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Lithium metal batteries (LMBs) with LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes have garnered significant interest as next-generation energy storage devices due to their high energy density. However, the instability of their electrode/electrolyte interfaces in regular carbonate electrolytes (RCEs) results in a rapid capacity decay. To address this, a colloid electrolyte consisting of Li3P nanoparticles uniformly dispersed in the RCE is developed by a one-step synthesis. This design concurrently creates stable cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) on both electrode surfaces. The cathode interface derived from this colloid electrolyte significantly facilitates the decomposition of Li salts (LiPF6 and LiDFOB) on the cathode surface by weakening the P-F and B-F bonds. This in situ formed P/LiF-rich CEI effectively protects the NCM811 cathode from side reactions. Furthermore, the Li3P embedded in the SEI optimizes and homogenizes the Li-ion transport, enabling dendrite-free Li deposition. Compared to the RCE, the designed colloid electrolyte enables robust cathode and anode interfaces in NCM811||Li full cells, minimizing gas and dendrite formation, and delivering a superior capacity retention of 82% over 120 cycles at a 4.7 V cutoff voltage. This approach offers different insights into electrolyte regulation and explores alternative electrolyte shapes and formulations.
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Background: The most effective approach to managing Alzheimer's disease (AD) lies in identifying reliable biomarkers for AD to forecast the disease in advance, followed by timely early intervention for patients. Methods: Transcriptomic data on peripheral blood mononuclear cells (PBMCs) from patients with AD and the control group were collected, and preliminary data processing was completed using standardized analytical methods. PBMCs were initially segmented into distinct subpopulations, and the divisions were progressively refined until the most significantly altered cell populations were identified. A combination of high-dimensional weighted gene co-expression analysis (hdWGCNA), cellular communication, pseudotime analysis, and single-cell regulatory network inference and clustering (SCENIC) analysis was used to conduct single-cell transcriptomics analysis and identify key gene modules from them. Genes were screened using machine learning (ML) in the key gene modules, and internal and external dataset validations were performed using multiple ML methods to test predictive performance. Finally, bidirectional Mendelian randomization (MR) analysis, regional linkage analysis, and the Steiger test were employed to analyze the key gene. Result: A significant decrease in non-classical monocytes was detected in PMBC of AD patients. Subsequent analyses revealed the inherent connection of non-classical monocytes to AD, and the NAP1L1 gene identified within its gene module appeared to exhibit some association with AD as well. Conclusion: The NAP1L1 gene is a potential predictive biomarker for AD.
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ETHNOPHARMACOLOGICAL RELEVANCE: Dioscoreae Rhizoma, a kind of Chinese yam, is a medicinal and edible plant used in China for strengthening the spleen and stomach. However, there is a lack of modern pharmacology studies regarding its anti-gastric injury activity. AIM OF THE STUDY: This study aimed to investigate the phytochemical composition of Chinese yam aqueous extract (CYW) and evaluate its gastroprotective effects against ethanol-induced gastric injury in vitro and in vivo. MATERIALS AND METHODS: The active components of CYW were identified using HPLC-QTOF-MS/MS in combination with the GNPS molecular networking and network pharmacology. In vitro studies were performed in the RAW264.7/GES-1 cell coculture system. In vivo study, mice were treated with CYW (0.31, 0.63, and 3.14 g/kg BW, orally) for 14 days, followed by a single oral dose of ethanol (10 mL/kg BW) to induce gastric injury. The biochemical, inflammation and oxidative stress markers were analyzed using commercial kits. Histopathology was used to assess the degree of gastric injury. Gene and protein expressions were studied using RT-qPCR and western blotting, respectively. RESULTS: CYW significantly restored the levels of SOD, GPx and CAT, and reduced the MDA content. Further analyses showed that CYW significantly alleviated the gastric oxidative stress by inhibiting the inflammation via decreasing p-NF-κB and p-IκB-α expression levels and inhibiting the generation of IL-6, TNF-α, and IL-1ß. At the same time, the fraction remarkably upregulated Bcl-2, downregulated Bax and increased growth factor secretion, thereby prevented gastric mucous cell. Besides, The combination of HPLC-QTOF-MS/MS, GNPS molecular networking analysis, and network pharmacology demonstrated that linoleic acid, 3-acetyl-11-keto-beta-boswellic acid, adenosine, aminocaproic acid, tyramine, DL-tryptophan, cycloleucine, lactulose, melibiose, alpha-beta-trehalose, and sucrose would be the main active compounds of CYW against ethanol-induced gastric injury. CONCLUSION: This study showed that CYW is potentially rich source of anti-oxidant and anti-inflammatory bioactive compounds. It showed efficacy against ethanol-induced gastric injury by inhibiting inflammation, oxidative stress, and apoptosis in the stomach. The results of the current work indicate that Dioscoreae Rhizoma could be utilized as a type of natural resource for production of new medicine and functional foods to prevent and/or ameliorate ethanol-induced gastric injury.
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Dioscorea , Etanol , Extratos Vegetais , Rizoma , Animais , Etanol/química , Dioscorea/química , Camundongos , Masculino , Rizoma/química , Extratos Vegetais/farmacologia , Extratos Vegetais/química , Células RAW 264.7 , Estresse Oxidativo/efeitos dos fármacos , Compostos Fitoquímicos/farmacologia , Compostos Fitoquímicos/análise , Mucosa Gástrica/efeitos dos fármacos , Mucosa Gástrica/patologia , Mucosa Gástrica/metabolismo , Humanos , Anti-Inflamatórios/farmacologia , Anti-Inflamatórios/isolamento & purificaçãoRESUMO
Nonporous adaptive crystals (NACs) are crystalline nonporous materials that can undergo a structural adaptive phase transformation to accommodate specific guest via porous cavity or lattice voids. Most of the NACs are based on pillararenes because of their flexible backbone and intrinsic porous structure. Here a readily prepared organic hydrochloride of 4-(4-(diphenylamino)phenyl)pyridin-1-ium chloride (TPAPyH), exhibiting the solvent dimension-dependent adaptive crystallinity is reported. Wherein it forms a nonporous α crystal in a solvent with larger dimensions, while forming two porous ß and γ crystals capable of accommodating solvent molecules in solvent with small size. Furthermore, the thermal-induced single-crystal-to-single-crystal (SCSC) transition from the ß to α phase can be initiated. Upon exposure to iodine vapor or immersion in aqueous solution, the nonporous α phase transforms to porous ß phase by adsorbing iodine molecules. Owing to the formation of trihalide anion I2Cl- within the crystal cavity, TPAPyH exhibits remarkable performance in iodine storage, with a high uptaking capacity of 1.27 g g-1 and elevated iodine desorption temperature of up to 110 and 82 °C following the first and second adsorption stage. The unexpected adaptivity of TPAPyH inspires the design of NACs for selective adsorption and separation of volatile compound from organic small molecules.
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Ephedra herb (EH), an important medicine prescribed in herbal formulas by Traditional Chinese Medicine practitioners, has been widely used in the treatment of viral pneumonia in China. However, the molecular basis of EH in viral pneumonia remains unclear. In this study, a ternary correlation multi-symptom network strategy was established based on in vivo chemical profile identification and metabolomics to explore the molecular basis of EH against viral pneumonia. Results showed that 143 compounds of EH and 70 prototype components were identified in vivo. EH could reduce alveolar-capillary barrier disruption in rats with viral pneumonia and significantly downregulate the expression of inflammatory factors and bronchoalveolar lavage fluid. Plasma metabolomics revealed that EH may be involved in the regulation of arachidonic acid, tryptophan, tyrosine, nicotinate, and nicotinamide metabolism. The multi-symptom network showed that 12 compounds have an integral function in the treatment of viral pneumonia by intervening in many pathways related to viruses, immunity and inflammation, and lung injury. Further verification demonstrated that sinapic acid and frambinone can regulate the expression of related genes. It has been shown to be a promising representative of the pharmacological constituents of ephedra.
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Medicamentos de Ervas Chinesas , Ephedra , Metabolômica , Ratos Sprague-Dawley , Animais , Ratos , Medicamentos de Ervas Chinesas/farmacologia , Medicamentos de Ervas Chinesas/química , Ephedra/química , Masculino , Pneumonia Viral/tratamento farmacológico , Pneumonia Viral/metabolismo , Pneumonia Viral/virologiaRESUMO
Recently, stimulus-responsive organic materials with room-temperature phosphorescence (RTP) properties have attracted significant attention owing to their potential applications in chemical sensing, anticounterfeiting, and displays. However, molecular design currently lacks systematicity and effectiveness. Herein, we report a capture-release strategy for the construction of reversible RTP via B/N Lewis pairs. Specifically, the RTP of the Lewis acid of 7-bromo-5,9-dioxa-13b-boranaphtho[3,2,1-de]anthracene (BrBA) can be deactivated through capturing by the Lewis base, N,N-diphenyl-4-(pyridin-4-yl)aniline (TPAPy), and reactivated by dissociation of B-N bonds to release BrBA. Reversible RTP is attributed to the exceptional self-assembly capability of BrBA, whereas the tunable RTP colors are derived from distinct Förster resonance energy transfer (FRET) processes. The potential applications of RTP materials in information storage and anti-counterfeiting were also experimentally validated. The capture-release approach proposed in this study offers an effective strategy for designing stimulus-responsive materials.
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Asparagi radix is an edible herb with medicinal properties and is now widely used in clinical applications for improving pulmonary inflammation. However, the lung-protective effect and the active constituents of Asparagi radix are yet to be elucidated. Herein, the potential pulmonary protective effect of the oligosaccharides of Asparagi radix was investigated. We firstly identified eighteen oligosaccharides with different degrees of polymerization from Asparagi radix using HPLC-QTOF MS. Oligosaccharides were analysed for 20 samples of Asparagi radix collected from various regions in China using HILIC-ELSD and were found to stably exist in this herb. In this study, we found that AROS significantly reduced NO production and effectively down-regulated the mRNA expression of IL-6, IL-1ß and TNF-α in RAW 264.7 cells, thereby reducing the inflammatory response induced by LPS. AROS also inhibited LPS-stimulated intracellular ROS production. A murine model of lipopolysaccharide (LPS)-induced acute lung injury was used to evaluate the in vivo anti-inflammatory and lung protective efficacies of AROS. AROS ameliorated the damage to the pulmonary cellular architecture pathological injury and lung edema. AROS significantly decreased the levels of cytokines IL-6, TNF-α and IL-1ß; the levels of MPO and MDA; and superoxide dismutase consumption in vivo. This effect of oligosaccharides can explain the traditional usage of Asparagus cochinchinensis as a tonic medicine for respiratory problems, and oligosaccharides from Asparagi radix used as a natural ingredient can play an important role in protecting lung injury.
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Lesão Pulmonar Aguda , Lipopolissacarídeos , Camundongos , Animais , Lipopolissacarídeos/efeitos adversos , Fator de Necrose Tumoral alfa/genética , Fator de Necrose Tumoral alfa/farmacologia , Interleucina-6/genética , Lesão Pulmonar Aguda/induzido quimicamente , Lesão Pulmonar Aguda/tratamento farmacológico , Lesão Pulmonar Aguda/genética , Pulmão , Citocinas/genética , Citocinas/metabolismo , NF-kappa B/metabolismoRESUMO
In recent years, public sports services have attracted great attention owing to their increasingly important role in public health. However, effective evaluation metrics measuring the efficiency of such services from a spatial perspective (e.g., accessibility and distribution of sports parks) remain absent. Indeed, most designs of sports park distribution in urban areas did not consider practical factors such as local road networks, population distribution, and resident preference, resulting in low utilization rates of these parks. In this study, a spatial accessibility-based method is proposed for evaluation of the distributions of sports parks. As a demonstration, the distribution of sports parks in the central urban area of Changsha, China was investigated using the proposed method by the GIS network analysis. Additionally, optimization strategies for sports park distribution (in terms of spatial distribution and overall accessibility) were developed by using spatial syntax.
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Benchmarking , Esportes , China , Saúde PúblicaRESUMO
Exploring blue organic light emitting diodes (OLED) is an important but challenging issue. Herein, to achieve blue-shifted emission, cyclohexane is fused to quinoxaline to weaken the electron-withdrawing ability and conjugation degree of the acceptor. As a result, blue to cyan fluorescent emitters of Me-DPA-TTPZ, tBu-DPA-TTPZ, and TPA-TTPZ were designed and synthesized with donors of diphenylamine and triphenylamine, which exhibit high photoluminescence quantum yields and good thermal stability. In OLEDs with emitters of TPA-TTPZ, the sensitized and nonsensitized devices demonstrate deep-blue (449 nm) and blue (468 nm) emission with maximum external quantum efficiency and CIE coordinates of 6.1%, (0.15, 0.10) and 5.1%, (0.17, 0.22), respectively, validating their potential as blue emitters in OLEDs.
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Recently, the remarkable advances in thermally activated delayed fluorescence (TADF) materials have attracted much attention due to their 100% exciton utilization efficiency in organic light-emitting diodes (OLEDs). Although the commercialization of TADF materials is at an early stage, they exhibit enormous potential for next-generation OLEDs due to the comparable electroluminescence performance to metal of their phosphorescent complex counterparts, but without the presence of precious metal elements. This review summarizes the different types of TADF small molecules with various photophysical properties and the state-of-the-art molecular design strategies. Furthermore, the device engineering is discussed, and emerging optoelectronic applications, such as organic light-emitting electrochemical cells, organic lasing, and organic scintillators, are introduced. It is anticipated that this review can clarify the design of efficient TADF emitters and point out the direction of future development.
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Photodynamic therapy (PDT) is emerging as a powerful tool for cancer treatment due to its unique advantages in terms of noninvasive and spatiotemporal selectivity. However, the residue of photosensitizers (PSs), which usually lead to thorny post-treatment side effects after photodynamic therapy (PDT), is one of bottlenecks for clinical translation. Herein, PSs with multiple degradation modes are developed to solve this issue. Upon 660 nm laser excitation, PSs can produce different types of reactive oxygen species (ROS), in which 1O2 and O2·- could kill the cancer cells, while ·OH could oxide the PSs themselves for photodegradation. After PDT, the residual few number of PSs could be further oxidized by endogenous ROS for biodegradation, and the degradation products could be further excreted by urine. This process therefore solves the slow-metabolism issue of traditional PSs. Among them, SQSe demonstrates the highest killing efficiency with best degradation ability, as confirmed by both in vitro and in vivo results. The postoperative safety of SQSe is further verified by assessment on in vivo artificially induced post-operative side effects.
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Neoplasias , Fotoquimioterapia , Humanos , Fármacos Fotossensibilizantes/química , Fotoquimioterapia/métodos , Espécies Reativas de Oxigênio/metabolismo , Óxidos/uso terapêutico , Neoplasias/tratamento farmacológicoRESUMO
Organic luminescent materials that can simultaneously achieve multimode mechanochromism and its water-vapor-induced recovery are desirable for practical applications but rarely reported. Herein, an amphiphilic compound, 4-(9H-carbazol-9-yl)-1-(2-hydroxyethyl)pyridin-1-ium bromide (CPAB), is designed by integrating a lipophilic aromatic unit and hydrophilic end in the molecular architecture. Self-recovered mechanochromism from brown to cyan is observed upon mechanical grinding in air. Comprehensive research by X-ray diffraction, infrared spectroscopy, and single-crystal analysis reveals that the photoluminescence switch originates from the variation in intermolecular hydrogen bonds and molecular packing mode. The amphiphilic nature of CPAB allows water molecules to enter the crystalline lattice, forming two polymorphs of the crystalline phase, namely CPAB-D and CPAB-W. The hydrosoluble CPAB exhibits excellent capability in probing the level 3 details of fingerprints because its lipophilic part can target the fatty acid residues of fingerprints, leading to strong aggregation-induced fluorescence. The research may inspire the design of latent fingerprint developers and application in forensics/anti-counterfeiting.
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Determining the degree and the spatial extent of structural order in liquids is a grand challenge. Here, we are able to resolve the structural order in a model organic electrolyte of 1 M lithium hexafluorophosphate (LiPF6) dissolved in 1:1 (v/v) ethylene carbonate:diethylcarbonate by developing an integrated method of liquid-phase transmission electron microscopy (TEM), cryo-TEM operated at -30°C, four-dimensional scanning TEM, and data analysis based on deep learning. This study reveals the presence of short-range order (SRO) in the high-salt concentration domains of the liquid electrolyte from liquid phase separation at the low temperature. Molecular dynamics simulations suggest the SRO originates from the Li+-(PF6-)n (n > 2) local structural order induced by high LiPF6 salt concentration.
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Moiré superlattices are twisted bilayer materials in which the tunable interlayer quantum confinement offers access to new physics and novel device functionalities. Previously, moiré superlattices were built exclusively using materials with weak van der Waals interactions, and synthesizing moiré superlattices with strong interlayer chemical bonding was considered to be impractical. Here, using lead sulfide (PbS) as an example, we report a strategy for synthesizing moiré superlattices coupled by strong chemical bonding. We use water-soluble ligands as a removable template to obtain free-standing ultrathin PbS nanosheets and assemble them into direct-contact bilayers with various twist angles. Atomic-resolution imaging shows the moiré periodic structural reconstruction at the superlattice interface due to the strong metavalent coupling. Electron energy loss spectroscopy and theoretical calculations collectively reveal the twist-angle-dependent electronic structure, especially the emergent separation of flat bands at small twist angles. The localized states of flat bands are similar to well-arranged quantum dots, promising an application in devices. This study opens a new door to the exploration of deep energy modulations within moiré superlattices alternative to van der Waals twistronics.
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How to improve the yield of crops has always been the focus of breeding research. Due to the population growth and global climate change, the demand for food has increased sharply, which has brought great challenges to agricultural production. In order to make up for the limitation of global cultivated land area, it is necessary to further improve the output of crops. Photosynthesis is the main source of plant assimilate accumulation, which has a profound impact on the formation of its yield. This review focuses on the cultivation of high light efficiency plants, introduces the main technical means and research progress in improving the photosynthetic efficiency of plants, and discusses the main problems and difficulties faced by the cultivation of high light efficiency plants. At the same time, in view of the frequent occurrence of high-temperature disasters caused by global warming, which seriously threatened plant normal production, we reviewed the response mechanism of plants to heat stress, introduced the methods and strategies of how to cultivate heat tolerant crops, especially rice, and briefly reviewed the progress of heat tolerant research at present. Given big progress in these area, the era of cultivating smart rice with high light efficiency and heat tolerance has come of age.
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Mechanoluminescence (ML) is the production of light from materials in response to the external stimulus of mechanical action. For organic compounds, the production of ML is tightly associated with fracture and plastic deformation of materials with piezoelectric effect in crystal lattice, and the ML property is highly dependent on the molecular packing mode, spatial conformation, and intermolecular interaction in the solid state. In the past few years, our group focused on the molecular design of pure organic ML compounds, with an attempt to discover different features of ML in pursuing the inherent emission mechanism and potential practical applications. We successfully found polymorph-dependent ML, ML with a phosphorescent property, conformation-dependent ML, ML with odd-even effect, wearable ML devices applied in heartbeat and pressure detection, etc. In this Perspective, we aim to deepen the understanding of ML and provide some guidance for the molecular design of organic light-emitting materials through the combination of our contributions.
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Compostos Orgânicos , Conformação Molecular , Compostos Orgânicos/químicaRESUMO
Three conjugated polymers that have the same donor-acceptor structure but totally different architectures are designed to show both Type-I and Type-II photosensitization abilities simultaneously, among which the hyperbranched polymer shows the best performance in both in vitro and in vivo experiments, superior to even the commonly used clinical photosensitizer of hemoporfin.
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Fotoquimioterapia , Fármacos Fotossensibilizantes , Fármacos Fotossensibilizantes/química , Polimerização , Polímeros/químicaRESUMO
High-efficiency blue perovskite emitters with fast fluorescence radiation are not only crucial to achieving high-quality displays but also highly desired for optical wireless communications and quantum information technologies. Here, we demonstrate the preparation of blue-emitting Eu3+-, Sb3+-, and Ba2+-induced CsPbBr3 nanoplatelets with narrow spectral widths. Among them, Sb3+-doped CsPbBr3 NPLs can reach a photoluminescence quantum yield of 95%, with a very short fluorescence lifetime of 1.48 ns and greatly reduced ligand dosage. Through nuclear magnetic resonance analysis and density functional theory calculations, we find that the dopant-ligand interaction and dopant-induced growth energy barrier decide the growth kinetics of doped nanoplatelets. These mechanisms offer a fresh route to controlling the dimension of nanoscale perovskite emitters and benefit the development of fast-radiative perovskite emitters.
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Pure organic room-temperature phosphorescence (RTP) has attracted wide interest due to its unique advantages and promising applications. However, it is still challenging to develop efficient RTP through precise molecular design. In this work, RTP is observed from two simple aromatic acids, nicotinic acid (NA) and isonicotinic acid (INA), in the crystal state. Single crystal structure analysis indicates that an intense hydrogen bond between the pyridine nitrogen atom and the carboxyl group results in zigzag and linear molecular packing modes in NA and INA crystal. From theoretical calculations, the hydrogen bond can effectively promote the intersystem crossing process and stabilize triplet exciton. The identical molecular orientations in the molecular array contribute to the larger dipole moment of INA as compared to that of NA, which should be responsible for the red-shifted photoluminescence and RTP of INA. When the hydrogen bond is destructed by grinding or deprotonation, the RTP decreases sharply, further confirming the crucial role of the hydrogen bond on RTP.