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Polymer dielectrics with excellent capacitive performance are urgently needed in advanced electrical and electronic systems. However, due to the dramatic increase in the conduction loss, the energy density and efficiency of polymers degrade severely at elevated temperatures, limiting their application in harsh environments up to 150 °C. Herein, an all-organic polyurea (PU)/polyetherimide (PEI) blend film is designed to prepare high-temperature polymer dielectric. It is found that carrier traps can be introduced by blending, and the hydrogen bond between PU and PEI increases the trap depth, leading to suppressed leakage current and enhanced breakdown strength, thus improving the energy storage performance. PU/30%PEI exhibits a high discharged energy density of ∼3.74 J/cm3 with an efficiency higher than 90% at 150 °C, which is 78% and 70% higher than pristine PU and PEI, respectively. This work provides a facile strategy to improve the energy storage performance of polymer dielectrics by introducing deep traps through blending. [ABSTRACT FROM AUTHOR]

Due to the potential applications in biomedical engineering, it becomes more and more important to understand the process of engulfment and internalization of nanoparticles (NPs) by cell membranes. Despite the fact that the interaction between cell membranes and passive particles has been widely studied, the interaction between cell membranes and self-propelled nonspherical NPs remains to be elucidated. Here, we present a theoretical model to systematically investigate the influence of the active force, aspect ratio of NPs, particle size, and membrane properties (adhesion energy density and membrane tension) on the cellular uptake of a nonspherical nanoparticle. It is found that the active force generated by an NP can trigger a type of first-order wrapping transition from a small partial wrapping state to a large one. In addition, the phase diagram in the force-aspect ratio (particle size, adhesion energy density, and membrane tension) space displays more complex behaviors compared with that for the passive wrapping mediated merely by adhesion. These results may provide useful guidance to the study of activity-driven cellular entry of active particles into cells. [ABSTRACT FROM AUTHOR]

X-ray free electron laser (XFEL) sources coupled to high-power laser systems offer an avenue to study the structural dynamics of materials at extreme pressures and temperatures. The recent commissioning of the DiPOLE 100-X laser on the high energy density (HED) instrument at the European XFEL represents the state-of-the-art in combining x-ray diffraction with laser compression, allowing for compressed materials to be probed in unprecedented detail. Here, we report quantitative structural measurements of molten Sn compressed to 85(5) GPa and ∼ 3500 K. The capabilities of the HED instrument enable liquid density measurements with an uncertainty of ∼ 1 % at conditions which are extremely challenging to reach via static compression methods. We discuss best practices for conducting liquid diffraction dynamic compression experiments and the necessary intensity corrections which allow for accurate quantitative analysis. We also provide a polyimide ablation pressure vs input laser energy for the DiPOLE 100-X drive laser which will serve future users of the HED instrument. [ABSTRACT FROM AUTHOR]

The analysis of water density fluctuations in the hydration shell of nonpolar solutes provides insights into water-mediated interactions, especially hydrophobic interactions. These fluctuations are sensitive to small perturbations due to changes in thermodynamic conditions, such as temperature and pressure, but also to the presence of cosolutes, such as salts or small organic molecules. Herein, we investigate the effect of two classes of adsorbing cosolutes, using urea and methanol as representatives, on the fluctuations in energy and solvent density within the solvation shell of a model extended hydrophobic solute. We focus on the interactions of the cosolutes with the hydrophobic hydration shell, rather than with the solute itself, which though important remain largely unexplored. We calculate and analyze the interfacial partial molar energy of the cosolute, using a methodology based on the small system method. This approach provides correlated solvent density and energy fluctuations and allows us to decompose them into contributions due to interactions between the different components present in the solvation shell of the solute. The results show that adsorbed urea molecules interact more favorably with water than nonadsorbed urea molecules, which leads to the attenuation of interfacial density fluctuations and thus to the stabilization of the solvation shell. By contrast, the adsorbed methanol molecules interact preferably with other methanol molecules in the solvation shell, leading to a nano-phase segregated structure, which enhances interfacial fluctuations. [ABSTRACT FROM AUTHOR]

Metal–Organic Polymers (MOPs) have attracted growing attention for lithium-ion battery (LIB) applications due to their merits in orderly ionic transportation and robust structure stability in electrochemical reactions. However, they suffer from poor electronic conductivity. In this work, we apply first-principles density functional theory to explore the potential of three one-dimensional (1D) electrically conductive C6H2S4TM (TM = Fe, Co, and Ni) MOPs with the π–d conjugated coordination as anode materials for Li+ ions storage. Our theoretical results reveal that these 1D MOPs possess a superior theoretical capacity of over 748 mA h g−1. In particular, the 1D C6H2S4Ni MOP shows an exceptional theoretical specific capacity of 1110 mA h g−1 based on the three-electron transferring reaction, which significantly outperforms the traditional graphite-based anode material in LIBs. Moreover, the resonant charge transfer between Ni metal and ligand within the 1D C6H2S4Ni MOP reduces the diffusion energy barrier of the Li atoms when they migrate on the surface of the MOP. The ultrahigh theoretical specific capacity of the C6H2S4Ni MOP predicts that it can be a promising anode material for LIBs. [ABSTRACT FROM AUTHOR]

This study explores the feasibility of precisely tuning the resistive switching behavior of Au/BiFeO 3 /Pt/Ti/SiO 2 /Si memristors through controlled modulation of laser energy density during pulsed laser deposition (PLD). By systematically reducing the laser energy density within the fabrication process, notable alterations in the properties of the BiFeO 3 (BFO) thin film are observed. As the laser energy density decreases, the grain size in the BFO film and the thickness of the film decrease. Furthermore, we obtain the minute structural variations in response to the diverse laser energy densities employed during the deposition process. Energy-dispersive x-ray spectroscopy analysis is employed to investigate the distribution of Ti 4 + ions within the BFO thin film. The reduction in the grain size and film thickness, along with the prominent nucleation of specifically oriented grains, and the diffusion of Ti 4 + ions, lead to the BFO memristor fabricated with a lower laser energy density having more grain boundaries and a shortened conduction path (grain boundary) in the thickness direction. Consequently, the enhanced movement of oxygen vacancies facilitates their preferential accumulation along the grain boundaries within the BFO layer, resulting in an augmented on/off ratio, rectification factor, and set current in the devices. Overall, our findings explain the significant influence of laser energy density in PLD on the microstructure and electrical properties of BFO thin films. Particularly, the lower energy densities are employed to improve electrical characteristics. This research not only enhances our fundamental understanding but also provides valuable insights into optimizing BFO memristors for reliable, robust, and practical applications. [ABSTRACT FROM AUTHOR]

The global demand for high energy density batteries, mostly for application in electric vehicles, offering increased durability, safety, and sustainability is growing rapidly. In the past, this demand has been met primarily by the development and/or improvement of new/established battery materials and technologies. The high-entropy design concept—aiming at increasing chemical complexity/occupational disorder—has recently been introduced into the field of electrochemical energy storage. Various high-entropy battery materials that are seemingly capable of outperforming low-entropy counterparts by offering desirable properties have been reported. However, future studies are required to explore if the concept is broadly applicable and can be extended to all types of battery materials, especially those that are of industrial relevance. Herein, we provide a brief overview of the existing high-entropy anodes, cathodes, and solid/liquid electrolytes for use in rechargeable Li- or Na-ion batteries and discuss potential research directions and opportunities. [ABSTRACT FROM AUTHOR]

A Landau–Devonshire thermodynamic energy density function for ferroelectric wurtzite aluminum scandium nitride (Al1−xScxN) solid solution is developed. It is parametrized using available experimental and theoretical data, enabling the accurate reproduction of composition-dependent ferroelectric properties, such as spontaneous polarization, dielectric permittivity, and piezoelectric constants, for both bulk and thin films. The maximum concentration of Sc for the wurtzite structure to remain ferroelectric is found to be 61 at. %. A detailed analysis of Al1−xScxN thin films reveals that the ferroelectric phase transition and properties are insensitive to substrate strain. This study lays the foundation for quantitative modeling of novel ferroelectric wurtzite solid solutions. [ABSTRACT FROM AUTHOR]

Dielectric capacitors prepared by antiferroelectric (AFE) materials have the advantages of large power density and fast discharge ability. It has been a focus on the improvement of the recoverable energy density (Wrec) and discharge energy–density (Wdis) in the AFE ceramics. To address the above issue, optimizing the proportion of components is proposed for enhancing ceramic antiferroelectricity, ultimately improving the breakdown strength (Eb) and Wrec. In this work, an ultrahigh Wrec (14.3 J/cm3) with an excellent energy efficiency (η) of 81.1% is obtained in (Pb0.96Sr0.02La0.02)(Hf0.9Sn0.1)O3 AFE ceramic at electric field of 490 kV/cm, which is the maximum value reported in lead-based AFE ceramics fabricated by the conventional solid-state reaction method so far. The multistage phase transition induced by the electric field is observed in the polarization–electric field (P–E) hysteresis loops. Furthermore, an outstanding power density (PD) of 335 MW/cm3 and an excellent Wdis of 8.97 J/cm3 with a rapid discharge speed (102 ns) are obtained at electric field of 390 kV/cm. In addition, (Pb0.96Sr0.02La0.02)(Hf0.9Sn0.1)O3 ceramics also possess an excellent thermal and frequency stability. These exceptional properties indicate that (Pb0.98−xSrxLa0.02)(Hf0.9Sn0.1)O3 ceramics are a potential candidate for pulsed power devices and power electronic devices. [ABSTRACT FROM AUTHOR]

Recently developed locally scaled self-interaction correction (LSIC) is a one-electron SIC method that, when used with a ratio of kinetic energy densities (zσ) as iso-orbital indicator, performs remarkably well for both thermochemical properties as well as for barrier heights overcoming the paradoxical behavior of the well-known Perdew–Zunger self-interaction correction (PZSIC) method. In this work, we examine how well the LSIC method performs for the delocalization error. Our results show that both LSIC and PZSIC methods correctly describe the dissociation of H 2 + and He 2 + but LSIC is overall more accurate than the PZSIC method. Likewise, in the case of the vertical ionization energy of an ensemble of isolated He atoms, the LSIC and PZSIC methods do not exhibit delocalization errors. For the fractional charges, both LSIC and PZSIC significantly reduce the deviation from linearity in the energy vs number of electrons curve, with PZSIC performing superior for C, Ne, and Ar atoms while for Kr they perform similarly. The LSIC performs well at the endpoints (integer occupations) while substantially reducing the deviation. The dissociation of LiF shows both LSIC and PZSIC dissociate into neutral Li and F but only LSIC exhibits charge transfer from Li+ to F− at the expected distance from the experimental data and accurate ab initio data. Overall, both the PZSIC and LSIC methods reduce the delocalization errors substantially. [ABSTRACT FROM AUTHOR]

In this work, the electrostatic response of an electrolyte solution to a spherical ion is studied with a Gaussian field theory. In order to capture the ionic correlation effect in concentrated solutions, the bulk dielectric response function is described by a two-Yukawa response function. The modified response function of the solution is solved analytically in the spherical geometry, from which the induced charge density and the electrostatic energy are also derived analytically. Comparisons with results for small ions in electrolyte solutions from the hyper-netted chain theory demonstrate the validity of the Gaussian field theory. [ABSTRACT FROM AUTHOR]

We present a derivation of the screening length for a solution containing a charge-regulated macroion, e.g. protein, with its counterions. We show that it can be obtained directly from the second derivatives of the total free energy by taking recourse to the "uncertainty relation" of the Legendre transform, which connects the Hessians or the local curvatures of the free energy as a function of density and its Legendre transform, i.e., osmotic pressure, as a function of chemical potentials. Based on the Fowler–Guggenheim–Frumkin model of charge regulation, we then analyze the "screening resonance" and the "overscreening" of the screening properties of the charge-regulated macroion solution. [ABSTRACT FROM AUTHOR]

Electrochemical Double Layer Capacitors (EDLCs) with ionic liquid electrolytes outperform conventional ones using aqueous and organic electrolytes in energy density and safety. However, understanding the electrochemical behaviors of ionic liquid electrolytes under compressive/tensile strain is essential for the design of flexible EDLCs as well as normal EDLCs, which are subject to external forces during assembly. Despite many experimental studies, the compression/stretching effects on the performance of ionic liquid EDLCs remain inconclusive and controversial. In addition, there is hardly any evidence of prior theoretical work done in this area, which makes the literature on this topic scarce. Herein, for the first time, we developed an atomistic model to study the processes underlying the electrochemical behaviors of ionic liquids in an EDLC under strain. Constant potential non-equilibrium molecular dynamics simulations are conducted for EMIM BF4 placed between two graphene walls as electrodes. Compared to zero strain, low compression of the EDLC resulted in compromised performance as the electrode charge density dropped by 29%, and the performance reduction deteriorated significantly with a further increase in compression. In contrast, stretching is found to enhance the performance by increasing the charge storage in the electrodes by 7%. The performance changes with compression and stretching are due to changes in the double-layer structure. In addition, an increase in the value of the applied potential during the application of strain leads to capacity retention with compression revealed by the newly performed simulations. [ABSTRACT FROM AUTHOR]

One of the well-known limitations of Kohn–Sham density functional theory is the tendency to strongly underestimate bandgaps. Meta-generalized gradient approximations (mGGAs), which include the kinetic energy density in the functional form, have been shown to significantly alleviate this deficiency. In this study, we explore the mechanisms responsible for this improvement from the angle of the underlying local densities. We find that the highest occupied and lowest unoccupied states are distinct in the space of the underlying descriptors. The gap opening is compared to a simple scaling of the local density approximation, and two mechanisms responsible for opening the mGGA gaps are identified. First of all, the relatively large negative derivative of the functional form with respect to reduced kinetic energy tends to elevate the lowest unoccupied state. Second, the curvature of functional, which ensures that it is bounded, tends to lower the highest occupied state. Remarkably, these two mechanisms are found to be transferable over a large and diverse database of compounds. [ABSTRACT FROM AUTHOR]

Understanding the interfacial phonon transport is essential for optimizing the thermal management of microelectronics, especially for high energy density devices. Some calculations have suggested that introducing interfacial defects or disorders will increase the interfacial thermal conductance, which helps heat dissipation, while some studies suggested otherwise. In this work, we introduced substitutional impurities in GaN by growing a ∼2-nm-thick AlxGa1−xN or InxGa1−xN alloyed interlayer at the Al/GaN interface and measured the interface thermal conductance by time-domain thermoreflectance at room temperature. Our results show that substituting Ga atoms near the interface with either lighter Al atoms or heavier In atoms at a nominal concentration of 20% or less will not necessarily change the thermal conductance of the Al/alloy interface but is detrimental to the thermal transport across the total Al/GaN interface, which provides an experimental guideline for the thermal design of GaN-based devices. [ABSTRACT FROM AUTHOR]

Machine learning (ML) of kinetic energy functionals (KEFs), in particular kinetic energy density (KED) functionals, is a promising way to construct KEFs for orbital-free density functional theory (DFT). Neural networks and kernel methods including Gaussian process regression (GPR) have been used to learn Kohn–Sham (KS) KED from density-based descriptors derived from KS DFT calculations. The descriptors are typically expressed as functions of different powers and derivatives of the electron density. This can generate large and extremely unevenly distributed datasets, which complicates effective application of ML techniques. Very uneven data distributions require many training datapoints, can cause overfitting, and can ultimately lower the quality of an ML KED model. We show that one can produce more accurate ML models from fewer data by working with smoothed density-dependent variables and KED. Smoothing palliates the issue of very uneven data distributions and associated difficulties of sampling while retaining enough spatial structure necessary for working within the paradigm of KEDF. We use GPR as a function of smoothed terms of the fourth order gradient expansion and KS effective potential and obtain accurate and stable (with respect to different random choices of training points) kinetic energy models for Al, Mg, and Si simultaneously from as few as 2000 samples (about 0.3% of the total KS DFT data). In particular, accuracies on the order of 1% in a measure of the quality of energy–volume dependence B ′ = E V 0 − Δ V − 2 E V 0 + E ( V 0 + Δ V) Δ V / V 0 2 (where V0 is the equilibrium volume and ΔV is a deviation from it) are obtained simultaneously for all three materials. [ABSTRACT FROM AUTHOR]

We model near-field thermal emission from metasurfaces structured as two-dimensional arrays of ellipsoidal SiC particles. The modeling approach is developed from fluctuational electrodynamics and is applicable to systems of ellipsoidal particles within the dipole limit. In all simulations, the radial lengths of particles are restricted to the range of 10–100 nm, and interparticle spacing is constrained to at least three times the particle characteristic length. The orientation and dimensions of constituent ellipsoidal particles are varied to tune localized surface phonon resonances and control the near-field energy density above metasurfaces. Results show that particle orientation can be used to regulate the relative magnitude of resonances in the energy density, and particle dimensions may be changed to adjust the frequency of these resonances within the Reststrahlen band. Metasurfaces constructed from particles with randomized dimensions display comparatively broadband thermal emission rather than the three distinct resonances seen in metasurfaces made with ellipsoidal particles of equivalent dimensions. When the interparticle spacing in a metasurface exceeds about three times the particle characteristic length, the spectral energy density above the metasurface is dominated by individual particle self-interaction and can be approximated as a linear combination of single-particle spectra. When interparticle spacing is at the lower limit of three times the characteristic length, however, multiparticle interaction effects increase and the spectral energy density above a metasurface deviates from that of single particles. This work provides guidance for designing all-dielectric, particle-based metasurfaces with desired near-field thermal emission spectra, such as thermal switches. [ABSTRACT FROM AUTHOR]

Aqueous Zn-ion hybrid supercapacitors (AZHSCs) combining the advantages of high‐energy batteries and high‐power supercapacitors see a bright future, but they still suffer from the poor capacity of carbonic cathodes. Herein, a functionalized porous carbon cloth (denoted as FPCC) electrode is demonstrated based on commercial carbon cloth (denoted as CC) tuning by structural and surface engineering. The constructed exfoliated porous carbon layer and the negatively charged functionalized interface not only increase the electrical double layer capacitance but also favor the chemical adsorption of Zn2+ to obtain additional pseudocapacitance. Consequently, the FPCC electrode delivers a high capacity of 0.16 mAh cm−2 at 4 mA cm−2, which is 923.8 times higher than CC, and a long cycle life (85.0% capacity retention after 30 000 cycles). More importantly, the Zn//FPCC AZHSC possesses an impressive energy density (3.3 mWh cm−3) and power density (240 mW cm−3), superior to many advanced batteries and supercapacitors. The quasi-solid-state device is also assembled as a demo. This modification strategy may provide new opportunities for high-performance AZHSCs. [ABSTRACT FROM AUTHOR]

The high catalytic activity and specificity of enzymes can be used to pretreat biomass. Herein, the resourceful, reproducible, cheap, and crude protein-rich cottonseed meal (CM) is selected as a precursor and the protease in the K2CO3–KHCO3 buffer solution is used as the enzyme degradation substance to pretreat CM. The crude protein content is significantly reduced by the protease degradation, and, meanwhile, it results in a looser and porous structure of CM. What is more, it significantly reduces the amount of activator. In the subsequent carbonization process, the K2CO3–KHCO3 in the buffer solution is also used as an activating agent (the mass ratio of CM to activator is 2:1), and after carbonization, the O, S, and N doped porous carbon is obtained. The optimized PCM-800-4 exhibits high heteroatom contents and a hierarchical porous structure. The specific capacitance of the prepared porous carbon reaches up to 233 F g−1 in 6M KOH even when 10 mg of active material is loaded. In addition, a K2CO3–KHCO3/EG based gel electrolyte is prepared and the fabricated flexible capacitor exhibits an energy density of 15.6 Wh kg−1 and a wide temperature range (−25 to 100 °C). This study presents a simple enzymatic degradation and reduced activator dosage strategy to prepare a cottonseed meal derived carbon material and looks forward to preparing porous carbon using other biomass. [ABSTRACT FROM AUTHOR]

The revised, regularized Tao–Mo (rregTM) exchange-correlation density functional approximation (DFA) [A. Patra, S. Jana, and P. Samal, J. Chem. Phys. 153, 184112 (2020) and Jana et al., J. Chem. Phys. 155, 024103 (2021)] resolves the order-of-limits problem in the original TM formulation while preserving its valuable essential behaviors. Those include performance on standard thermochemistry and solid data sets that is competitive with that of the most widely explored meta-generalized-gradient-approximation DFAs (SCAN and r2SCAN) while also providing superior performance on elemental solid magnetization. Puzzlingly however, rregTM proved to be intractable for de-orbitalization via the approach of Mejía-Rodríguez and Trickey [Phys. Rev. A 96, 052512 (2017)]. We report investigation that leads to diagnosis of how the regularization in rregTM of the z indicator functions (z = the ratio of the von-Weizsäcker and Kohn–Sham kinetic energy densities) leads to non-physical behavior. We propose a simpler regularization that eliminates those oddities and that can be calibrated to reproduce the good error patterns of rregTM. We denote this version as simplified, regularized Tao–Mo, sregTM. We also show that it is unnecessary to use rregTM correlation with sregTM exchange: Perdew–Burke–Ernzerhof correlation is sufficient. The subsequent paper shows how sregTM enables some progress on de-orbitalization. [ABSTRACT FROM AUTHOR]

Dielectric energy storage capacitors offer great potential in pulsed power devices due to the high power density and fast charging-discharging rate. Designing a host material with high field-induced polarization is of importance for developing dielectric energy storage materials via further composition modulation. In this paper, we compare the microstructure, dielectric, and ferroelectric properties as well as the energy storage performance of samples K1/2Bi1/2TiO3(KBT), 75KBT-25BiFeO3 (KBTF25), and 88KBT-12Bi0.85Nd0.15FeO3 (KBNTF12) in detail. It is found that, among three samples, sample KBNTF12 possesses the most complex local structure coexisting of a four-distortions with different polarities; meanwhile, sample KBNTF12 behaves as a strong relaxor, thus giving a high field-induced polarization. Besides, sample KBNTF12 realizes the highest electric breakdown strength Eb among three samples, which is resorted to the highest resistivity of grain boundary. Highest ΔP and Eb of sample KBNTF12 among three samples render it achieve ultrahigh stored energy density Ws of 6.94 J/cm3, high recoverable energy density Wr of 5.23 J/cm3, and high efficiency η of 75.4%. Our work suggests that 88KBT-12BNF binary composition be an optimal candidate for dielectric energy storage ceramics. [ABSTRACT FROM AUTHOR]

In a recent study, we developed a kinetic-energy density functional that can be utilized in orbital-free quantum mechanical/molecular mechanical (OF-QM/MM) simulations. The functional includes the nonlocal term constructed from the response function of the reference system of the QM solute. The present work provides a method to combine the OF-QM/MM with a theory of solutions based on the energy representation to compute the solvation free energy of the QM solute in solution. The method is applied to the calculation of the solvation free energy Δμ of a QM water solute in an MM water solvent. It is demonstrated that Δμ is computed as −7.7 kcal/mol, in good agreement with an experimental value of −6.3 kcal/mol. We also develop a theory to map the free energy δμ due to electron density polarization onto the coordinate space of electrons. The free energy density obtained by the free-energy mapping for the QM water clarifies that each hydrogen atom makes a positive contribution (+34.7 kcal/mol) to δμ, and the oxygen atom gives the negative free energy (−71.7 kcal/mol). It is shown that the small polarization free energy −2.4 kcal/mol is generated as a result of the cancellation of these counteracting energies. These analyses are made possible by the OF-QM/MM approach combined with a statistical theory of solutions. [ABSTRACT FROM AUTHOR]

Generally, the second-harmonic generation and slow light of multi-band topological edge states (TESs) have been studied separately. Therefore, the influence of simultaneous slow light and topology protection on second-harmonic generation (SHG) is deficient. Here, we propose a high-efficiency SHG using dual-frequency TESs in topological photonic crystals (TPCs) with slow-light conditions. The wave vector matching condition and energy conservation condition (frequency doubling) can be achieved by adequately adjusting the overall structural parameters of TPCs. The double-resonant nonlinear interaction between two TESs is enabled using a square lattice TPC. Due to the topological localization of the TES and the long interaction time of slow-light effect, the energy densities of the fundamental wave and SHG are significantly increased. Consequently, the high intrinsic efficiency of SHG can be obtained in the order of 7.40 × 10−4. Our work opens new avenues for using topological protected and slow light enhanced nonlinear frequency conversion in a TPC system. [ABSTRACT FROM AUTHOR]

Density functional theory has been widely used in quantum mechanical simulations, but the search for a universal exchange-correlation (XC) functional has been elusive. Over the last two decades, machine-learning techniques have been introduced to approximate the XC functional or potential, and recent advances in deep learning have renewed interest in this approach. In this article, we review early efforts to use machine learning to approximate the XC functional, with a focus on the challenge of transferring knowledge from small molecules to larger systems. Recently, the transferability problem has been addressed through the use of quasi-local density-based descriptors, which are rooted in the holographic electron density theorem. We also discuss recent developments using deep-learning techniques that target high-level ab initio molecular energy and electron density for training. These efforts can be unified under a general framework, which will also be discussed from this perspective. Additionally, we explore the use of auxiliary machine-learning models for van der Waals interactions. [ABSTRACT FROM AUTHOR]

The elastic behavior of nematics is commonly described in terms of the three so-called bulk deformation modes, i.e., splay, twist, and bend. However, the elastic free energy contains also other terms, often denoted as saddle–splay and splay–bend, which contribute, for instance, in confined systems. The role of such terms is controversial, partly because of the difficulty of their experimental determination. The saddle–splay (K24) and splay–bend (K13) elastic constants remain elusive also for theories; indeed, even the possibility of obtaining unambiguous microscopic expressions for these quantities has been questioned. Here, within the framework of Onsager theory with Parsons–Lee correction, we obtain microscopic estimates of the deformation free energy density of hard rod nematics in the presence of different director deformations. In the limit of a slowly changing director, these are directly compared with the macroscopic elastic free energy density. Within the same framework, we derive also closed microscopic expressions for all elastic coefficients of rodlike nematics. We find that the saddle–splay constant K24 is larger than both K11 and K22 over a wide range of particle lengths and densities. Moreover, the K13 contribution comes out to be crucial for the consistency of the results obtained from the analysis of the microscopic deformation free energy density calculated for variants of the splay deformation. [ABSTRACT FROM AUTHOR]

Recent work on incorporating strong-correlation (sc) corrections into the scLH22t local hybrid functional [A. Wodyński and M. Kaupp, J. Chem. Theory Comput. 18, 6111–6123 (2022)] used a hybrid procedure, applying a strong-correlation factor derived from the reverse Becke–Roussel machinery of the KP16/B13 and B13 functionals to the nonlocal correlation term of a local hybrid functional. Here, we show that adiabatic-connection factors for strong-correlation-corrected local hybrids (scLHs) can be constructed in a simplified way based on a comparison of semi-local and exact exchange-energy densities only, without recourse to exchange-hole normalization. The simplified procedure is based on a comparative analysis of Becke's B05 real-space treatment of nondynamical correlation and that in LHs, and it allows us to use, in principle, any semi-local exchange-energy density in the variable used to construct local adiabatic connections. The derivation of competitive scLHs is demonstrated based on either a modified Becke–Roussel or a simpler Perdew–Burke–Ernzerhof (PBE) energy density, leading to the scLH23t-mBR and scLH23t-tPBE functionals, which both exhibit low fractional spin errors while retaining good performance for weakly correlated situations. We also report preliminary attempts toward more detailed modeling of the local adiabatic connection, allowing a reduction of unphysical local maxima in spin-restricted bond-dissociation energy curves (scLH23t-mBR-P form). The simplified derivations of sc-factors reported here provide a basis for future constructions and straightforward implementation of exchange-correlation functionals that escape the zero-sum game between low self-interaction and static-correlation errors. [ABSTRACT FROM AUTHOR]

The all-solid-state batteries (ASSBs) are of particular interest because of their higher energy density and improved safety. However, the interfacial instability and resulting high interfacial resistance between the cathode and solid electrolyte (SE) have become the major challenges for the practical application of ASSBs. Herein, we report a stable LiFePO4 cathode/γ-Li3PO4 SE interface and systemically investigate the mechanism of Li-ion transport at the interface and the effects of surface nitrogen doping using first-principles calculations. It is found that delithiation at the LiFePO4/γ-Li3PO4 interface initially occurs at the topmost layer of the LiFePO4 cathode side, and hopping through the interface barrier is a rate-limiting step for Li mobility. Nitrogen doping leads to local structural distortion occurred at the interface, affecting the interfacial Li+ diffusion kinetics. Furthermore, the underlying mechanisms in which the different N doping sites alter the Li diffusion barrier are analyzed. We find that, by a rational design, N doping could significantly enhance Li+ diffusion kinetics. Further analysis of the electronic structure of the interface system reveals that the Li3PO4 electrolyte is electrochemically stable against the LiFePO4 cathode in the N-doped interface. Our findings provide a microscopic understanding of the Li+ transport at solid–solid LiFePO4/γ-Li3PO4 interface and suggest that controlling synthesis condition can be critical for enhancing Li+ transport at the N-doped LiFePO4/γ-Li3PO4 interface in an ASSB. [ABSTRACT FROM AUTHOR]

[Display omitted] Three-dimensional interconnected nickel–cobalt layered double hydroxides (NiCo-LDHs) were prepared on nickel foam by ion exchange using a cobalt-based metal–organic framework (Co-MOF) as a template at different temperatures. The effects of the Co-MOF preparation temperature on the growth, mass, morphology, and electrochemical properties of the Co-MOF and derived NiCo-LDH samples were studied. The synthesis temperature from 30 to 50 °C gradually increased the mass of the active material and the thickness of the Co-MOF sheets grown on the nickel foam. The higher the temperature is, the larger the proportion of Co3+. β-Cobalt hydroxide (β-Co(OH) 2) sheets were generated above 60 °C. The morphology and mass loading pattern of the derived flocculent layer clusters of NiCo-LDH were inherited from metal-organic frameworks (MOFs). The areal capacitance of NiCo-LDH shows an inverted U-shaped curve trend with increasing temperature. The electrode material synthesized at 50 °C had a tremendous specific capacitance of 7631 mF·cm−2 at a current density of 2 mA·cm−2. The asymmetric supercapacitor assembled with the sample and active carbon (AC) achieved an energy density of 55.0 Wh·kg−1 at a power density of 800.0 W·kg−1, demonstrating the great potential of the NiCo-LDH material for energy storage. This work presents a new strategy for designing and fabricating advanced green supercapacitor materials with large power and energy densities. [ABSTRACT FROM AUTHOR]

[Display omitted] Na metal batteries using inorganic solid-state electrolytes (SSEs) have attracted extensive attention due to their superior safety and high energy density. However, their development is plagued by the unclear structural/volumetric evolution of SSEs and the corresponding Na+ migration mechanisms. In this work, NaSn 2 F 5 (NSF) clusters are composed of nanoparticles (NPs) with matched lattices induced by dislocations, which can mitigate the volume swelling/shrinkage of the NPs. NSF behaves like a single ion conductor with a high Na+ transference number (t Na+) of 0.79. Specially, the ionic conductivity (σ) of NSF is increased from 7.64 × 10-6 to 5.42 × 10-5 S cm−1 after partial irreversible oxidation of Sn2+ (0.118 Å) → Sn4+ (0.069 Å) with the shrunk ionic radius during the charge process, giving more spaces for Na+ migration. Furthermore, a poly(acrylonitrile)-NaSn 2 F 5 -NaPF 6 composite polymer electrolyte (NSF CPE) was fabricated with a σ of 4.13 × 10-4 S cm−1 and a t Na+ of 0.60. The NSF CPE-based symmetric cell can operate over 3000 h due to the couplings between the different components in NSF CPE, which is beneficial for ion transfer and the construction of stable solid electrolyte interface. And the quasi -solid-state Na|NSF CPE|Na 3 V 2 (PO 4) 3 full cell displays excellent electrochemical performance. [ABSTRACT FROM AUTHOR]

Composite of CoS 1.97 nanoparticles decorated CuS hollow cubes and reduced graphene oxide (rGO) (CCSrGO) thin film flexible positive electrode is fabricated as the anode material of supercapacitor with broad application prospects in electrochemical energy storage. [Display omitted] Stretchable flexible thin-film electrodes are extensively explored for developing new wearable energy storage devices. However, traditional carbon-based materials used in such independent electrodes have limited practical applications owing to their low energy storage capacity and energy density. To address this, a unique structure and remarkable mechanical stability thin-film flexible positive electrode comprising CoS 1.97 nanoparticles decorated hollow CuS cubes and reduced graphene oxide (rGO), hereinafter referred to as CCSrGO, is prepared. Transition metal sulfide CoS 1.97 and CuS shows high energy density owing to the synergistic effects of its active components. The electrode can simultaneously meet the high-energy density and safety requirements of new wearable energy storage devices. The electrode has excellent electrochemical performance (1380 F/g at 1 A/g) and ideal capacitance retention (93.8 % after 10,000 cycles) owing to its unique three-dimensional hollow structure and polymetallic synergies between copper and cobalt elements, which are attributed to their different energy storage mechanisms. Furthermore, a flexible asymmetric supercapacitor (FASC) was constructed using CCSrGO as the positive electrode and rGO as the negative electrode (CCSrGO//rGO), which delivers an energy density of 100 Wh kg−1 and a corresponding power density of 2663 W kg−1 within a voltage window of 0–1.5 V. The resulting FASC can power a light-emitting diode (LED) at different bending and twisting angles, exerting little effect on the capacitance. Therefore, the prepared CCSrGO//rGO FASC devices show great application prospects in energy storage. [ABSTRACT FROM AUTHOR]

The interpenetrating polymer networks PVA-SA-PPy hydrogels were prepared by the freeze-thawing and in-situ polymerization method. The PVA network and SA network formed interpenetrating networks through hydrogen bonding and physical entanglement, which boosted the mechanical properties and ion diffusion characteristics. [Display omitted] Flexible supercapacitors (FSCs) have attracted much attention due to their strong mechanical flexibility, wearability and portability, which greatly rely on the employed flexible electrodes. The conductive polymer hydrogels with excellent flexibility, processability and capacitive performance are one of the most promising candidates, which are still limited by their poor mechanical properties. Constructing robust interpenetrating polymer networks (IPN) is an effective approach to promote their mechanical properties. Herein, interpenetrating polyvinyl alcohol (PVA)-sodium alginate (SA)-polypyrrole (PPy) hydrogels are prepared by the freeze–thaw and in-situ polymerization method. The IPN structure composed of PVA and SA not only enhances the mechanical properties of hydrogels, but also provides substantial active sites for electrochemical reactions. Moreover, the hydrogen-bonding interaction between different components in the PVA-SA-PPy hydrogel boosts the charge/ion transfer. The optimal PVA-SA-PPy hydrogels show an elongation at break of 380 %, a tensile strength of 1.5 MPa, and a specific capacitance of 2646 mF cm−2 at 2 mA cm−2. The symmetric PVA-SA-PPy FSCs show an energy density of 96.7 μWh cm−2 at a power density of 999.9 μW cm−2, and the capacitance retention is 66.3 % after 10,000 cycles. These exceptional mechanical and electrochemical properties make the PVA-SA-PPy hydrogels a promising candidate for FSCs. [ABSTRACT FROM AUTHOR]

[Display omitted] • A novel Ru-doped CoNiFe − LDH was prepared by one-step hydrothermal method. • DFT calculations verified that Ru doping improved the electronic structure of LDH. • The optimal Ru-doped CoNiFe − LDH exhibited superior performance for supercapacitor and OER. In recent years, ternary layered double hydroxide (LDH) has become a research hotspot for electrode materials and oxygen evolution reaction (OER) catalyst due to the enhanced synergistic effect between individual elements. However, the application of LDH is greatly limited by its low electrical conductivity and the disadvantage that nanosheets tend to accumulate and mask the active sites. Herein, a novel Ru-doped CoNiFe − LDH was prepared via a facile hydrothermal method. According to the density functional theory (DFT) calculations, the doping of Ru element could improve electron state density and band gaps of LDH and consequently boosted the electrochemical reaction kinetics as well as electrical conductivity. Furthermore, introduction of Ru atom induced the formation of porous flower-like structures in nanosheets. Compared to CoNiFe − LDH (28.9 m2/g), Ru-doped CoNiFe − LDH performed larger specific surface area of 53.1 m2/g, resulting in more electrochemically active sites. In these case, Ru-doped CoNiFe − LDH demonstrated better energy storage performance of 176.0 mAh/g at 1 A/g compared to original CoNiFe − LDH (78.9 mAh/g at 1 A/g). Besides, the assembled Ru-doped CoNiFe − LDH//activated carbon (AC) device delivered a maximum energy density of 36.4 W h kg−1 at the power density of 740.3 W kg−1 and an outstanding cycle life (78.7 % after 10,000 cycles). Meanwhile, Ru-doped CoNiFe − LDH exhibited lower overpotential (339 mV at 50 mA cm−2) and Tafel slope (93.2 mV dec−1). Therefore, this work provided novel and valuable insights into the rational doping of Ru elements for the controlled synthesis of supercapacitor electrode materials and OER catalysts. [ABSTRACT FROM AUTHOR]

Benefitting from the synergetic effects of heterostructured sulfide as the charge transfer accelerator and N -doped carbon matrix as an armor, the bimetallic FeS 2 /MoS 2 heterostructure confined in nitrogen-doped carbon (FMS@NC) delivers a comprehensive K-ions storage ability. Moreover, the as-built K-ion capacitor based on FMS@NC anode and activated carbon cathode achieves a high energy/power density as well as ultra-long cycling stability. [Display omitted] The means of structural hybridization such as heterojunction construction and carbon-coating engineering for facilitating charge transfer and electron transport are considered viable strategies to address the challenges associated with the low rate capability and poor cycling stability of sulfide-based anodes in potassium-ion batteries (PIBs). Motivated by these concepts, we have successfully prepared a hydrangea-like bimetallic sulfide heterostructure encapsulated in nitrogen-doped carbon (FMS@NC) using a simple solvothermal method, followed by poly-dopamine wrapping and a one-step sulfidation/carbonization process. When served as an anode for PIBs, this FMS@NC demonstrates a high specific capacity (585 mAh g−1 at 0.05 A/g) and long cycling stability. Synergetic effects of mitigated volume expansions and enhanced conductivity that are responsbile for such high performance have been verified to originate from the heterostructured sulfides and the N -doped carbon matrix. Meanwhile, comprehensive characterization reveals existence of an intercalation-conversion hybrid K-ion storage mechanism in this material. Impressively, a K-ion capacitor with the FMS@NC anode and a commercial activated carbon cathode exhibits a superior energy density of up to 192 Wh kg−1, a high power density, and outstanding cycling stability. This study provides constructive guidance for designing high-performance and durable potassium-ion storage anodes for next-generation energy storage devices. [ABSTRACT FROM AUTHOR]

A high performance lamellar structured Fe-doped MnS/graphene anode has been developed for sodium-ion storage. Due to the synergistic positive effect of graphene confinement, strong Mn S C bonding and Fe-doping, the composite exhibits excellent rate performance and long-term stability. A prototype sodium-ion capacitor fabricated with Fe-MnS/PG anode and nitrogen-doped carbon cathode can deliver both high energy and high power densities. [Display omitted] Manganese sulfide (MnS) is a promising converion-type anode for sodium storage, owing to the virtues of high theoretical capacity, coupled with it crustal abundance and cost-effectiveness. Nevertheless, MnS suffers from inadequate electronic conductivity, sluggish Na+ reaction kinetics and considerable volume variation during discharge/charge process, thereby impeding its rate capability and capacity retention. Herein, a novel lamellar heterostructured composite of Fe-doped MnS nanoparticles/positively charged reduced graphene oxide (Fe-MnS/PG) was synthesized to overcome these issues. The Fe-doping can accelerate the ion/electron transfer, endowing fast electrochemical kinetics of MnS. Meanwhile, the graphene space confinement with strong Mn S C bond interactions can facilite the interfacial electron transfer, hamper volume expansion and aggregation of MnS nanoparticles, stabilizing the structural integrity, thus improving the Na+ storage reversibility and cyclic stability. Combining the synergistic effect of Fe-doping and space confinement with strong Mn S C bond interactions, the as-produced Fe-MnS/PG anode presents a remarkable capacity of 567 mAh/g at 0.1 A/g and outstanding rate performance (192 mAh/g at 10 A/g). Meanwhile, the as-assembled sodium-ion capacitor (SIC) can yield a high energy density of 119 Wh kg−1 and a maximum power density of 17500 W kg−1, with capacity retention of 77 % at 1 A/g after 5000 cycles. This work offers a promising strategy to develop MnS-based practical SICs with high energy and long lifespan, and paves the way for fabricating advanced anode materials. [ABSTRACT FROM AUTHOR]

[Display omitted] • Use of a university two-step strategy to construct 3D VO 2 /CNT@PANI with core–shell architecture. • Taking full advantage of the synergistic effect, the optimal VO 2 /CNT@PANI exhibits superior electrochemical performances. • Fabrication of a full-printable in-planar symmetric supercapacitor with a remarkable areal energy density and cycling life. • Great potential application prospects in the field of portable/wearable electronics. As a progressive electronic energy storage device, the flexible supercapacitor holds tremendous promise for powering wearable/portable electronic products. Of various pseudocapacitor materials, vanadium dioxide (VO 2) has garnered extensive attention due to its impressive theoretical capacitance. However, the challenges of inferior cycling life and lower energy density to be addressed. Herein, we prepare VO 2 nanorods with winding carbon nanotubes (CNT) via a facile solvothermal route, followed by in situ polymerization of polyaniline (PANI) shell. Taking full advantage of the synergistic effect, the VO 2 /CNT@PANI composite delivers a high specific capacitance of 354.2F/g at 0.5 A/g and a long cycling life of ∼ 88.2 % over 5000 cycles resulting from the enhanced conductivity of CNT and stabilization of PANI shell. By screen printing the formulated inks with outstanding rheological behaviours, we manufacture an in-planar VO 2 /CNT@PANI symmetric supercapacitor (VO 2 /CNT@PANI SSC) device featuring an orderly arrangement structure. This device yields a remarkable areal energy density of 99.57 μWh/cm2 at a power density of 387.5 μW/cm2 while retaining approximately ∼ 87.6 % of its initial capacitance after prolonged use. Furthermore, we successfully powered a portable game machine for more than 2 min using two SSCs connected in series with ease. Therefore, this work presents a universal strategy that utilises combination and coating to boost electrochemical performance for flexible high-performance supercapacitors. [ABSTRACT FROM AUTHOR]

CoNi LDH nanostructures with large specific surface areas were prepared through a facile sonochemical approach in the solutions with different pH values. The CoNi LDH exhibited battery-type electrochemical response with the highest capacity of 740.8C/g at 1 A/g in 2 M of KOH electrolyte. The assembled CoNi LDH//AC hybrid supercapacitor delivered the highest energy density of 35.6 W h kg−1 at the power density of 781.1 W kg−1. [Display omitted] • CoNi LDH nanostructures with large surface area were sonochemically prepared. • A high specific capacity of 740.8C/g at 1 A/g was delivered. • Just a little capacity decay over 5000 cycles at a high current density of 8 A/g. • The HSC device delivered an energy density of 35.6 W h kg−1 at 781.1 W kg−1. Fabricating battery-type electrode materials with large specific surface area and mesopores is an efficient method for enhancing the electrochemical performance of supercapacitors. This method may provide more active sites for Faradic reactions and shorten the ion-diffusion paths. In this study, the CoNi layered double hydroxides (LDHs) with the morphology of nanoflowers and nanoflakes were prepared in solutions with pH values of 7.5 (CoNi LDH-7.5) and 8.5 (CoNi LDH-8.5) via a simple sonochemical approach. These CoNi LDHs possessed large specific surface areas and favourable electrochemical properties. The CoNi LDH-7.5 delivered a specific capacity of 740.8C/g at a current density of 1 A/g, surpassing CoNi LDH-8.5 with 668.1C/g. The hybrid supercapacitor (HSC) was assembled with activated carbon as the anode and CoNi LDH as the cathode to assess its practical application potential in the field of electrochemical energy storage. The CoNi LDH-7.5//AC HSC achieved the highest energy density of 35.6 W h kg−1 at a power density of 781.1 W kg−1. In addition, both HSCs exhibited little capacity decay over 5,000 cycles at a high current load of 8 A/g. These electrochemical properties of CoNi LDHs make them promising candidates for battery-type electrode materials. The current sonochemical method is simple and can be applied to the preparation of other LDHs-based electrode materials with favourable electrochemical performance. [ABSTRACT FROM AUTHOR]

The impact of the sintering temperature on the phase composition and electrical properties of 5% SrTiO 3 –95%BaZr 0.15 Ti 0.85 O 3 (ST-BZT) ceramics fabricated by solid-state method and consolidated by two-step sintering is presented. A systematic analysis of the phase composition, microstructures, dielectric, ferroelectric, and energy storage characteristics. A di-phase SrTiO 3 –BaZrTiO 3 composite is obtained at low sintering temperatures below 1400 °C. Increasing the sintering temperature causes a shift of the Curie temperature from 62 °C to 55 °C together with changes of permittivity values and of the ferroelectric loops, thus indicating a progressive interdiffusion process at the interfaces, together with a better densification. Remarkably, the ST-BZT composition sintered at 1500 °C exhibits characteristics of a single phase (Ba,Sr) (Zr,Ti)O 3 solid solution, with high room temperature permittivity around 2950 and good ferroelectric response (saturation polarization P max = 12.6 μC/cm2 and remnant polarization P r = 2.16 μC/cm2). Consequently, this composition displays a much greater recoverable energy density (W rec = 54.5 mJ/cm3) in comparison to the ones of the di-phase ST-BZT composites and the parent phases. However, the (Sr 0.05 Ba 0.95) (Zr 0.14 Ti 0.86)O 3 solid solution, demonstrates a lower energy efficiency (72%) in comparison to the ST-BZT di-phase composites sintered at lower temperatures, which exhibit higher energy efficiency values around 86%. In addition, the charge-discharge experiments were performed under different electric fields to disclose the difference in energy storage properties in 5% SrTiO 3 –95%BaZr 0.15 Ti 0.85 O 3 ceramics. This suggests that the sintering strategy plays a crucial role in determining the energy efficiency of the obtained ceramics. Additionally, all the investigated ST-BZT ceramics present high energy efficiency at low-applied electric fields, suggesting their potential as candidates for energy storage capacitors operating at moderate fields. [ABSTRACT FROM AUTHOR]

High-entropy perovskite oxides (HEPOs) have attracted considerable attention as dielectric ceramics. However, the energy-storage performance of these HEPOs still requires improvement. In this study, a series of (1- x)(Bi 0. 4 Ba 0. 2 K 0. 2 Na 0.2)TiO 3 - x NaNbO 3 high-entropy ceramics were designed and prepared using a high-entropy strategy. The introduction of antiferroelectric NaNbO 3 into the (Bi 0. 4 Ba 0. 2 K 0. 2 Na 0.2)TiO 3 medium-entropy matrix increased the configurational entropy and cationic disorder, resulting in improved energy storage performance. The ceramic with an optimal composition of 0.775(Bi 0. 4 Ba 0. 2 K 0. 2 Na 0.2)TiO 3 -0.225NaNbO 3 achieved a high recoverable energy density (W rec) of 2.523 J/cm3 and a high efficiency (η) of 83.7% at an electric field of 220 kV/cm. Furthermore, the material demonstrated good temperature and frequency stability, as well as good anti-fatigue properties. This paper presents a dielectric ceramic suitable for energy storage under low to moderate electric fields. [ABSTRACT FROM AUTHOR]

The energy storage properties of pure PLZST-based antiferroelectric ceramics are excellent; however, the high sintering temperature renders them unsuitable for co-firing with copper inner electrodes as MLCC dielectric materials. The proven BASK glass additive was employed in this study to lower the sintering temperature of PLSZT ceramics, while simultaneously doping Sm3+ ions to enhance their sintering performance under reducing atmospheres. The precise evaluation process confirmed that the addition of glass effectively reduced the sintering temperature to 1040 °C. Furthermore, the defect association of Sm3+ doping hindered the formation of oxygen vacancies, facilitated ceramic grain growth, and significantly enhanced insulation resistivity. Consequently, an ultrahigh recoverable energy density (W rec) of 5.19 J/cm3 with a high energy storage efficiency (η) of 94.5% are achieved at an electric field of 430 kV/cm. Moreover, the AFE ceramics possess excellent discharge energy storage properties with a high discharge energy density (W d) of 4.26 J/cm3 and a large power density (P d) of 139 MW/cm3. [ABSTRACT FROM AUTHOR]

In research out of the sustainable electrochemical energy storage material, NiCo-LDH/MnO 2 composite has been prepared via simple hydrothermal method. The experimental characterizations of XRD, SEM/TEM and XPS have been utilized to explore the structure and morphology of prepared composite. The needle-like MnO 2 was found adhered to NiCo-LDH sheet. The composite's electrochemical properties were evaluated through cyclic voltammetry, galvanostatic charge-discharge and electrochemical impedance spectroscopy. It has been realized that the MnO 2 dosage not only changes the composite's microstructure but also affects its electrochemical properties. The best specific capacitance (2602 F g−1 at a current density of 1 A g−1) was achieved for the composite sample with 38% MnO 2 (mass), which is almost two times high from the same composite in previous reports. With the sample, the assembled asymmetric supercapacitor exhibits a remarkable energy density of 19.56 Wh.Kg−1 at 800.29 W Kg−1. It could be attributed to the synergetic effects of two components as well as their good interfacial coupling. The good electrochemical activity makes our synthesized composite feasible to be applied as electrode material and provides valuable insights for the development of smart capacitors utilizing NiCo-LDH. [ABSTRACT FROM AUTHOR]

Glass ceramic dielectric materials with high power density and high energy density have important application value in the miniaturization and integration of lightweight pulse power devices. In this work, SrO 2 –BaO 2 –Nb 2 O 5 –SiO 2 –Al 2 O 3 –B 2 O 3 glass ceramics doped with various contents of CeO 2 were prepared via high-temperature melting combined with temperature-controlled crystallization process. Results showed that CeO 2 doping increased the content of Ba 0.27 Sr 0.75 Nb 2 O 5.78 tungsten bronze phase precipitate from the glass matrix in glass ceramics (from 55.7% to 82.2%), thereby increasing dielectric constant of SrO 2 –BaO 2 –Nb 2 O 5 –SiO 2 –Al 2 O 3 –B 2 O 3 glass ceramics (from 66.5 to 101.9). Besides that, CeO 2 -doped ceramics exhibited excellent temperature stability and low loss (below 0.015). The highest breakdown strength (1590 kV/cm) and energy density (12.88 J/cm3) were achieved in the ceramic with a CeO 2 doping concentration of 3.0 mol.%, being 3.03 times higher than those in undoped glass ceramic. The increase in energy density of the ceramics was attributed to moderate CeO 2 doping concentration that improved the crystallinity (from 83.8% to 89.8%) and reduced the interfacial activation energy of the glass ceramics. [ABSTRACT FROM AUTHOR]

Rare earth element doped bimetallic oxides are a new technology for improving the electrochemical performance of electrode materials. In this study, 0.5% La-NiMoO4 flower-like structured nanomaterials were directly grown on nickel-based surfaces through a fast and simple room temperature stirring method. The characterization methods such as SEM and TEM confirmed that the prepared product has a three-dimensional nanoflower-like structure, and also demonstrated that the prepared 0.5% La-NiMoO4 nanoflower material was successfully doped with rare earth elements. We also conducted electrochemical tests on the material, and the results showed that at a reaction time of 16 h, the 0.5% La-NiMoO4 flower-like structure exhibited excellent electrochemical performance. At a current density of 2 A g-1, the specific capacitance was 2100 F g-1. After 5500 cycles of charging and discharging at a current density of 1 A g-1, the capacitance retention rate was 99.8%. A 0.5% La-NiMoO4/Ni//Fe2O3/Ni asymmetric supercapacitor device was assembled using 0.5% La-NiMoO4 as the positive electrode and Fe2O3 as the negative electrode. At a current density of 15 A g-1 and a working window voltage of 1.8 V, the power density of the asymmetric device was 8000 W kg-1 (energy density 56.5 W h kg-1). At a current density of 5 A g-1, the device underwent 5000 cycles of charge and discharge, and the capacitance retention rate was 89.5%. The 0.5% La-NiMoO4 electrode material prepared in this study through a simple, fast, environmentally friendly method exhibits good electrochemical performance, making it a potential electrode material for development. [ABSTRACT FROM AUTHOR]

Ceramic-based dielectric capacitors are showing great potential in advanced high-power applications. However, simultaneous achievement of high energy density (W rec) and temperature stability is still a main bottleneck. Herein, an extraordinary nanoscale structural heterogeneity is developed to promote temperature-stable energy storage in Er/Mn co-doped Bi 0.5 Na 0.5 TiO 3 based ceramics via domain and defect dipoles engineering. The composition-driven domain reconstruction by Er/Mn co-doping can induce internal random fields with rapid response to the electric field, and thus enhance ΔP and η. Meanwhile, the donor-accpetor Er/Mn doping could manipulate defect dipoles coupling to resist the applied field evolution to elevate BDS and η. Besides, the improved relaxor feature and core-shell structure give rise to the enhanced temperature stability. Ceramics with 2 mol % Er 2 O 3 demonstrate high W rec ∼2.79 J/cm3, large efficiency ∼89.4% and outstanding dielectric stability within 70–500 °C. The proposed nanostructural heterogeneity was verified as a promising pathway to manufact temperature-stable energy storage ceramics. The nanoscale structural heterogeneity via domain and defect dipoles strategies is developed to promote temperature-stable energy storage in NBT-based ceramics. [Display omitted] [ABSTRACT FROM AUTHOR]

Phase change material (PCM) is an ideal heat storage material with huge latent heat and nearly constant phase change temperature, but there are serious problems in application such as leakage and low thermal conductivity. Porous ceramic is widely used in PCM packaging because of its advantages of controllable porosity and high thermal conductivity. Porous Al 2 O 3 ceramics were prepared by foaming injection coagulation method. In order to improve the thermal conductivity of porous ceramic matrix, Porous Al 2 O 3 @Graphite Ceramics (PAGC) were prepared by sucrose decomposition. Form-Stable Phase Change Materials (FSPCMs) were prepared by adsorption of Lauric Acid/Myristic Acid (LA/MA) in PAGC by vacuum impregnation method. SEM showed that the prepared PAGC had a three-dimensional interpenetrating structure and high porosity. TEM and XPS showed that alumina skeleton were uniformly coated with graphite. After PAGC impregnated by LA/MA, the maximum PCM storage reached 62.11 wt %. The maximum latent heat of FSPCMs reaches 83.33 J/g. Thermogravimetric analysis, thermal cycling test and Fourier transform infrared spectroscopy show that the prepared FSPCMs has good thermal stability, thermal reliability, chemical stability and compressive strength. More importantly, the thermal conductivity of the prepared FSPCMs is greatly improved, reaching up to 3.73 W/mK. It is 20.72 times the original PCM, mainly due to the synergistic effect of the Al 2 O 3 skeleton and the graphite coating to build a continuous highway for heat transfer. This study provides a practical means to greatly improve the thermal conductivity of FSPCMs, which will promote the practical application of FSPCMs. [ABSTRACT FROM AUTHOR]

Dielectric (Ba 0.4 Sr 0.6)TiO 3 (BST) ceramics are promising dielectric energy storage materials due to their moderate dielectric constant, low dielectric loss, and slight nonlinearity. However, their energy density is limited by their low breakdown strength (BDS). In this study, we aimed to address this limitation by incorporating various amounts of Bi 0.2 Sr 0.7 (Mg 1/3 Nb 2/3)O 3 (SBMN) into the BST matrix. The (1– x)BST x SBMN ceramics were prepared by conventional solid-state sintering, resulting in single-phase solid solutions. Compared to pure BST ceramics, the (1– x)BST– x SBMN ceramics exhibited lower remnant polarization and significantly enhanced BDS. Furthermore, the relaxation of the ceramics enhanced with increasing doping concentration, with an efficiency of η = 94.0% achieved at x = 0.20. Among them, the breakdown field strength of 0.85BST–0.15SBMN ceramics was 597 kV cm−1, achieving a recoverable energy storage density of W rec = 2.81 J cm−3 and an efficiency of η = 90.8% under an external electric field of 480 kV cm−1. Subsequent tests revealed that the introduction of SBMN not only increased the band gap and conduction activation energy of the material, leading to an increase in BDS, but also promoted the formation of polar nanoregions (PNRs) which contributed to boosted energy efficiency, resulting in a significant enhancement in the energy storage performance of BST ceramics. [Display omitted] [ABSTRACT FROM AUTHOR]

The aim of the present investigation is to study the effect of calcination temperature on the electrochemical performance of MnMoO4 nanoparticles, which are synthesized using a facile and time-saving microwave-assisted annealing technique. The prepared samples are calcinated at 300 °C, 500 °C, and 700 °C for 3 h. The microporous morphology is obtained when the MnMoO4 nanoparticles are calcinated at 500 °C. The electrode prepared with MnMoO4 nanoparticles exhibited a remarkable-specific capacity of 1613 C g−1 and 1549 C g−1 at 10 mV s−1 and 2 A g−1, respectively. An asymmetric supercapacitor is fabricated by depositing MnMoO4 nanoparticles and activated carbon on Ni-foam as positive and negative electrodes, respectively. The device demonstrated a magnificent energy density of 68 W h kg−1 at 850 W kg−1 and displayed an excellent cycling stability of 139% after 5000 cycles. [ABSTRACT FROM AUTHOR]

Pores form inside the ZnO varistor during the sintering process, especially in the edge area. The pore defects frequently lead to breakdown of the varistor. In this study, a simulation model was developed to calculate the electric field and energy density within the varistor. The presence of edge pores resulted in the distortion of the electric field and uneven energy distribution, causing a decrease in the energy capacity of the varistor. Combining the simulations with the results of impact energy tolerance tests on varistors, the mechanism of varistor failure induced by edge pores was revealed. To enhance the energy capacity of varistors, a repair medium with high permeability was developed herein. By employing a secondary sintering method, new grains were grown within the open pores at the edge of the varistor, improving the energy capacity of the varistor from 600 to 1000 A for a 2 ms square wave. Moreover, the mismatch between coefficients of thermal expansion was addressed. This work helped clarify the effects of edge defects in varistors, and a strategy for enhancing their energy capacity was demonstrated. [ABSTRACT FROM AUTHOR]

Barium titanate (BaTiO 3 , BT) is widely used in capacitors because of its excellent dielectric properties. However, owing to its high remanent polarisation (P r) and low dielectric breakdown field strength (E b), achievement of high energy storage performance is challenging. Herein, a systematic strategy was proposed to reduce P r and elevate E b of BT via: (i) modification of the relaxor behavior by alloying it with Bi(Mg 2/3 Ta 1/3)O 3 (BMT) and (ii) heightening E b by introducing NaTaO 3 (NT) with high band gap. Consequently, the energy storage efficiency (η) of 90 % and high E b of 780 kV cm−1 were achieved simultaneously for the BT-BMT- x NT system, which facilitated the recoverable energy density (W rec) of 6.02 J cm−3. At 300 kV cm−1, its temperature (20–120 °C) and frequency (1–500 Hz) stabilities were found to be good. Moreover, the BT-BMT-0.15NT possessed ultrafast discharge rate (t 0.9 < 51 ns) and ultrahigh power density (P D > 94 MW cm−3). This study offers an effective strategy for the design of novel high-performance dielectric energy storage materials. [ABSTRACT FROM AUTHOR]