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Thick electrodes with high mass loading and increased content of active materials are critical for achieving higher energy density in contemporary lithium-ion batteries (LIBs). Nonetheless, producing thick electrodes through the commonly used slurry coating technology remains a formidable challenge. In this study, we have addressed this challenge by developing a dry electrode technology by using ultralong multiwalled carbon nanotubes (MWCNT) as a conductive additive and secondary binder. The mixing process of electrode compositions and the fibrillation process of the polytetrafluoroethylene (PTFE) binder were optimized. The resulting LiCoO2 (LCO) electrode exhibited a remarkable mass loading of 48 mg cm-2 and an active material content of 95 wt %. Notably, the thick LCO electrode demonstrated a superior mechanical strength and electrochemical performance. After 100 cycles at a current density of 1/3 C, the electrode still exhibited a capacity retention of 91% of its initial capacity. This dry electrode technology provides a practicable and scalable approach to the powder-to-film LIB electrode manufacturing process.
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The practical application of lithium-oxygen batteries (LOBs) with ultrahigh theoretical energy density faces the problems of poor kinetics and deficient reversibility. The electrolyte is of vital significance to the electrochemical stability and reaction pathway of LOBs due to the formation of soluble products. Here, a 15-crown-5 ether (15C5) is employed to regulate the solvation structure of Li+ and manipulate the reaction mechanism through regulating the binding ability toward Li+. The promoted dissociation of LiNO3 by 15C5 increases the catalytical active anions in the electrolyte and stabilizes the Li-containing reduced oxygen species to promote the solution pathway of discharge product growth. Besides, 15C5 also facilitates the kinetics of the electrochemical decomposition of Li2O2 and prolongs the cycle life to 178 cycles. This work inspires a novel approach to improve the battery performance through electrolyte component design.
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Background: Periodontal disease and coronary heart disease are both prevalent diseases worldwide and cause patients physical and mental suffering and a global burden. Recent studies have suggested a link between periodontal disease and coronary heart disease, but there is less research in this field from the perspective of bibliometrics. Objective: This study aimed to quantitatively analyze the literature on periodontal disease and coronary heart disease to summarize intellectual bases, research hotspots, and emerging trends and pave the way for future research. Methods: The Science Citation Index Expanded database was used to retrieve study records on periodontal disease and coronary heart disease from 1993 to 2022. After manual screening, the data were used for cooperative network analysis (including countries/regions, institutions and authors), keyword analysis, and reference co-citation analysis by CiteSpace software. Microsoft Excel 2019 was applied for curve fitting of annual trend in publications and citations. Results: A total of 580 studies were included in the analysis. The number of publications and citations in this field has shown an upward trend over the past 30 years. There was less direct collaboration among authors and institutions in this field but closer collaboration between countries. The United States was the country with the most published articles in this field (169/580, 29.14%). Based on the results of keyword analysis and literature co-citation analysis, C-reactive protein, oral flora, atherosclerosis, infection, and inflammation were previous research hotspots, while global burden and cardiovascular outcomes were considered emerging trends in this field. Conclusion: Studies on periodontal disease and coronary heart disease, which have attracted the attention of an increasing number of researchers, have been successfully analyzed using bibliometrics and visualization techniques. This paper will help scholars better understand the dynamic evolution of periodontal disease and coronary heart disease and point out the direction for future research. Clinical significance: This paper presents an overview between periodontal disease and coronary heart disease. Further exploration of the two diseases themselves and the potential causal relationship between the two is necessary and relevant, which may impact basic research, diagnosis, and treatment related to both diseases. This will aid the work of researchers and specialist doctors, and ultimately benefit patients with both diseases.
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Lithium (Li) metal is widely recognized as a viable candidate for anode material in future battery technologies due to its exceptional energy density. Nevertheless, the commercial Li foils in common use are too thick (≈100 µm), resulting in a waste of Li resources. Herein, by applying the vacuum evaporation plating technology, the ultra-thin Li foils (VELi) with high purity, strong adhesion, and thickness of less than 10 µm are successfully prepared. The manipulation of evaporation temperature allows for convenient regulation of the thickness of the fabricated Li film. This physical thinning method allows for fast, continuous, and highly accurate mass production. With a current density of 0.5 mA cm-2 for a plating amount of 0.5 mAh cm-2, VELi||VELi cells can stably cycle for 200 h. The maximum utilization of Li is already more than 25%. Furthermore, LiFePO4||VELi full cells present excellent cycling performance at 1 C (1 C = 155 mAh g-1) with a capacity retention rate of 90.56% after 240 cycles. VELi increases the utilization of active Li and significantly reduces the cost of Li usage while ensuring anode cycling and multiplication performance. Vacuum evaporation plating technology provides a feasible strategy for the practical application of ultra-thin Li anodes.
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The low ionic conductivity of LiCoO2 limits the rate performance of the overall electrode. Here, a polymeric composite binder composed of poly(vinylidene fluoride) (PVDF) and poly(ethylene oxide) (PEO) is reported to efficiently improve the ion transport in the LiCoO2 electrode. This is where the lithium-ion transport channel constructed by oxygen atoms of PEO can afford the electrode a lithium-ion transport number (tLi+) as high as 0.70 with the optimized composite binder in a mass ratio of 1:1 (O5F5), significantly higher than that of traditional PVDF (0.44). As a result, the O5F5 binder endows the LiCoO2 electrode with an impressive capacity of 90 mAh g-1 even at 15 C, which is twice as high as the PVDF electrode. In addition, the initial Coulombic efficiency of the LiCoO2 electrode with the O5F5 binder is close to 100% and the capacity retention is 91% after 100 cycles at 1 C. This study overcomes the problem of slow ion conductivity of the LiCoO2 electrode, providing an easy method for developing high-rate cathode binders.
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Aqueous Zn ion-based fiber-shaped batteries (AZFBs) with the merits of high flexibility and safety have received much attention for powering wearable electronic devices. However, the relatively low specific capacity provided by cathode materials limits their practical application. Herein, we first propose a simple strategy for fabricating high-capacity Zn-iodine fiber-shaped batteries with a high concentration electrolyte and a reduced graphene oxide fiber (GF) cathode. It was found that oxygen functional groups in the graphene sheet demonstrate strong interaction with polyiodides but hinder electron conductivity; thus, the optimal balance between the specific capacity and coulombic efficiency of the GF electrode can be a function of the surface properties at different hydrothermal temperatures. Besides, the regulated high concentration electrolyte effectively suppresses the diffusion of polyiodides, which is attributed to the constrained freedom of water. More importantly, a four-electron redox mechanism was experimentally revealed through in situ Raman spectra. As a result, this fiber-shaped battery delivers a superior high reversible capacity of 390 mA h cm-3 at 1 A cm-3, an excellent rate performance of 125.7 mA h cm-3 at a high current density of 8 A cm-3 and outstanding cycling life with 82% capacitance retention after 2500 cycles.
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Lithium-ion thermoelectrochemical cell (LTEC), featuring simultaneous energy conversion and storage, has emerged as promising candidate for low-grade heat harvesting. However, relatively poor thermosensitivity and heat-to-current behavior limit the application of LTECs using LiPF6 electrolyte. Introducing additives into bulk electrolyte is a reasonable strategy to solve such problem by modifying the solvation structure of electrolyte ions. In this work, we develop a dual-salt electrolyte with fluorosurfactant (FS) additive to achieve high thermopower and durability of LTECs during the conversion of low-grade heat into electricity. The addition of FS induces a unique Li+ solvation with the aggregated double anions through a crowded electrolyte environment, resulting in an enhanced mobility kinetics of Li+ as well as boosted thermoelectrochemical performances. By coupling optimized electrolyte with graphite electrode, a high thermopower of 13.8 mV K-1 and a normalized output power density of 3.99 mW m-2 K-2 as well as an outstanding output energy density of 607.96 J m-2 can be obtained. These results demonstrate that the optimization of electrolyte by regulating solvation structure will inject new vitality into the construction of thermoelectrochemical devices with attractive properties.
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The high dissolution of polyiodides and unstable interface at the anode/electrolyte severely restrict the practical applications of rechargeable aqueous Zn-iodine batteries. Herein, we develop a zinc ion-based montmorillonite (ZMT) electrolyte membrane for synergizing ion sieve and solvation regulation to achieve highly stable Zn-iodine batteries. The rich M-O band and special cation-selective transport channel in ZMT locally tailor the solvation sheath around Zn2+ and therefore achieve high transference number (t+ = 0.72), benefiting for uniform and reversible deposition/stripping of Zn. Meanwhile, the mechanisms for three-step polyiodide generation and shuttle-induced Zn corrosion are highlighted by in situ characterization techniques. It is confirmed that the strong chemical adsorption between O atoms in ZMT and polyiodides species is the key to effectively inhibit the shuffle effect and side reactions. Consequently, the ZMT-based Zn-iodine battery delivers a high capacity of 0.45 mAh cm-2 at 1 mA cm-2 with a much improved Coulombic efficiency of 99.5% and outstanding capacity retention of 95% after 13â¯500 cycles at 10 mA cm-2. Moreover, owing to its high durability and chemical inertness and structural stability, ZMT-based electrolyte membranes can be recycled and applied in double-sided pouch cells, delivering a high areal capacity of 2.4 mAh cm-2 at 1 mA cm-2.
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Neurons are the fundamental units of neural networks. In this paper, we propose a method for explaining neural networks by visualizing the learning process of neurons. For a trained neural network, the proposed method obtains the features learned by each neuron and displays the features in a human-understandable form. The features learned by different neurons are combined to analyze the working mechanism of different neural network models. The method is applicable to neural networks without requiring any changes to the architectures of the models. In this study, we apply the proposed method to both Fully Connected Networks (FCNs) and Convolutional Neural Networks (CNNs) trained using the backpropagation learning algorithm. We conduct experiments on models for image classification tasks to demonstrate the effectiveness of the method. Through these experiments, we gain insights into the working mechanisms of various neural network architectures and evaluate neural network interpretability from diverse perspectives.
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Algoritmos , Redes Neurales de la Computación , HumanosRESUMEN
Flexible power supply devices provide possibilities for wearable electronics in the Internet of Things. However, unsatisfying capacity or lifetime of typical batteries or capacitors seriously limit their practical applications. Different from conventional heat-to-electricity generators, zinc ion thermal charging cells has been a competitive candidate for the self-power supply solution, but the lack of promising cathode materials has restricted the achievement of promising performances. Herein, we propose an attractive cathode material by rational heterostructure engineering of hydrated vanadium pentoxide. Owing to the integration of thermodiffusion and thermoextraction effects, the thermopower is significantly improved from 7.8 ± 2.6 mV K-1 to 23.4 ± 1.5 mV K-1. Moreover, an impressive normalized power density of 1.9 mW m-2 K-2 is achieved in the quasi-solid-state cells. In addition, a wearable power supply constructed by three units can drive the commercial health monitoring system by harvesting body heat. This work demonstrates the effectiveness of electrodes design for wearable thermoelectric applications.
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The employment of Li metal anodes is a key to realizing ultra-high energy batteries. However, the commercialization of lithium metal batteries (LMBs) remains challenging partially due to the thermodynamic instability and competitive oxidative decomposition of the solvent. Herein, a bi-functional electrolyte for stabilizing the interfaces of both the Li metal anode and LiCoO2 (LCO) cathode is designed by introducing lithium nitrate (LiNO3) through Ethylene Glycol Bis(Propionitrile) Ether (DENE). For the anode, the C8H12N2O2-LiNO3 coordination-solvation contributes to forming a stable Li3N-enhanced solid electrolyte interphase (SEI), which increases the average Li coulombic efficiency (CE) up to 98.5%. More importantly, in situ electrochemical dilatometry further reveals that the highly reversible behavior and a low volume expansion of lithium deposition are related to the stable Li3N-enhanced SEI. The designed electrolyte enables the LiâLCO cell to achieve an average CE of 99.2% and a high capacity retention of 88.2% up to 4.6 V after 100 cycles. This work provides a strategic guidance in developing high-voltage LiâLCO batteries with dual electrolyte additives.
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As a new class of crystalline materials, covalent organic frameworks (COFs) have long-range ordered channels and feasibility to functionalize. The well-arranged pores make it possible to contain and transport ions. Here, we designed a novel functionalized anionic COF-SS-Li by a post-synthetic method utilizing the Povarov reaction of BDTA-COF, anchoring -SO3- groups to the COF backbone and converting the imine linkage to a more stable quinoline unit. The grafted -SO3- groups and directional channels can promote the lithium-ion transport through a hopping mechanism. As a solid-state lithium-ion electrolyte, COF-SS-Li exhibits the conductivities of 9.63 × 10-5 S cm-1 at 20 °C and 1.28 × 10-4 S cm-1 at 40 °C and a wide electrochemical window of 4.85 V. The assembled Li|COF-SS-Li|Li symmetric cell can cycle stably for 600 h at 0.1 mA cm-2. Also, the Li|COF-SS-Li|LiFePO4 cell delivers an initial capacity of 117 mAh g-1 at 0.1 A g-1 and retains a capacity rate of 56.7% after 500 cycles. The research enriches the solid-state electrolytes for lithium-ion batteries.
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Objectives: To systematically analyze adverse events (AEs) in treatment of spinal muscular atrophy (SMA) with Nusinersen in children and adolescents. Methods: The study is registered on PROSPERO (CRD42022345589). Databases were searched and literature relating to Nusinersen in the treatment of spinal muscular atrophy in children from the start of database establishment to December 1, 2022, was retrospectively analyzed. R.3.6.3 statistical software was used, and random effects meta-analysis was performed to calculate weighted mean prevalence and 95% confidence intervals (CI). Results: In total, 15 eligible studies were included, with a total of 967 children. Rate of definite Nusinersen-related AEs was 0.57% (95% CI: 0%-3.97%), and probable Nusinersen-related AEs 7.76% (95% CI: 1.85%-17.22%). Overall rate of AEs was 83.51% (95% CI: 73.55%-93.46%), and serious AEs 33.04% (95% CI: 18.15%-49.91%). For main specific AEs, fever was most common, 40.07% (95% CI: 25.14%-56.02%), followed by upper respiratory tract infection 39.94% (95% CI: 29.43%-50.94%), and pneumonia 26.62% (95% CI: 17.99%-36.25%).The difference in overall AE rates between the two groups (Nusinersen group and placebo group) was significant (OR = 0.27,95% CI: 0.08-0.95, P = 0.042). Moreover, incidence of serious adverse events, and fatal adverse events were both significantly lower than in the placebo group (OR = 0.47, 95%CI: 0.32-0.69, P < 0.01), and (OR = 0.37, 95%CI: 0.23-0.59, P < 0.01), respectively. Conclusion: Nusinersen direct adverse events are rare, and it can effectively reduces common, serious, and fatal adverse events in children and adolescents with spinal muscular atrophy.
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A two-dimensional covalent organic framework (NTCDI-COF) with rich redox active sites, high stability and crystallinity was designed and prepared. As a cathode material for lithium-ion batteries (LIBs), NTCDI-COF exhibits excellent electrochemical performance with an outstanding discharge capacity of 210 mA h g-1 at 0.1 A g-1 and high capacity retention of 125 mA h g-1 after 1500 cycles at 2 A g-1. A two-step Li+ insertion/extraction mechanism is proposed based on the ex situ characterization and density functional theory calculation. The constructed NTCDI-COF//graphite full cells can realize a good electrochemical performance.
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The solvation structure of Li+ in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency (ICE) and poor cycle performance of silicon-based materials. Nevertheless, the chemical prelithiation agent is difficult to dope active Li+ in silicon-based anodes because of their low working voltage and sluggish Li+ diffusion rate. By selecting the lithium-arene complex reagent with 4-methylbiphenyl as an anion ligand and 2-methyltetrahydrofuran as a solvent, the as-prepared micro-sized SiO/C anode can achieve an ICE of nearly 100%. Interestingly, the best prelithium efficiency does not correspond to the lowest redox half-potential (E1/2), and the prelithiation efficiency is determined by the specific influencing factors (E1/2, Li+ concentration, desolvation energy, and ion diffusion path). In addition, molecular dynamics simulations demonstrate that the ideal prelithiation efficiency can be achieved by choosing appropriate anion ligand and solvent to regulate the solvation structure of Li+. Furthermore, the positive effect of prelithiation on cycle performance has been verified by using an in-situ electrochemical dilatometry and solid electrolyte interphase film characterizations.
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Polymer binders play an important role in enhancing the electrochemical performance of silicon-based anodes to alleviate the volume expansion for lithium-ion batteries. It is difficult for common one-dimensional (1D) linear binders to limit the volume expansion of a silicon-based electrode when combined with silicon-based particles with scant binding points. Therefore, it is necessary to design a three-dimensional (3D) network structure, which has multiple binding points with the silicon particles to dissipate the mechanical stress in the continuous charge and discharge circulation. Here, a covalent and hydrogen bond synergist 3D network green binder (poly(acrylic acid) (PAA)-dextrin 9 (Dex9)) was prepared by the simple in situ thermal condensation of a one-dimensional liner binder PAA and Dex in the electrode fabrication process. The optimized SiOx@PAA-Dex9 electrode exhibits an initial Coulombic efficiency (ICE) of 82.4% at a current density of 0.2 A g-1. At a high current density of 1 A g-1, it retains a capacity of 607 mAh g-1 after 300 cycles, which is approximately twice as high as that of the SiOx@PAA electrode. Furthermore, the results of in situ electrochemical dilatometry (ECD) and characterization of electrode structures demonstrate that the PAA-Dex9 binder can effectively buffer the huge volume change and maintain the integrity of the SiOx electrodes. The research overcomes the low electrochemical stability difficulty of the 3D binder and sheds light on developing the simple fabrication procedure of an electrode.
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The introduction of groups with high enthalpies of formation can effectively improve the detonation performance of the compounds. A series of novel energetic compounds (10-13) with high enthalpies of formation, high density, and high nitrogen-oxygen content were designed and synthesized by combining gem-polynitromethyl, 1,2,4-oxadiazole, furoxan, and azo groups. All the new compounds were thoroughly characterized by IR, NMR, elemental analysis, and differential scanning calorimetry. Compounds 10 and 11 were also further characterized with single-crystal X-ray diffraction. Compound 11 has high density (1.93 g cm-3), high enthalpy of formation (993.5 kJ mol-1), high detonation velocity (9411 m s-1), and high heat of detonation (6889 kJ kg-1) and is a potentially excellent secondary explosive.
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As a promising candidate for large-scale energy storage, aqueous zinc-ion batteries (ZIBs) still lack cathode materials with large capacity and high rate capability. Herein, a spherical carbon-confined nanovanadium oxynitride with a polycrystalline feature (VNxOy/C) was synthesized by the solvothermal reaction and following nitridation treatment. As a cathode material for ZIBs, it is interesting that the electrochemical performance of the VNxOy/C cathode is greatly improved after the first charging process viain situ electrochemically oxidative activation. The oxidized VNxOy/C delivers a greatly enhanced reversible capacity of 556 mAh g-1 at 0.2 A g-1 compared to the first discharge capacity of 130 mAh g-1 and a high capacity of 168 mAh g-1 even at 80 A g-1. The ex situ characterizations verify that the insertion/extraction of Zn2+ does not affect the crystal structure of oxidized VNxOy/C to promise a stable cycle life (retain 420 mAh g-1 after 1000 cycles at 10 A g-1). The experimental analysis further elucidates that charging voltage and H2O in the electrolyte are curial factors to activate VNxOy/C in that the oxygen replaces the partial nitrogen and creates abundant vacancies, inducing a conversion from VNxOy/C to VNx-mOy+2m/C and then resulting in considerably strengthened rate performance and improved Zn2+ storage capability. The study broadens the horizons of fast ion transport and is exceptionally desirable to expedite the application of high-rate ZIBs.
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With the associated advantages of low costs and abundant resources, sodium-ion capacitors (SICs) present a suitable means for large-scale energy storage. However, their practical application is still significantly limited by the sluggish electrochemical reaction kinetics of battery-type anodes. Herein, the nitrogen-doped carbon-encapsulated Fe7Se8 nanorods (Fe7Se8@NC) with a core-shell structure were prepared via an in-situ self-polymerization and carbonization-selenization approach, which improves ion transport and maintains the structural stability of the nanorods. The designed Fe7Se8@NC nanorods exhibit desirable rate capability with a capacity of 290.7 mAh/g at 10 A/g and long-term cyclability with 84.6 % retention over 6000 cycles at 5 A/g. Moreover, research has shown that the diffusion dynamics of Na+ is improved in ether-based electrolytes and that the irreversible reactions at low voltages can be inhibited by a high discharge cut-off voltage. Furthermore, we demonstrated the specific sodium storage mechanism and excellent electrochemical reversibility of the Fe7Se8@NC electrode through in-situ and ex-situ characterization techniques. As expected, the assembled SICs with the Fe7Se8@NC anode and active carbon cathode deliver prominent energy/power densities and an ultra-long cycle life over 5000 cycles, shedding new light on the design of transition metal dichalcogenides as anode materials for advanced energy storage systems.
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The solvation of cations is one of the important factors that determine the properties of electrolytes. Rational solvation structures can effectively improve the performance of various electrochemical energy storage devices. Water-in-Salt (WIS) electrolytes with a wide electrochemically stable potential window (ESW) have been proposed to realize high cell potential aqueous electrochemical energy storage devices relying on the special solvation structures of cations. The ratio of H2O molecules participating in the primary solvation structure of a cation (a cation hydration ratio) is the key factor for the kinetics and thermodynamics of the WIS electrolytes under an electric field. Here, acetates with different cations were used to prepare WIS electrolytes. And, the effect of different cation hydration ratios on the properties of WIS electrolytes was investigated. Various WIS electrolytes exhibited different physicochemical properties, including the saturated concentration, conductivity, viscosity, pH values and ESW. The WIS electrolytes with a low cation hydration ratio (<100%, an NH4-based WIS electrolyte) or a high cation hydration ratio (>100%, a K-based WIS electrolyte and a Cs-based WIS electrolyte) exhibit more outstanding conductivity or a wide ESW, respectively. SCs constructed from active carbon (AC) and these WIS electrolytes exhibited distinctive electrochemical properties. A SC with an NH4-based WIS electrolyte was characterized by higher capacity and better rate capability. SCs with a K-based WIS electrolyte and a Cs-based WIS electrolyte were characterized by a wider operating cell potential, higher energy density and better ability to suppress self-discharge and gas production. These results show that a WIS electrolyte with a low cation hydration ratio or a high cation hydration ratio is suitable for the construction of power-type or energy-type aqueous SCs, respectively. This understanding provides the foundation for the development of novel WIS electrolytes for the application of SCs.