNA in cells and can also open new ways for detection of many other biomolecules.
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Microscopia de Fluorescência , Nanoestruturas/química , RNA Mensageiro/análise , Proteína BRCA1/antagonistas & inibidores , Proteína BRCA1/genética , Proteína BRCA1/metabolismo , Carbocianinas/química , Linhagem Celular Tumoral , Corantes Fluorescentes/química , Humanos , Oligonucleotídeos/química , Oligonucleotídeos/metabolismo , RNA Interferente Pequeno/química , RNA Interferente Pequeno/metabolismoRESUMO
In the presented paper we investigated a 2-pyridylthiazole derivative, 4-phenyl-2-(2-pyridyl)thiazole (2-PTP), as the molecular fluorescent switches. It was firstly found that 2-PTP could perform a "turn-on" fluorescent sensing for Fe(III) with selectivity and reversibility. A 2:1 stoichiometry between 2-PTP and Fe(III) was determined according to the molar ratio method. The binding constant was evaluated as (1.90 ± 0.05) × 10(5) (L/mol)(2). The detection limit was found as 2.2 × 10(-7) M (S/N = 3). Secondly, 2-PTP also exhibited a pH-dependent dual-emission. The pK a(2-PTP-H(+)/2-PTP) value was then estimated as 2.0. To explain the identical emission at 479 nm of both the Fe(III) coordinated form and the protonated form of the ligand, we proposed a "locked" conformation. Finally, combining the two external stimuli as inputs, an OR logic gate was constructed using the fluorescent emission at 479 nm as the output channel.
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A new fluorophore, 4-methyl-2-(2-pyridyl)-5-(2-thiophenyl)thiazole (2-PTT), was reported as a ratiometically fluorescent sensor of zinc(II) based on dual-emission with selectivity and sensitivity. Two emission bands at 440 and 497 nm were observed before and after addition of zinc(II), respectively. Job's plot disclosed the 1:1 stoichiometry between 2-PTT and zinc(II). The binding constant was evaluated as 2.09 × 10(5) M(-1) based on fluorescence titration experiment.
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The bandgap modulation and electronic properties modulation of two-dimensional HfSi2N4 monolayer induced by strain, electric field and atomic adsorption are studied by first principles. The HfSi2N4 monolayer was found to be dynamically, thermally, and mechanically stable at equilibrium, and it is a direct semiconductor with a bandgap of 1.87 eV. The bandgap of the HfSi2N4 monolayer can be precisely modulated by strain. Under the action of strain, HfSi2N4 monolayer not only transforms from direct semiconductor to indirect semiconductor, but also improves the absorption of visible light. An external electric field in the 0-0.5 eV/Å range can also modulate the bandgap of HfSi2N4 monolayer from 1.87 eV to 0 eV, and most importantly, at an external electric field of 0.5 eV/Å, HfSi2N4 monolayer shows the characteristics of spin gapless semiconductor. The calculated adsorption energy shows that the structures of H, O and F atoms adsorbed by HfSi2N4 monolayer can all exist stably. The bandgap of the configuration after adsorption of O and F atoms is significantly reduced compared with that of HfSi2N4 monolayer. Furthermore, the HfSi2N4 monolayer after adsorption of H and F atoms is transformed into a magnetic semiconductor. METHOD: All calculations were performed using Vienna ab initial simulation package, The electronic structure, mechanical properties, electronic properties and other properties were carried out using generalized gradient approximation (GGA-PBE), supplemented by HSE06 and GGA + U. The total-energy and force convergence are less than 10-6 eV and 0.001 eV/Å, respectively. The vacuum on the z-axis is selected 20 Å. The vdW interactions were corrected using the Grimme scheme (DFT-D3).
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Li dendrite and the shuttle effect are the two primary hindrances to the commercial application of lithium-sulfur batteries (LSBs). Here, a multifunctional separator has been fabricated via successively coating carbon nanotubes (CNTs) and lithium phytate (LP) onto a commercial polypropylene (PP) separator to improve the performance of LSBs. The LP coating layer with abundant electronegative phosphate group as permselective ion sieve not only reduces the polysulfide shuttle but also facilitates uniform Li+ flux through the PP separator. And the highly conductive CNTs on the second layer act as a second collector to accelerate the reversible conversion of sulfide species. The synergistic effect of LP and CNTs further increases the electrolyte wettability and reaction kinetics of cells with a modified separator and suppresses the shuttle effect and growth of Li dendrite. Consequently, the LSBs present much enhanced rate performance and cyclic performance. It is expected that this study may generate an executable tactic for interface engineering of separator to accelerate the industrial application process of LSBs.
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Cytokinesis is required for faithful division of cytoplasmic components and duplicated nuclei into two daughter cells. Midbody, a protein-dense organelle that forms at the intercellular bridge, is indispensable for successful cytokinesis. However, the regulatory mechanism of cytokinesis at the midbody still remains elusive. Here, we unveil a critical role for NudC-like protein 2 (NudCL2), a co-chaperone of heat shock protein 90 (Hsp90), in cytokinesis regulation by stabilizing regulator of chromosome condensation 2 (RCC2) at the midbody in mammalian cells. NudCL2 localizes at the midbody, and its downregulation results in cytokinesis failure, multinucleation and midbody disorganization. Using iTRAQ-based quantitative proteomic analysis, we find that RCC2 levels are decreased in NudCL2 knockout (KO) cells. Moreover, Hsp90 forms a complex with NudCL2 to stabilize RCC2, which is essential for cytokinesis. RCC2 depletion mirrors phenotypes observed in NudCL2-downregulated cells. Importantly, ectopic expression of RCC2 rescues the cytokinesis defects induced by NudCL2 deletion, but not vice versa. Together, our data reveal the significance of the NudCL2/Hsp90/RCC2 pathway in cytokinesis at the midbody.
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In order to fabricate a novel antioxidant nanofiber facial mask, a metal cone modified in-situ electrospinning with precise deposition was employed by utilizing Enteromorpha prolifera polysaccharides (EPPs). The metal cone could control the deposition area to achieve precise fabrication of facial mask on skin. The EPPs exhibited remarkable antioxidant ability, as evidenced by the half-maximal inhibitory concentrations (IC50) of 1.44 mg/mL and 0.74 mg/mL against DPPH and HO⢠free radicals, respectively. The antioxidant ability of the facial mask was improved by elevating the electrospinning voltage from 15 kV to 19 kV, due to the improved release capacity of EPPs by 7.09 %. Moreover, the facial mask demonstrated robust skin adhesion and moisture-retaining properties compared with commercial facial mask, which was benefited by the in-situ electrospinning technology. Furthermore, cytotoxicity assay, animal skin irritation test, and ocular irritation test collectively affirmed the safety of the facial mask. Thus, this research introduces a novel in situ electrospinning with precise deposition method and a natural antioxidant additive for preparing facial mask.
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Algas Comestíveis , Nanofibras , Ulva , Animais , Antioxidantes/farmacologia , Ulva/química , Polissacarídeos/farmacologia , Polissacarídeos/químicaRESUMO
Due to their high wavelength selectivity and strong anti-interference capability, solar-blind UV photodetectors hold broad and important application prospects in fields like flame detection, missile warnings, and secure communication. Research on solar-blind UV detectors for amorphous Ga2O3 is still in its early stages. The presence of intrinsic defects related to oxygen vacancies significantly affects the photodetection performance of amorphous Ga2O3 materials. This paper focuses on growing high quality amorphous Ga2O3 films on silicon substrates through atomic layer deposition. The study investigates the impact of annealing atmospheres on Ga2O3 films and designs a blind UV detector for Ga2O3. Characterization techniques including atomic force microscopy (AFM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) are used for Ga2O3 film analysis. Ga2O3 films exhibit a clear transition from amorphous to polycrystalline after annealing, accompanied by a decrease in oxygen vacancy concentration from 21.26% to 6.54%. As a result, the response time of the annealed detector reduces from 9.32 s to 0.47 s at an external bias of 10 V. This work demonstrates that an appropriate annealing process can yield high-quality Ga2O3 films, and holds potential for advancing high-performance solar blind photodetector (SBPD) development.
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African swine fever virus (ASFV) is a large double-stranded DNA virus with a complex structural architecture and encodes more than 150 proteins, where many are with unknown functions. E184L has been reported as one of the immunogenic ASFV proteins that may contribute to ASFV pathogenesis and immune evasion. However, the antigenic epitopes of E184L are not yet characterized. In this study, recombinant E184L protein was expressed in prokaryotic expression system and four monoclonal antibodies (mAbs), designated as 1A10, 2D2, 3H6, and 4C10 were generated. All four mAbs reacted specifically with ASFV infected cells. To identify the epitopes of the mAbs, a series of overlapped peptides of E184L were designed and expressed as maltose binding fusion proteins. Accordingly, the expressed fusion proteins were probed with each E184L mAb separately by using Western blot. Following a fine mapping, the minimal linear epitope recognized by mAb 1A10 was identified as 119IQRQGFL125, and mAbs 2D2, 3H6, and 4C10 recognized a region located between 153DPTEFF158. Alignment of amino acids of E184L revealed that the two linear epitopes are highly conserved among different ASFV isolates. Furthermore, the potential application of the two epitopes in ASFV diagnosis was assessed through epitope-based ELISA using 24 ASFV positive and 18 negative pig serum and the method were able to distinguish positive and negative samples, indicating the two epitopes are dominant antigenic sites. To our knowledge, this is the first study to characterize the B cell epitopes of the antigenic E184L protein of ASFV, offering valuable tools for future research, as well as laying a foundation for serological diagnosis and epitope-based marker vaccine development.