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Polarons are quasiparticles formed as a result of lattice distortions induced by charge carriers. The single-electron Holstein model captures the fundamentals of single polaron physics. We examine the power of the exponential ansatz for the polaron ground-state wavefunction in its coupled cluster, canonical transformation, and (canonically transformed) perturbative variants across the parameter space of the Holstein model. Our benchmark serves to guide future developments of polaron wavefunctions beyond the single-electron Holstein model.

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The potential-dependent negative fractional reaction orders with respect to the CO partial pressures were measured for CO2 electroreduction (CO2R) on Au under mass-transfer-controlled conditions using a rotating ring-disk electrode setup. At high overpotentials, the CO reaction order approaches -1 due to enhanced CO adsorption on Au, which is supported by kinetic analysis and density functional theory (DFT) simulations. This work illustrates that the CO site-blocking effect cannot be ignored, even on a weak CO-binding metal such as Au in the electrochemical environment. The CO site-blocking effect can greatly hamper the activity and the selectivity of the CO2R to CO. This observation enriches the current mechanistic understanding of the CO2R and could have significant implications not only in the theoretical modeling of the CO2R but also in the evaluation of intrinsic CO2R activity at practical current density and high conversion conditions.

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Lattice strain is widely investigated to improve the performance of heterogeneous catalysts, however, the effect of lattice strain is under-explored in high-entropy oxide based photocatalyst. In this study, noble-metal-free (CoCrMnFeNi)Ox with lattice strain is synthesized using a temperature-controlled, template-free and salt-assisted strategy. In the presence of lattice strain, an intensive internal electric field is formed in (CoCrMnFeNi)Ox, promoting the separation of photoinduced charge carriers. The size of the (CoCrMnFeNi)Ox can be tuned by varying the calcination temperature. Specifically, (CoCrMnFeNi)Ox prepared at a higher temperature possesses a smaller grain size exposing more active sites, resulting in an enhanced CO2 photomethanation performance. This work provides valuable insights for the rational design of the photocatalysts and highlights the promising role of high-entropy oxides in heterogeneous photocatalysis.

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Employing water as a hydrogen source to participate in the hydrogen atom transfer (HAT) process is a low-cost and carbon-free process demonstrating great economic and environmental potential in catalysis. However, the low efficiency of hydrogen atom abstraction from water leads to slow kinetics of HAT for most hydrogenative reactions. Here, we prepared ultrathin Bi4O5Cl2 nanosheets where the surface can be in situ reconstructed via hydroxylation under light illumination to facilitate the abstraction of hydrogen atoms from pure water for efficient nitrogen fixation. Consequently, the isotope labeling in situ Fourier-transform infrared spectroscopy (FT-IR) involving H2O and D2O has clearly revealed that the hydroxyl groups tend to be adsorbed on the chloride vacancy sites on the Bi4O5Cl2 surface to form hydroxylated surfaces, where the hydroxylated photocatalyst surface enables partial dehydrogenation of water into H2O2, allowing the utilization of H atoms for efficient of N2 hydrogenation via HAT steps. This work elucidates the in-depth reaction mechanism of hydrogen atom extraction from H2O molecules via the light-generated chloride vacancy to promote photocatalytic nitrogen fixation, ultimately enabling the inspiration and providing crucial rules for the design of important functional materials that can efficiently deliver active hydrogen for chemical synthesis.

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We apply the Lang-Firsov (LF) transformation to electron-boson coupled Hamiltonians and variationally optimize the transformation parameters and molecular orbital coefficients to determine the ground state. Møller-Plesset (MP-n, with n = 2 and 4) perturbation theory is then applied on top of the optimized LF mean-field state to improve the description of electron-electron and electron-boson correlations. The method (LF-MP) is applied to several electron-boson coupled systems, including the Hubbard-Holstein model, diatomic molecule dissociation (H2, HF), and the modification of proton transfer reactions (malonaldehyde and aminopropenal) via the formation of polaritons in an optical cavity. We show that with a correction for the electron-electron correlation, the method gives quantitatively accurate energies comparable to that by exact diagonalization or coupled-cluster theory. The effects of multiple photon modes, spin polarization, and the comparison to the coherent state MP theory are also discussed.

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block2 is an open source framework to implement and perform density matrix renormalization group and matrix product state algorithms. Out-of-the-box it supports the eigenstate, time-dependent, response, and finite-temperature algorithms. In addition, it carries special optimizations for ab initio electronic structure Hamiltonians and implements many quantum chemistry extensions to the density matrix renormalization group, such as dynamical correlation theories. The code is designed with an emphasis on flexibility, extensibility, and efficiency and to support integration with external numerical packages. Here, we explain the design principles and currently supported features and present numerical examples in a range of applications.

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Characterizing the electronic structure of the iron-sulfur clusters in nitrogenase is necessary to understand their role in the nitrogen fixation process. One challenging task is to determine the protonation state of the intermediates in the nitrogen fixing cycle. Here, we use a dimeric iron-sulfur model to study relative energies of protonation at C, S, or Fe. Using a composite method based on coupled cluster and density matrix renormalization group energetics, we converge the relative energies of four protonated configurations with respect to basis set and correlation level. We find that accurate relative energies require large basis sets as well as a proper treatment of multireference and relativistic effects. We have also tested ten density functional approximations for these systems. Most of them give large errors in their relative energies. The best performing functional in this system is B3LYP, which gives mean absolute and maximum deviations of only 10 and 13 kJ/mol with respect to our correlated wave function estimates, respectively, comparable to the uncertainty in our correlated estimates. Our work provides benchmark results for the calibration of new approximate electronic structure methods and density functionals for these problems.

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Due to intense interest in the potential applications of quantum computing, it is critical to understand the basis for potential exponential quantum advantage in quantum chemistry. Here we gather the evidence for this case in the most common task in quantum chemistry, namely, ground-state energy estimation, for generic chemical problems where heuristic quantum state preparation might be assumed to be efficient. The availability of exponential quantum advantage then centers on whether features of the physical problem that enable efficient heuristic quantum state preparation also enable efficient solution by classical heuristics. Through numerical studies of quantum state preparation and empirical complexity analysis (including the error scaling) of classical heuristics, in both ab initio and model Hamiltonian settings, we conclude that evidence for such an exponential advantage across chemical space has yet to be found. While quantum computers may still prove useful for ground-state quantum chemistry through polynomial speedups, it may be prudent to assume exponential speedups are not generically available for this problem.

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ABSTRACT Introduction: Synchronized swimming is a sport of artistic expression, skill, and physical fitness. Explosive, high-intensity movements rely mainly on the athlete's good basal strength. Although China attaches great importance to the physical training of synchronized swimming athletes, there is no theoretical achievement in consolidating specific training. Objective: To analyze the impact of CORE strengthening on the physical training of synchronized swimming athletes. Methods: This article selects 30 synchronized swimmers as volunteers for the research. A basal metabolism test was used to verify the maximal oxygen consumption (VO2max), ventilatory anaerobic threshold (VT), and other indicators. The isokinetic force measurement system measured the athletes' maximum lumbar-abdominal muscle flexion/extension torque, explosive strength, fast muscle strength capacity, total work, and anti-fatigue capacity. Results: The synchronized limb training results of the swimming team were positively correlated with the stability of the CORE muscles. There is a positive relationship between 30 years old and maximal strength training and performance in athletes. Abdominal muscular endurance showed the highest correlation coefficient with synchronized swimming performance. Conclusion: Coaches should organize adequate strength training according to the growth and development characteristics of athletes and the characteristics of synchronized swimming movements. In this way, an excellent physical training effect can be achieved by CORE training. Level of evidence II; Therapeutic studies - investigation of treatment outcomes.

RESUMO Introdução: O nado sincronizado é um esporte de expressão artística, habilidade e aptidão física. Movimentos explosivos, de alta intensidade, dependem principalmente da boa força basal do atleta. Embora a China atribua grande importância ao treinamento físico de atletas do nado sincronizado, não há conquista teórica na consolidação de um treinamento específico. Objetivo: Analisar o impacto da aplicação do fortalecimento do core sobre o treinamento físico de atletas do nado sincronizado. Métodos: Este artigo seleciona 30 nadadores sincronizados como voluntários para a pesquisa. Um teste de metabolismo basal foi utilizado para verificar o consumo máximo de oxigênio (VO2max), o limiar anaeróbico ventilatório (VT) e outros indicadores. Utilizou-se o sistema de medição de força isocinética para medir o torque máximo de flexão/extensão muscular lombar-abdominal dos atletas, força explosiva, capacidade de força rápida muscular, trabalho total e capacidade anti-fadiga. Resultados: Os resultados de treinamento dos membros sincronizados da equipe de natação foram positivamente correlacionados com a estabilidade dos músculos do core. Há uma relação positiva entre os 30 anos de idade e o melhor desempenho no treinamento de força máxima em atletas. A resistência muscular abdominal apresentou o maior coeficiente de correlação com desempenho sincronizado de natação. Conclusão: Os treinadores devem organizar o treinamento de força adequado de acordo com as características de crescimento e desenvolvimento dos atletas e as características dos movimentos sincronizados de natação. Desta forma, um excelente efeito de treinamento físico pode ser alcançado pelo treino do core. Nível de evidência II; Estudos terapêuticos - investigação dos resultados do tratamento.

RESUMEN Introducción: La natación sincronizada es un deporte de expresión artística, de habilidad y de condición física. Los movimientos explosivos y de alta intensidad dependen principalmente de la buena fuerza basal del deportista. Aunque China atribuye una gran importancia a la preparación física de las atletas de natación sincronizada, no existe ningún logro teórico en la consolidación de un entrenamiento específico. Objetivo: Analizar el impacto de la aplicación del fortalecimiento del core en la preparación física de las atletas de natación sincronizada. Métodos: En este artículo se seleccionan 30 nadadores de sincronizados como voluntarios para la investigación. Se utilizó una prueba de metabolismo basal para verificar el consumo máximo de oxígeno (VO2max), el umbral anaeróbico ventilatorio (VT) y otros indicadores. Fue aplicado el sistema de medición de la fuerza isocinética para medir el par máximo de flexión/extensión de los músculos lumbares-abdominales de los atletas, la fuerza explosiva, la capacidad de fuerza muscular rápida, el trabajo total y la capacidad antifatiga. Resultados: Los resultados del entrenamiento de las extremidades sincronizadas del equipo de natación se correlacionaron positivamente con la estabilidad de los músculos del core. Existe una relación positiva entre los 30 años de edad y la fuerza máxima de entrenamiento y el rendimiento en los atletas. La resistencia muscular abdominal mostró el mayor coeficiente de correlación con el rendimiento de la natación sincronizada. Conclusión: Los entrenadores deben organizar un entrenamiento de fuerza adecuado en función de las características de crecimiento y desarrollo de los deportistas y de las características de los movimientos de la natación sincronizada. De este modo, se puede conseguir un excelente efecto de entrenamiento físico entrenando el core. Nivel de evidencia II; Estudios terapéuticos - investigación de los resultados del tratamiento.

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ABSTRACT Introduction: Sports injuries restrict the acquisition of optimal results and represent a great threat to the athlete's physical health, lower limb injuries being the most prominent, mainly those caused by landing. Objective: Use biomechanics to analyze the joint load of the lower limbs during the landing process in the gymnastics backflip, establishing movement control and reducing the risk of lower limb injury. Methods: The male athletes of the National Gymnastics Team were selected as the research objects, and the three-dimensional backflip (BS) motion trajectory was completed after the landing process was completed, the vertical ground reaction force (VGRF) after landing and the lower limb muscle electromyography (EMG) after landing was collected, and the human multi-body system model and the landing platform model of the landing action were completed with the help of the system simulation software. Results: Statistics show that gymnasts train more intensively during competition or daily training, performing more than 200 landings per week, a factor that increases the risk of injuries during the backflip in athletes. Conclusion: The lower limb joint load of the landing action in gymnastics backflip is high, which will cause a certain risk of injury, and specific measures can be taken to control it. Level of evidence II; Therapeutic studies - investigation of treatment outcomes.

RESUMO Introdução: Lesões esportivas restringem a aquisição dos resultados ótimos e representam uma grande ameaça à saúde física do esportista, sendo as lesões nos membros inferiores as mais proeminentes, majoritariamente as causadas pela aterrissagem. Métodos: Os atletas masculinos da Equipe Nacional de Ginástica foram selecionados como objetos de pesquisa, e a trajetória de movimento tridimensional do backflip (BS) foi completada após a conclusão do processo de aterrissagem, a força vertical de reação ao solo (VGRF) após a aterrissagem e a eletromiografia do músculo do membro inferior (EMG) após a coleta do pouso, e o modelo do sistema humano de multicorpos e o modelo da plataforma de aterrissagem da ação de aterrissagem foram completados com a ajuda do software de simulação do sistema. Resultados: As estatísticas mostram que os ginastas treinam mais intensamente durante a competição ou no treinamento diário, efetuando mais de 200 aterrissagens semanais, fator que aumenta o risco de lesões durante o backflip nos atletas. Conclusão: A carga articular dos membros inferiores da ação de aterrissagem no backflip da ginástica é alta, o que causará um certo risco de ferimentos, e medidas específicas podem ser tomadas para controlá-lo. Nível de evidência II; Estudos terapêuticos - investigação dos resultados do tratamento.

RESUMEN Introducción: Las lesiones deportivas limitan la obtención de resultados óptimos y representan una gran amenaza para la salud física del deportista, siendo las lesiones en los miembros inferiores las más destacadas, principalmente las causadas por el aterrizaje. Objetivo: Utilizar la biomecánica para analizar la carga articular de los miembros inferiores durante el proceso de aterrizaje en el backflip gimnástico, estableciendo el control del movimiento y reduciendo el riesgo de lesiones en los miembros inferiores. Métodos: Se seleccionaron como objetos de investigación los atletas masculinos del Equipo Nacional de Gimnasia, y se completó la trayectoria de movimiento tridimensional del backflip (BS) tras el proceso de aterrizaje, se recogió la fuerza de reacción vertical del suelo (VGRF) tras el aterrizaje y la electromiografía (EMG) de los músculos de las extremidades inferiores tras el aterrizaje, y se completó el modelo del sistema multicuerpo humano y el modelo de la plataforma de aterrizaje de la acción de aterrizaje con la ayuda del software de simulación de sistemas. Resultados: Las estadísticas muestran que los gimnastas entrenan más intensamente durante la competición o el entrenamiento diario, realizando más de 200 aterrizajes a la semana, un factor que aumenta el riesgo de lesión durante el backflip en los atletas. Conclusión: La carga de la articulación del miembro inferior en la acción de aterrizaje en el backflip de gimnasia es elevada, lo que provocará un cierto riesgo de lesión, y se pueden tomar medidas específicas para controlarla. Nivel de evidencia II; Estudios terapéuticos - investigación de los resultados del tratamiento.

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Cold stress is a significant environmental stimulus that negatively affects the health, production, and welfare of animals and birds. However, the specific effects of cold stimulation combined with lipopolysaccharide (LPS) on the mouse intestine remain poorly understood. Therefore, we designed this research to explore the effect of cold stimulation + LPS on mice intestine via microbiome and microbiota sequencing. Forty-eight mice were randomly divided into four experimental groups (n = 12): Control (CC), LPS-induced (CL), cold normal saline-induced (MC) and LPS + cold normal saline-induced (ML). Our results showed body weight was similar among different groups of mice. However, the body weight of mice in groups CC and CL were slightly higher compared to those in groups MC and ML. The results of gene expressions reflected that CL and ML exposure caused gut injury and barrier dysfunction, as evident by decreased ZO-1, OCCLUDIN (P < 0.01), and CASPASE-1 (P < 0.01) expression in the intestine of mice. Moreover, we found that cold stress induced oxidative stress in LPS-challenged mice by increasing malondialdehyde (MDA) accumulation and decreasing the antioxidant capacity [glutathione peroxidase (GSH-Px), superoxide dismutase (SOD), total and antioxidant capacity (T-AOC)]. The cold stress promoted inflammatory response by increased IL-1ß in mice treated with cold normal saline + LPS. Whereas, microbiome sequencing revealed differential abundance in four phyla and 24 genera among the mouse groups. Metabolism analysis demonstrated the presence of 4,320 metabolites in mice, with 43 up-regulated and 19 down-regulated in CC vs. MC animals, as well as 1,046 up-regulated and 428 down-regulated in ML vs. CL animals. It is Concluded that cold stress enhances intestinal damage by disrupting the balance of gut microbiota and metabolites, while our findings contribute in improving management practices of livestock in during cold seasons.

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A novel Zn benzotriazolate metal-organic framework (MOF), [Zn9(OAc)6(bbtm)6] (1, bbtm2- = bis(benzotriazolyl)methanone, OAc- = acetate), has been synthesized and structurally characterized using micro-crystal electron diffraction. The framework contains 12-connected nonanuclear Zn clusters with Zn-OAc groups separated by short intercluster Zn···Zn distances of 6.06 Å. Postsynthetic OAc-/OH- ligand exchange followed by thermal activation generates 1a-OH, which adsorbs CO2 at very low pressures (1.37 mmol/g at 2.5 mbar) and requires an unusually high desorption temperature (>160 °C). Diffuse reflectance IR Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations have been used to interrogate the CO2 binding mechanism in 1a-OH. The formation of unsymmetric bridging carbonate ligands within the Zn···Zn pockets accompanied by strong hydrogen bonding of the carbonate with a neighboring zinc aqua ligand explains the remarkably strong CO2 affinity of 1a-OH.

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Deoxygenation of aldehydes and their tautomers to alkenes and alkanes has implications in refining biomass-derived fuels for use as transportation fuel. Electrochemical deoxygenation in ambient, aqueous solution is also a potential green synthesis strategy for terminal olefins. In this manuscript, direct electrochemical conversion of vinyl alcohol and acetaldehyde on polycrystalline Cu to ethanol, ethylene and ethane; and propenol and propionaldehyde to propanol, propene and propane is reported. Sensitive detection was achieved using a rotating disk electrode coupled with gas chromatography-mass spectrometry. In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy, and in-situ Raman spectroscopy confirmed the adsorption of the vinyl alcohol. Calculations using canonical and grand-canonical density functional theory and experimental findings suggest that the rate-determining step for ethylene and ethane formation is an electron transfer step to the adsorbed vinyl alcohol. Finally, we extend our conclusions to the enol reaction from higher-order soluble aldehyde and ketone. The products observed from the reduction reaction also sheds insights into plausible reaction pathways of CO2 to C2 and C3 products.

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The quantitative description of correlated electron materials remains a modern computational challenge. We demonstrate a numerical strategy to simulate correlated materials at the fully ab initio level beyond the solution of effective low-energy models and apply it to gain a detailed microscopic understanding across a family of cuprate superconducting materials in their parent undoped states. We uncover microscopic trends in the electron correlations and reveal the link between the material composition and magnetic energy scales through a many-body picture of excitation processes involving the buffer layers. Our work illustrates a path toward a quantitative and reliable understanding of more complex states of correlated materials at the ab initio many-body level.

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The gut microbiome is highly linked to inflammatory bowel disease (IBD). A total of 3890 publications related to the two terms from 2000 to 2020 were extracted from the Web of Science Core Collection to study the association from a bibliometric perspective. Publications on this topic have grown rapidly since 2008. The United States and Harvard University are the country and institution with the largest number of publications, respectively. Inflammatory Bowel Diseases is the most productive journal with 211 published articles. The most influential journal in this field is Gut with 13,359 citations. The co-citation analysis of references showed that the IBD-related topics with the highest focus are "gut microbiota," "metagenomics," "bacterial community," "fecal microbiota transplantation," "probiotics," and "colitis-associated colorectal cancer." Keyword cluster and keyword burst analyses showed that "gut microbiota," "metagenomics," and "fecal microbiota transplantation" are currently the most researched topics in the field of IBD. The literature in this field is mainly distributed between alterations of the intestinal microbiota, microbial metabolites, and related host signaling pathways. Probiotic treatment also frequently appears in literature. This bibliometric analysis can guide future research and promote the development of the field of gut microbiome and IBD.

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Simulating photosynthesis has long been one of the ideas for realizing the conversion of solar energy into industrial chemicals. Heterogeneous N2 photofixation in water is a promising way for sustainable production of ammonia. However, a mechanistic understanding of the complex aqueous photocatalytic N2 reduction is still lacking. In this study, a light-dependent surface hydrogenation mechanism and light-independent protection of catalyst surface for N2 reduction are revealed on ultrathin Bi4 O5 Br2 (BOB) nanosheets, in which the creation and annihilation of surface bromine vacancies can be controlled via a surface bromine cycle. Our rapid scan in situ FT-IR spectra verify that photocatalytic N2 reduction proceeds through an associative alternating mechanism on BOB surface with bromine vacancies (BrV-BOB). This work provides a new strategy to combine light-dependent facilitated reaction with light-independent regeneration of catalyst for advancing sustainable ammonia production.

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Although various single-atom catalysts have been designed, atomically engineering their coordination environment remains a great challenge. Herein, a one-pot template-sacrificing pyrolysis approach is developed to synthesize well-defined Ni-N4-O catalytic sites on highly porous graphitic carbon for electrocatalytic CO2 reduction to CO with high Faradaic efficiency (maximum of 97.2%) in a wide potential window (-0.56 to -1.06 V vs RHE) and with high stability. In-depth experimental and theoretical studies reveal that the axial Ni-O coordination introduces asymmetry to the catalytic center, leading to lower Gibbs free energy for the rate-limiting step, strengthened binding with *COOH, and a weaker association with *CO. The present results demonstrate the successful atomic-level coordination environment engineering of high-surface-area porous graphitic carbon-supported Ni single-atom catalysts (SACs), and the demonstrated method can be applied to synthesize an array of SACs (metal-N4-O) for various catalysis applications.

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Density matrix embedding theory (DMET) formally requires the matching of density matrix blocks obtained from high-level and low-level theories, but this is sometimes not achievable in practical calculations. In such a case, the global band gap of the low-level theory vanishes, and this can require additional numerical considerations. We find that both the violation of the exact matching condition and the vanishing low-level gap are related to the assumption that the high-level density matrix blocks are noninteracting pure-state v-representable (NI-PS-V), which assumes that the low-level density matrix is constructed following the Aufbau principle. To relax the NI-PS-V condition, we develop an augmented Lagrangian method to match the density matrix blocks without referring to the Aufbau principle. Numerical results for the 2D Hubbard and hydrogen model systems indicate that, in some challenging scenarios, the relaxation of the Aufbau principle directly leads to exact matching of the density matrix blocks, which also yields improved accuracy.

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Lithium iron phosphate (LiFePO4) batteries have been dominant in energy storage systems. However, it is difficult to estimate the state of charge (SOC) and safety early warning of the batteries. To solve these problems, this paper developed a multiple timescale comprehensive early warning strategy based on the consistency deviation of the electrical and thermal characteristics of LiFePO4 batteries. The unscented Kalman filter method was employed to estimate the battery SOC. The established comprehensive early warning strategy was verified through fault-triggered experiments at different time scales with different equivalent resistances. The results show that the comprehensive early warning strategy can realize early warning for different timescale failures of LiFePO4 batteries under different energy storage conditions. For more dangerous severe failures that can break the safety valve, safety early warning can be realized 15 min in advance. This study provides a reference to ensure safe and reliable operations of energy storage systems.

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Drosophila suzukii (Diptera: Drosophilidae) infests a variety of commercial fruits, including cherries and other soft-skinned fruits. After the cropping season of most cultivated crop hosts, it heavily infests the fruit of a wild host-plant, Osyris wightiana in southwest China. Here, we employ gas chromatography-electroantennographic detection (GC-EAD) together with behavioral bioassays and a trapping experiment to identify volatile semiochemicals emitted by O. wightiana that are involved in D. suzukii attraction. GC-EAD recordings of D. suzukii antenna showed responses to 13 compounds, including α-pinene, 3-methylbutyl acetate, 2-hexanol, E-ß-ocimene, Z-3-hexenol, ß-caryophyllene, α-humulene, and six unidentified compounds. The flies were attracted by seven individual EAD-active compounds at low doses (0.01 and 0.1 µg), but were repelled at high doses (10 and 100 µg). In a similar manner, a blend of seven EAD-active compounds at low doses (0.1 and 1 µg) was attractive to female flies, but became repulsive at high doses (10 µg). The low dose of the blend was as attractive as the fruit volatiles, although both were less attractive than the fruits. The blend attracted both female and male D. suzukii and other Drosophila flies. The percentage of D. suzukii out of all flies captured by the blend was significantly greater than that captured by the control. These results indicate that the EAD-active volatile compounds emitted by fruits of O. wightiana play an important role in D. suzukii attraction, and have the potential to be used for management of D. suzukii.