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The overall electrochemical performance of natural graphite is intimately associated with the solid electrolyte interphase (SEI) layer developed on its surface. To suppress the interfacial electrolyte decomposition reactions and the high irreversible capacity loss relating to the SEI formation on a natural graphite (NG) surface, we propose a new design of the artificial SEI by the functional molecular cross-linking framework layer, which was synthesized by grafting acrylic acid (AA) and N,N'-methylenebisacrylamide (MBAA) via an in situ polymerization reaction. The functional polymeric framework constructs a robust covalent bonding onto the NG surface with -COOH and facilitates Li+ conduction owing to the effect of the -CONH group, contributing to forming an SEI layer of excellent stability, flexibility, and compactness. From all the benefits, the initial coulombic efficiency, rate performance, and cycling performance of the graphite anode are remarkably improved. In addition, the full cell using the LiNi0.5Co0.2Mn0.3O2 cathode against the modified NG anode exhibits much-prolonged cycle life with a capacity retention of 82.75% after 500 cycles, significantly higher than the cell using the pristine NG anode. The mechanisms relating to the artificial SEI growth on the graphite surface were analyzed. This strategy provides an efficient and feasible approach to the surface optimization for the NG anode in LIBs.
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Grafite , Eletrodos , EletrólitosRESUMO
Hierarchical olive-like structured carbon-Fe3O4 nanocomposite particles composed of a hollow interior and a carbon coated surface are prepared by a facile, silk protein-assisted hydrothermal method. Silk nanofibers as templates and carbon precursors first regulate the formation of hollow Fe2O3 microspheres and then they are converted into carbon by a reduction process into Fe3O4. This process significantly simplifies the fabrication and carbon coating processes to form complex hollow structures. When tested as anode materials for lithium-ion batteries, these hollow carbon-coated particles exhibit high capacity (900 mAh g(-1)), excellent cycle stability (180 cycles) and rate performance due to their unique hierarchical hollow structure and carbon coating.
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Carbono/química , Fontes de Energia Elétrica , Compostos Férricos/química , Nanocompostos/química , Seda/química , Animais , Bombyx , Eletroquímica , Microscopia Eletrônica de Varredura , Microesferas , Nanofibras/química , Nanopartículas/química , Nanotubos de Carbono/química , Difração de Raios XRESUMO
This study presents an approach to achieve a near-zero temperature coefficient of resonance frequency (τf) in rare-earth titanate microwave dielectric ceramics (MWDCs) by inducing a phase transition. By Zr4+ substitution at the B site, a series of Sm2Ti1-xZrxO5 (0.02 ≤ x ≤ 0.55) ceramics are synthesized using the solid-state method to intentionally alter the radius ratio of the A/B sites, realizing in a controlled phase transition from orthorhombic (Pnma) to biphasic coexistence and ultimately to cubic (Fd3Ì m) structure. The phase composition is rigorously identified through X-ray diffraction (XRD) Rietveld refinement, high-resolution transmission electron microscopy (HRTEM), selected-area electron diffraction (SAED), and Raman spectroscopy. A comprehensive analysis is conducted to elucidate the relationships between factors such as ionic polarizability, packing fraction, bond valence, complex chemical bonding, and far-infrared reflectivity spectra with microwave dielectric properties. The results demonstrate that these ceramics exhibit a broad range of permittivity (14.30-23.18), high-quality factors (14,828-22,300 GHz), opposite temperature coefficient of resonance frequency (-16.0 to + 22.4 ppm/°C), and nice thermal conductivity (1.81-2.76 W·m-1·K-1), particularly at x = 0.30 with a near-zero τf value of +1.6 ppm/°C. The findings not only provide insights into designing MWDCs with a near-zero τf but also offer a promising route for developing advanced microwave materials with improved performance and reliability.
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Few-shot learning (FSL) is a paradigm that simulates the fast learning ability of human beings, which can learn the feature differences between two groups of small-scale samples with common label space, and the label space of the training set and the test set is not repeated. By this way, it can quickly identify the categories of the unseen image in the test set. This method is widely used in image scene recognition, and it is expected to overcome difficulties of scarce annotated samples in remote sensing (RS). However, among most existing FSL methods, images were embed into Euclidean space, and the similarity between features at the last layer of deep network were measured by Euclidean distance. It is difficult to measure the inter-class similarity and intra-class difference of RS images. In this paper, we propose a multi-scale covariance network (MCMNet) for the application of remote sensing scene classification (RSSC). Taking Conv64F as the backbone, we mapped the features of the 1, 2, and 4 layers of the network to the manifold space by constructing a regional covariance matrix to form a covariance network with different scales. For each layer of features, we introduce the center in manifold space as a prototype for different categories of features. We simultaneously measure the similarity of three prototypes on the manifold space with different scales to form three loss functions and optimize the whole network by episodic training strategy. We conducted comparative experiments on three public datasets. The results show that the classification accuracy (CA) of our proposed method is from 1.35 % to 2.36% higher than that of the most excellent method, which demonstrates that the performance of MCMNet outperforms other methods.
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Aprendizagem , Tecnologia de Sensoriamento Remoto , Humanos , Inteligência , Reconhecimento PsicológicoRESUMO
The application of nickel-rich cathodes in lithium-ion batteries has been hampered by its rapid capacity/voltage fading and limited performance of rate. In this work, a passivation technique is used to create a stable composite interface on single-crystal LiNi0.8Co0.1Mn0.1O2 (NCM811) surface, which greatly improves the cycle life-span and high-voltage constancy of cathode with 4.5 and 4.6 V cut-off voltage. The improved Li+ conductivity of the interface enables a firm cathode-electrolyte interphase (CEI), which reduces interfacial side reactions, lowers the risk of safety hazards, and improves irreversible phase transitions. As a result, the electrochemical performance of single-crystal Ni-rich cathode are remarkably enhanced. The specific capacity of 152 mAh g-1 can be delivered at a charging/discharging rate of 5 C under 4.5 V cut-off voltage, much higher than 115 mAh g-1 of the pristine NCM811. After 200 cycles at 1 C, the composite interface modified NCM811 demonstrates outstanding capacity retention of 85.4% and 83.8% at 4.5 V and 4.6 V cut-off voltage, respectively.
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In this study, (La0.2Nd0.2Sm0.2Ho0.2Y0.2)(Nb1-xVx)O4 (0.1 ≤ x ≤ 0.4) ceramics were prepared using a high-entropy strategy via the solid-phase method. The crystal structure, microstructure, vibration modes, and phase transition were studied by X-ray diffraction, scanning electron microscopy/transmission electron microscopy (SEM/TEM), and Raman spectroscopy techniques. The phase of ceramics was confirmed to be a monoclinic fergusonite in the range of x ≤ 0.28, a tetragonal scheelite was in the range of 0.3 ≤ x ≤ 0.32, a complex phase of tetragonal scheelite, and zircon was observed in the ceramics when x ≥ 0.35. A zircon phase was also detected by TEM at x = 0.4. The ceramic at x = 0.25 exhibited outstanding temperature stabilization with εr = 18.06, Q × f = 56,300 GHz, and τf = -1.52 ppm/°C, while the x = 0.2 ceramic exhibited a low dielectric loss with εr = 18.14, Q × f = 65,200 GHz, and τf = -7.96 ppm/°C. Moreover, the permittivity, quality factor, and the temperature coefficient of resonance frequency were related to the polarizability, packing fraction, density, and the temperature coefficient of permittivity caused by phase transition. This is an effective method to regulate near-zero τf by the synergism of the high-entropy strategy and substituting Nb with V in LnNbO4 ceramics.
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In order to improve the oil adsorption capacity of chickpea protein, enzymatic cross-linking combined ultrasound was used to modify chickpea protein. Electrophoretic results showed that enzymatic cross-linking made the protein bands thinner, but ultrasound had no significant effect. The oil adsorption capacity of chickpea protein increased from 1.88 to 2.43 g/g; the surface hydrophobicity increased from 3933 to 4575; the zeta potential and emulsification performance were improved.After enzymatic cross-linking, the content of the free sulfhydryl group and emulsifying stability were decreased, and the particle size and the content of disulfide bonds were increased.After ultrasonic treatment, these properties showed an opposite trend. Fourier Transform Infrared Spectroscopy showed that ß-turn and random coil increased, the structure of protein became more loose and disordered. These results indicate that enzymatic cross-linking combined with ultrasound improves the functional properties of chickpea protein and extends its application.
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Cicer , Adsorção , Interações Hidrofóbicas e Hidrofílicas , Tamanho da Partícula , Proteínas de Soja/químicaRESUMO
The modification of the structure and function of wheat gluten because of planetary ball milling was investigated. Reduced SDS-PAGE revealed that the subunit compositions and bands of gluten did not change with an increase in grinding time. FTIR analysis showed that α-helices and ß-sheets decreased, whereas ß-turns increased, indicating that the secondary structure of gluten became looser and more disorderly. Owing to the mechanical force of planetary ball milling constantly breaking the disulfide bonds in gluten, the number of free sulfhydryl groups increased, and surface hydrophobicity increased from 940.97 to 1197.50 after 20 min ball-milling treatments, whereas the foaming capacity was improved from 8.7 to 31 cm3. After 40 min, mastersizer analysis showed that particle size decreased from 85.9 to 32.3 µm, and the whiteness increased from 49.51 to 65.59. These results indicate that planetary grinding technology improves the functional properties of wheat gluten and expands its application potential.
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Glutens , Triticum , Interações Hidrofóbicas e Hidrofílicas , Tamanho da Partícula , Estrutura Secundária de ProteínaRESUMO
A solid electrolyte interphase (SEI) layer on a graphite anode plays a crucial role in deciding electrochemical properties of the electrode including the first Coulombic efficiency, rate capability, operating temperature, and long-term cycling stability. However, the ultrathin functional SEI layer is always naturally grown via electrolyte reduction decomposition reactions. Herein, we report a new strategy of in situ transformed solid electrolyte interphase of high stability by implanting a 4-vinylbenzoic acid (4-VBA) nanolayer on a mildly oxidized graphite surface. A 4-VBA layer of 40 nm contributes to the transformation of a robust and stable SEI layer, which not only significantly enhances the overall electrochemical performances of the natural graphite electrode but also greatly prolongs the cycle life of the full cell with the LiNi0.6Co0.2Mn0.2O2 cathode. The effectively suppressed surface evolution aroused from the stable organic SEI transformed from the implanted 4-VBA nanolayer explains the enhanced electrochemical properties.
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A comprehensive understanding of the relationships between PM2.5 concentration and socioeconomic factors provides new insight into environmental management decision-making for sustainable development. In order to identify the contributions of socioeconomic development to PM2.5, their spatial interaction and temporal variation of long time series are analyzed in this paper. Unary linear regression method, Spearman's rank and bivariate Moran's I methods were used to investigate spatioâ»temporal variations and relationships of socioeconomic factors and PM2.5 concentration in 31 provinces of China during the period of 1998â»2016. Spatial spillover effect of PM2.5 concentration and the impact of socioeconomic factors on PM2.5 concentration were analyzed by spatial lag model. Results demonstrated that PM2.5 concentration in most provinces of China increased rapidly along with the increase of socioeconomic factors, while PM2.5 presented a slow growth trend in Southwest China and a descending trend in Northwest China along with the increase of socioeconomic factors. Long time series analysis revealed the relationships between PM2.5 concentration and four socioeconomic factors. PM2.5 concentration was significantly positive spatial correlated with GDP per capita, industrial added value and private car ownership, while urban population density appeared a negative spatial correlation since 2006. GDP per capita and industrial added values were the most important factors to increase PM2.5, followed by private car ownership and urban population density. The findings of the study revealed spatial spillover effects of PM2.5 between different provinces, and can provide a theoretical basis for sustainable development and environmental protection.
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Poluentes Atmosféricos/análise , Material Particulado/análise , China , Monitoramento Ambiental , Produto Interno Bruto , Humanos , Indústrias , Densidade Demográfica , Análise de Regressão , Fatores Socioeconômicos , População UrbanaRESUMO
To enhance the electrochemical properties of silicon anodes in lithium-ion batteries, dimethylacrylamide (DMAA) was selected as a novel electrolyte additive. The addition of 2.5 wt% DMAA to 1.0 M LiPF6/EC : DMC : DEC : FEC (3 : 3 : 3 : 1 weight ratio) electrolyte significantly enhanced the electrochemical properties of the silicon anode including the first coulombic efficiency, rate performance and cycle performance. The solid electrolyte interphase (SEI) layers developed on the silicon anode in different electrolytes were investigated by a combination of electrochemical and spectroscopic studies. The improved electrochemical performances of the Si anode were ascribed to the effective passivation of DMAA on the silicon anode. The addition of DMAA helped develop a uniform SEI layer, which prevented side reactions at the interface of silicon and electrolyte.
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Many factors have been brought forward to explain the capacity degradation mechanisms of LiNixCoyMnzO2 (NCM)/graphite cells at extreme conditions such as under high temperature or with high cutoff voltage. However, the main factors dominating the long-term cycling performance under normal operations remain elusive. Quantitative analyses of the electrode surface evolution for a commercial 18650 LiNi0.5Co0.2Mn0.3O2 (NCM523)/graphite cell during ca. 3000 cycles under normal operation are presented. Electrochemical analyses and inductively coupled plasma-optical emission spectroscopy (ICP-OES) confirm lithium inventory loss makes up for ca. 60% of the cell's capacity loss. Electrochemical deterioration of the NCM523 cathode is identified to be another important factor, which accounts for more than 30% of the capacity decay. Irregular primary particle cracking due to the mechanical stress and the phase change aroused from Li-Ni mixing during repetitive cycles are identified to be the main contributors for the NCM cathode deterioration. The amount of transition metal dissolved into electrolyte is determined to be quite low, and the resulting impedance rise after about 3000 cycles is obtained to be twice that of the reference cell, which are not very significant affecting the long-term cycling performance under normal operations.
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BACKGROUND: High cost of imported pacemakers is a main obstacle for Chinese patients suffering from bradyarrhythmia, and a domestically developed pacemaker will help lower the burden. This study aimed to evaluate the safety and efficacy of Qinming8631 DR (Qinming Medical, Baoji, China), the first domestically developed dual-chamber pacemaker of China, compared with a commercially available pacemaker Talos DR (Biotronik, Berlin, Germany) in Chinese patients. METHODS: A prospective randomized trial was conducted at 14 centers in China. Participants were randomized into trial (Qinming8631 DR) and control (Talos DR) groups. Parameters of the pacing systems were collected immediately after device implantation and during follow-ups. The effective pacing rate at 6-month follow-up was recorded as the primary end point. Electrical properties, magnet response, single- and double-pole polarity conversion, rate response function, and adverse events of the pacing system were analyzed. The Cochran-Mantel-Haenszel Chi-square test, paired t-test, and Wilcoxon signed-rank test were used for measuring primary qualitative outcomes and comparing normally and abnormally distributed measurement data. RESULTS: A total of 225 patients with a diagnosis of bradyarrhythmia and eligible for this study were randomly enrolled into the trial (n = 113) and control (n = 112) groups. They underwent successful pacemaker implantation with acceptable postoperative pacing threshold and sensitivity. Effective pacing rates of trial and control groups were comparable both in the full analysis set and the per protocol set (81.4% vs. 79.5%, P = 0.712 and 95.4% vs. 89.5%, P = 0.143, respectively). In both data sets, noninferiority of the trial group was above the predefined noninferiority limit(-9.5%). CONCLUSIONS: This study established the noninferiority of Qinming8631 DR to Talos DR. The safety and efficacy of Qinming8631 DR pacemaker were comparable to those of Talos DR in treating patients with cardiac bradyarrhythmia.
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Estimulação Cardíaca Artificial/métodos , Marca-Passo Artificial/efeitos adversos , Idoso , Bradicardia/terapia , China , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Estudos ProspectivosRESUMO
How to restrain the dissolution of polysulfides from the sulfur cathode is the current research focus of Li-S batteries. Here, we find that moderate dissolution of polysulfides is of great importance for high-efficiency and stable discharge/charge cycling. Both overprotection and inadequate protection of the sulfur cathode are unfavorable for the cycling of Li-S batteries.
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ZnO nanostructures were manipulated, via a low-temperature solution process, from pure nanorod arrays to complex nanostructures of microflowers on nanorod arrays with adjusted quantities of flowers. We proposed the mechanism of local dissolution-driven growth to rationally discuss the novel growth process. These nanostructures were used as photoanodes in dye-sensitized solar cells. Compared to pure nanorod arrays, the nanorod array-microflower hierarchical structures improved the power conversion efficiency from 0.41% to 0.92%, corresponding to a 124% efficiency increase. The enhancement of the efficiency was mainly ascribed to the synergistic effect of the enhanced surface area for higher dye loading and the improved light harvesting from efficient light scattering. Present results provide a promising route to improve the capability of light-harvesting for ZnO nanorod array-based DSSCs.