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Low-temperature operation poses a significant challenge for current commercial rechargeable lithium-ion batteries (LIBs). Organic polymer electrode materials, exhibiting a nonintercalation redox mechanism, offer a viable solution to mitigate the decline in electrochemical performance at low temperatures in LIBs. Herein, a radical polymer P(DATPAPO-TPA) with a conjugated nitrogen-rich triphenylamine derivative as the backbone and high-density nitroxide pendants has been synthesized. Due to the large interstitial spaces between adjacent structural units and polymer chains, resulting from the significant torsion angle between the benzene rings in the P(DATPAPO-TPA) skeleton, ions could effectively transport. This structural feature demonstrated a notable discharge capacity of 143.3 mA h·g-1 and a high charge-discharge plateau at â¼3.75 V vs Li+/Li, outperforming most reported radical polymer cathode materials. In addition, its capacity retention could reach 83.1% after 2000 cycles at an ultrahigh current density of 50 C, showing excellent rate capability and promising cyclability. Also notable was P(DATPAPO-TPA)'s favorable low-temperature performance that maintains a high discharge capacity of 139.2 mA h·g-1 at 0 °C. The synthesized P(DATPAPO-TPA) is a tangible illustration of a viable design strategy for low-temperature electrode materials, thereby contributing to broadening applications for radical polymer electrode materials.
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Autoimmune skin disease is a kind of heterogeneous disease with complicated pathogenesis. Many factors such as genetic, infectious, environmental and even psychological factors may interact together to trigger a synergistic effect for the development of abnormal innate and adaptive immune responses. Although the exact mechanisms remain unclear, recent evidence suggests that pyroptosis plays a pivotal role in the development of autoimmune skin disease. The feature of pyroptosis is the first formation of pores in cellular membranes, then cell rupture and the release of intracellular substances and pro-inflammatory cytokines, such as interleukin-1 beta (IL-1ß) and IL-18. This hyperactive inflammatory programmed cell death damages the homeostasis of the immune system and advances autoimmunity. This review briefly summarises the molecular regulatory mechanisms of pyrin domain-containing protein 3 (NLRP3) inflammasome and gasdermin family, as well as the molecular mechanisms of pyroptosis, highlights the latest progress of pyroptosis in autoimmune skin disease, including systemic lupus erythematosus, psoriasis, atopic dermatitis and systemic scleroderma and attempts to identify its potential advantages as a therapeutic target or prognostic biomarker for these diseases.
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Doenças Autoimunes , Inflamassomos , Proteína 3 que Contém Domínio de Pirina da Família NLR , Piroptose , Humanos , Doenças Autoimunes/imunologia , Doenças Autoimunes/metabolismo , Inflamassomos/metabolismo , Proteína 3 que Contém Domínio de Pirina da Família NLR/metabolismo , Dermatopatias/imunologia , Animais , Proteínas de Ligação a Fosfato/metabolismo , Interleucina-1beta/metabolismo , Escleroderma Sistêmico/imunologia , Lúpus Eritematoso Sistêmico/imunologia , Peptídeos e Proteínas de Sinalização Intracelular/metabolismo , Psoríase/imunologia , Psoríase/metabolismo , Autoimunidade , Interleucina-18/metabolismo , Dermatite Atópica/imunologiaRESUMO
BACKGROUND: Psoriasis is a prevalent chronic inflammatory dermatosis characterized by excessive proliferation of keratinocytes. Protein lysine 2-hydroxyisobutyrylation (Khib) is a newly identified post-translational modification that regulates various biological processes. Abnormal Khib modification has been closely associated with the development of autoimmune diseases. OBJECTIVE: To investigate the abnormal Khib profile and its pathogenic role in psoriasis. METHODS: We utilized liquid chromatography-tandem mass spectrometry to analyze Khib-modified proteins in the epidermis of psoriasis and healthy controls. Mutated cells and mice with downregulated Ebp1Khib210 were generated to investigate its functional effects in psoriasis. RESULTS: The omic analysis revealed dysregulation of Khib modification in psoriatic lesions, exhibiting a distinct profile compared to controls. We observed the downregulation of Ebp1Khib210 in psoriatic lesions and IMQ-induced psoriatic mice. Notably, the expression of Ebp1Khib210 was upregulated in psoriatic patients following effective treatment. Decreased Ebp1Khib210 enhanced keratinocyte viability, proliferation, and survival while inhibiting apoptosis in vitro. Additionally, Pa2g4K210A mice with downregulated Ebp1Khib210 exhibited more severe psoriatic lesions and enhanced keratinocyte proliferation. Moreover, we found that Ebp1K210A mutation increased the interaction between Ebp1 and nuclear Akt, thereby inhibiting MDM2-mediated TIF-IA ubiquitination, and resulting to increased rRNA synthesis and keratinocyte proliferation. The downregulation of Ebp1Khib210 was attributed to inflammation-induced increases in HDAC2 expression. CONCLUSION: Our findings demonstrate that downregulation of Ebp1Khib210 promotes keratinocyte proliferation through modulation of Akt signaling and TIF-IA-mediated rRNA synthesis. These insights into Khib modification provide a better understanding of the pathogenesis of psoriasis and suggest potential therapeutic targets.
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We investigated the factors influencing the progression of the pandemic from a global perspective by using the Geodetector and Correlation methods and explored the pandemic response policies and effects in different countries. The results yielded three notable findings. First, empirical results show the COVID-19 pandemic is influenced by various factors, including demographic and economic parameters, international travelers, urbanization ratio, urban population, etc. Among them, the correlation between urban population and confirmed cases is strongest. Cities become the key factor affecting the COVID-19 pandemic, with high urbanization levels and population mobility increases the risk of large-scale outbreaks. Second, among control measures, School-closures, International-travel-restrictions, and Public-gathering-restriction have the best control effect on the epidemic. In addition, the combination of different types of control measures is more effective in controlling the outbreak, especially for Public-gathering-restrictions â© School-closures, International-travel-restrictions â© Workplace-closures, Public-transport-restrictions â© International-travel-restrictions. Third, implementing appropriate control measures in the first month of an outbreak played a critical role in future pandemic trends. Since there are few local cases in this period and the control measures have an obvious effect.
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Cubic Pd nanocrystals (CPNCs) as one of typical nanostructures are generally fabricated using I- or Br- as capping ions. However, which ion, I- or Br-, exclusively mediates the growth of CPNCs in a given reaction system is not well understood. Herein, regardless of I- or Br- as the capping ion, we successfully achieved CPNCs in the same reaction system simply by adjusting the pH. Based on the Finke-Watzky kinetic model, an increase in pH accelerates the overall reduction rate of Pd2+, and the formation of CPNCs only occurs over the range of specific solution reduction rate constants (k1). This kinetically illuminates that the reduction rate of Pd2+ is the physicochemical parameter that determines which ion, I- or Br-, dictates the growth of CPNCs. Also, density functional theory (DFT) calculations further elucidate the dependence of the reduction rate of Pd2+ on pH and the configuration of the activated Pd2+ complex.
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In addition to electrically driven organic light-emitting diode (OLED) displays that rely on complicated and costly circuits for switching individual pixel illumination, developing a facile approach that structures pixel-free light-emitting displays with exceptional precision and spatial resolution via external photo-modulation holds significant importance for advancing consumer electronics. Here, optically switchable organic light-emitting pixel-free displays (OSPFDs) are presented and fabricated by judiciously combining an adaptive photosensitive ionic polymer as electron transport materials (ETM) with external photo-modulation as the switching mode while ensuring superior illumination performance and seamless imaging capability. By irradiating the solution-processed OSPFDs with light at specific wavelengths, efficient and reversible tuning of both electron transport and electroluminescence is achieved simultaneously. This remarkable control is achieved by altering the energetic matching within OSPFDs, which also exhibits a high level of universality and adjustable flexibility in the three primary color-based light-emitting displays. Moreover, the ease of creating and erasing desired pixel-free emitting patterns through a non-invasive photopatterning process within a single OSPFD is demonstrated, thereby rendering this approach promising for commercial displaying devices and highly precise pixelated illuminants.
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Contrastive learning (CL) has emerged as a powerful approach for self-supervised learning. However, it suffers from sampling bias, which hinders its performance. While the mainstream solutions, hard negative mining (HNM) and supervised CL (SCL), have been proposed to mitigate this critical issue, they do not effectively address graph CL (GCL). To address it, we propose graph positive sampling (GPS) and three contrastive objectives. The former is a novel learning paradigm designed to leverage the inherent properties of graphs for improved GCL models, which utilizes four complementary similarity measurements, including node centrality, topological distance, neighborhood overlapping, and semantic distance, to select positive counterparts for each node. Notably, GPS operates without relying on true labels and enables preprocessing applications. The latter aims to fuse positive samples and enhance representative selection in the semantic space. We release three node-level models with GPS and conduct extensive experiments on public datasets. The results demonstrate the superiority of GPS over state-of-the-art (SOTA) baselines and debiasing methods. In addition, the GPS has also been proven to be versatile, adaptive, and flexible.
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Harnessing the spontaneous surface instability of pliable substances to create intricate, well-ordered, and on-demand controlled surface patterns holds great potential for advancing applications in optical, electrical, and biological processes. However, the current limitations stem from challenges in modulating multidirectional stress fields and diverse boundary environments. Herein, this work proposes a universal strategy to achieve arbitrarily controllable wrinkle patterns via the spatiotemporal photochemical boundaries. Utilizing constraints and inductive effects of the photochemical boundaries, the multiple coupling relationship is accomplished among the light fields, stress fields, and morphology of wrinkles in photosensitive polyurethane (PSPU) film. Moreover, employing sequential light-irradiation with photomask enables the attainment of a diverse array of controllable patterns, ranging from highly ordered 2D patterns to periodic or intricate designs. The fundamental mechanics of underlying buckling and the formation of surface features are comprehensively elucidated through theoretical stimulation and finite element analysis. The results reveal the evolution laws of wrinkles under photochemical boundaries and represent a new effective toolkit for fabricating intricate and captivating patterns in single-layer films.
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Protective materials are essential for personal, electronic, and military defenses owing to their efficient impact-resistant and energy-absorbing properties. Inspired by the bottom-up fabrication process and energy dissipation mechanism of natural organisms with hierarchical structures, we demonstrated a self-wrinkled photo-curing coating as a new protective material for enhancing the anti-impact property of the substrates. Owing to the self-assembly of polydimethylsiloxane (PDMS) containing polymeric photoinitiator on the surface, the liquid coating formulation was photo-cured by one-step UV irradiation with simultaneous generation of self-wrinkled surface morphology and a gradient cross-linked architecture. The maximum impact resistance height (hmax) of the glass substrate coated with plain coating increased from 120 to 180 cm when coated with wrinkled gradient coating. Furthermore, the Young's modulus, fracture stress, and toughness of the wrinkled gradient coating film improved from 39.6 MPa, 2.4 MPa, and 74.1 MJ/cm3 to 235.0 MPa (â¼5× increase), 18.5 MPa (â¼6.6× increase), and 845.0 MJ/cm3 (â¼10.8× increase) compared to the pure coating film as reference. The theoretical simulation and experimental results proved that the surface self-wrinkled morphology and intrinsic hierarchical architecture contribute to the energy dissipation and impact resistance of the cured coating. The photo-curing process, a bottom-up strategy, is conducted in a non-contact mode compared with nano-printing and lithography, enabling bulk materials to be engineered.
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Micropatterning various ion-based modality materials offers compelling advantages for functionality enhancement in iontronic pressure sensing, piezoionic mechanoreception, and skin-interfaced electrode adhesion. However, most existing patterning techniques for iontronic materials suffer from low flexibility and limited modulation capability. Herein, we propose a facile and robust method to fabricate hierarchical and asymmetrical iontronic micropatterns (denoted as HAIMs) through programmed regulation of the internal stress distribution and the local ionic migration among an iontronic host. The resultant HAIMs with arbitrarily regulated morphologies and region-dependent ionic electrical performance can be readily made via localized photodimerization of an anthracene-functionalized ionic liquid copolymer (denoted as An-PIL) and subsequent vapor oxidative polymerization of 3,4-ethylenedioxythiophene (EDOT). Based on the piezoionic effect within the resultant distinct doped PEDOT, HAIMs can serve as a scalable iontronic potential generator. Successful syntheses of these fascinating micropatterns may accelerate the development of patterned iontronic materials in a flexible, programmable, and functionally adaptive form.
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Líquidos Iônicos , Polímeros , PolimerizaçãoRESUMO
Recently, the problem of water pollution, caused by antibiotics, is becoming more and more serious. Photocatalysis is one of the promising technologies for removing antibiotics from water. Herein, the In2.77S4/Ti3C2 composites were prepared by an in-situ hydrothermal growth method for photocatalytic degradation of tetracycline (TC). The as-developed composites were characterized by various methods. The UV-Vis DRS spectra reveals that the introduction of Ti3C2 makes the bandgap of the as-prepared composites smaller and the visible light absorption ability improved. The photocatalytic degradation efficiency of the as-prepared composite is enhanced under visible light illumination. It is shown as first increasing and then decreasing with increasing the content of Ti3C2 in the composite and reaches to the maximum of 89.3% in 90 min, which is higher than 75.1% of In2.77S4 and 6.7% of Ti3C2. The reason of improvement is the interface between In2.77S4 and Ti3C2 is tightly combined to form a heterojunction. Moreover, the photocurrent intensity of the as-obtained composite is improved, while its Nyquist arc radius is decreased. In addition, holes are the main active species and ·OH and ·O2 - play an auxiliary role during the degradation of TC.
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Polyester fabric (PET fabric) has aroused widespread attention from people thanks to the advantages of smooth feel, easy washing, quick-drying, high strength, and chemical resistance. However, PET fabric's wide application has been limited by its hydrophobicity, poor resistance to bacterial contamination, and static accumulation. Herein, a super-hydrophilic PET fabric was achieved via a spray-drying layer-by-layer self-assembly method for comfortable garment manufacturing. The as-prepared PET fabric exhibited good superhydrophilicity, excellent antistatic property, and durable antibacterial performance. Moreover, the water contact angle of the treated fabric decreased to 0° from 121° of the original PET fabric, and the capillary height also increased from 7.1 cm to 21.4 cm. Besides, the treated fabric showed a durable antibacterial rate of 99.5% against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) after ten standard washing cycles. The prepared fabric was also identified with good cytocompatibility, making it a good material for garments in real life. Promisingly, this novel approach can be easily integrated into the finishing of textiles and is expected to be applied to various substrates with superhydrophilic and antibacterial properties.
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Poliésteres , Staphylococcus aureus , Têxteis , Antibacterianos/farmacologia , Escherichia coli , HumanosRESUMO
Ultrasensitive and ultraprecise detection of toxic target molecules is highly desirable for monitoring water pollution and improving human safety. Herein, a novel formaldehyde (HCHO) responsive ionic microchannel was successfully fabricated through constructing ethylenediamine (EDA)-functionalized poly(ionic liquid)/polyacrylonitrile nanofibrous membrane (PIL/PAN NFM). By employing the reactivity of HCHO with EDA immobilized on the prepared ionic nanofibrous membrane, the resultant ionic current output can switch from low to high because of the electron affinity increase and zeta potential decrease of the microchannels when reacting with more HCHO. Meanwhile, benefiting from the poly(ionic liquid) backbones in the designed ionic microchannels, the ions in electrolyte were greatly enriched in the channels and facilitating more ion transport paths formed along with the ionic nanofibers, therefore amplifying the detected ionic current signals. On the basis of the ionic current amplification mechanism, it is further used to detect a trace of HCHO in an aqueous solution. Finally, the ionic microchannels exhibited high sensitivity for the determination of HCHO ranging from 360 ppm (3.6 × 102 mg/L) to 0.036 ppt (3.6 × 10-8 mg/L) (R2 = 0.93) through an established linear correlation between responsive ionic current and HCHO concentrations. Furthermore, the ionic microchannels can remove a large number of HCHO molecules from an aqueous solution due to the abundant amino grafted on the membrane. In a sum, this work paves a promising way toward the design of artificial microchannels for various harmful compounds' detection.
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Wasted wool fabrics are a kind of textile waste source and the upcycle of them can not only benefit the environmental protection, but also turn waste into treasure by developing other potential applications. In this work, ionic liquid (IL) 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) was used as a green solvent to upcycle wasted wool fabrics into a wool keratin (WK)/IL/polyacrylonitrile (PAN) composite nanofibrous membrane with good antibacterial and high moisture permeability through electrospinning. The morphology and structure of the regenerated nanofibrous membrane were characterized by Scanning Electronic Microscopy (SEM), Energy Dispersive Spectrometer (EDS), Fourier Transfer Infrared Spectroscopy (FTIR). The antibacterial test demonstrates that it has 89.21% inhibition rate against E. coli, and 60.70% against S. aureus. Furthermore, the keratin containing in the membrane can effectively improve the hydrophilic property of it, as Moisture Management Test (MMT) indicates that it performs an excellent wetting performance and water transport property. In addition, IL is supposed to be recycled from the composite membrane through immersing in distilled water, which makes the fabrication process green and sustainable.
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Nanofibras , Animais , Antibacterianos , Escherichia coli , Permeabilidade , Staphylococcus aureus , Têxteis , Fibra de LãRESUMO
Real-life wearable electronics with long-term stable sensing performance are of significant practical interest to public. Wearable pressure sensors with washable, comfortable, breathable, and stable sensing ability are a key requirement to meet the desire. However, effects of ubiquitous ambient moisture and intrinsic defects of current capacitive sensing materials are two factors leading to unstable sensing performance of current pressure sensors. Existing ionic liquid-based materials (i.e., ionic hydrogel, ionic film, or ionic/elastomers composite) have been used for efficient capacitive pressure sensing but are highly sensitive and especially affected by moisture. In this work, we introduce a washable capacitive pressure-sensing textile based on the use of a hydrophobic poly(ionic liquid) nanofibrous membrane (PILNM) with good mechanical properties and satisfactory moisture proof sensing performance. The PILNM membranes possessing rich ions and microporous structures are novel ideal polymeric dielectric materials for amplification of signals with negligible stimulations. Moreover, the PILNMs exhibit very high stable sensing signals under moisture interference (up to 70% relative humidity) and repeated washings (more than 10 washings), especially suitable for wearable electronics. Notably, the PILNM-based wearable pressure-sensing textiles offer high sensitivity for low pressure and bent chord length changes with a low-pressure detection limit even under harsh deformations. Owing to the superior performance, the PILNM-based wearable pressure-sensing textiles are comfortable to wear and suitable for monitoring different human motions and pulse vibrations at various body positions. Meanwhile, the assembled multiple wearable pressure-sensing array can spatially map the contact area of the pressure stimuli and synchronously reflect finger movements.
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Líquidos Iônicos/química , Nanofibras/química , Pressão , Dispositivos Eletrônicos Vestíveis , Elastômeros/química , Humanos , Membranas Artificiais , Polímeros/química , TêxteisRESUMO
Integration of 1D, core/shell, and jagged features into one entity may provide a promising avenue for further enhancing catalyst performance. However, designing such unique nanostructures is extremely challenging. Herein, 1D serrated Au/Pd core/shell nanowires (CSNWs) with jagged edges were produced simply by a one-pot, dual-capping-agent-assisted method involving co-reduction, galvanic replacement, directional coalescence of preformed nanoparticles, and site-selective epitaxial growth of Pd. Au/PdCSNWs, compared with the commercially available Pd/C, exhibited enhanced electrocatalytic performance towards liquid fuel oxidation because of the synergistic effect of the electronic structure and low-coordinated jagged edges.
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Nanofios/química , Petróleo , Catálise , Elétrons , Ouro , Oxirredução , PaládioRESUMO
Three-dimensional (3D) cubic superstructures of PtPd nanocubes were achieved by spontaneous adjustment of PtIV reduction kinetics, and exhibited enhanced catalytic activity and long-term durability towards methanol oxidation compared with the state-of-the-art Pt/C. This work demonstrates the first example of designing 3D shaped architectures of PtPd nanocubes for methanol electrooxidation.