Research on Preparation and Electrochemical Performance of the High Compacted Density Ni-Co-Mn Ternary Cathode Materials

The high compacted density LiNi0.5-xCo0.2Mn0.3MgxO2 cathode material for lithium-ion batteries was synthesized by high temperature solid-state method, taking the Mg element as a doping element and the spherical Ni0.5Co0.2Mn0.3 (OH)2, Li2CO3 as raw materials. The effects of calcination temperature on the structure and properties of the products were investigated. The structure and morphology of cathode materials powder were analyzed by X-ray diffraction spectroscopy (XRD) and scanning electronmicroscopy (SEM). The electrochemical properties of the cathode materials were studied by charge-discharge test and cyclic properties test. The results show that LiNi0.4985Co0.2Mn0.3 Mg0.0015O2 cathode material prepared at calcination temperature 930°C has a good layered structure, and the compacted density of the electrode sheet is above 3.68 g/cm3. The discharge capacity retention rate is more than 97.5% after 100 cycles at a charge-discharge rate of 1C, displaying a good cyclic performance.

Effects of current density on preparation and performance of Al/conductive coating/α-PbO_2-Ce O_2-TiO_2/β-Pb O_2-MnO_2-WC-ZrO_2 composite electrode materials

Al/conductive coating/α-Pb O2-Ce O2-Ti O2/β-PbO 2-MnO 2-WC-Zr O2 composite electrode material was prepared on Al/conductive coating/α-PbO 2-Ce O2-Ti O2 substrate by electrochemical oxidation co-deposition technique. The effects of current density on the chemical composition, electrocatalytic activity, and stability of the composite anode material were investigated by energy dispersive X-ray spectroscopy（EDXS）, anode polarization curves, quasi-stationary polarization（Tafel） curves, electrochemical impedance spectroscopy（EIS）, scanning electron microscopy（SEM）, and X-ray diffraction（XRD）. Results reveal that the composite electrode obtained at 1 A/dm2 possesses the lowest overpotential（0.610 V at 500 A/m2） for oxygen evolution, the best electrocatalytic activity, the longest service life（360 h at 40 °C in 150 g/L H2SO4 solution under 2 A/cm2）, and the lowest cell voltage（2.75 V at 500 A/m2）. Furthermore, with increasing current density, the coating exhibits grain growth and the decrease of content of Mn O2. Only a slight effect on crystalline structure is observed.

Databases of 2D material-substrate interfaces and 2D charged building blocks

Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials science.Layered materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new materials in this respect.In van der Waals(vdW)layered materials,these building blocks are charge neutral and can be isolated from their bulk phase(top-down),but usually grow on substrate.In ionic layered materials,they are charged and usually cannot exist independently but can serve as motifs to construct new materials(bottom-up).In this paper,we introduce our recently constructed databases for 2D material-substrate interface(2DMSI),and 2D charged building blocks.For 2DMSI database,we systematically build a workflow to predict appropriate substrates and their geometries at substrates,and construct the 2DMSI database.For the 2D charged building block database,1208 entries from bulk material database are identified.Information of crystal structure,valence state,source,dimension and so on is provided for each entry with a json format.We also show its application in designing and searching for new functional layered materials.The 2DMSI database,building block database,and designed layered materials are available in Science Data Bank at https://doi.org/10.57760/sciencedb.j00113.00188.

First-Principles Study of Blue Phosphorene and Graphene Intralayer Heterostructure as Anode Materials for Rechargeable Li-lon Batteries

There is an ideal desire to develop the high-performance anodes materials for Liion batteries(LIBs),which requires not onlyhigh stability and reversibility,but also rapidcharging/discharging rate.In this work,webuiltablue phosphorene-graphene(BlueP-G)intralayer heterostructure by connecting BlueP and graphene monolayers at zigzag edges with covalent bonds.Based on the density functional theory simulation,the electronic structure of the heterostructure,Li adsorption and Li diffusion on heterostructure were systematically investigated.Compared with the pristine BlueP,the existence of graphene layer increases the overall conductivity of BlueP-G intralayer heterostructure.The significantly enhanced adsorption energy indicates the Li deposition on anode surface is energetically favored.The fast diffusion of Li with energy barrier as low as 0.02-0.09 eV indicates the growth of Li dendrite could be suppressed and the stability and reversibility of the battery will be increased.With a combination of increased conductivity of electronic charge,excellent Li adsorption and Li mobility on surface,BlueP-G intralayer heterostructure with zigzag interface is quite promising in the application of anode material for Li-ion batteries.

Modification strategies improving the electrochemical and structural stability of high-Ni cathode materials

With the increasing spotlight in electric vehicles,there is a growing demand for high-energy-density batteries to enhance driving range.Consequently,several studies have been conducted on high-energy-density LiNi_(x)Co_(y)Mn_(z)O_(2)cathodes.However,there is a limit to permanent performance deterioration because of side reactions caused by moisture in the atmosphere and continuous microcracks during cycling as the Ni content to express high energy increases and the content of Mn and Co that maintain structural and electrochemical stabilization decreases.The direct modification of the surface and bulk regions aims to enhance the capacity and long-term performance of high-Ni cathode materials.Therefore,an efficient modification requires a study based on a thorough understanding of the degradation mechanisms in the surface and bulk region.In this review,a comprehensive analysis of various modifications,including doping,coating,concentration gradient,and single crystals,is conducted to solve degradation issues along with an analysis of the overall degradation mechanism occurring in high-Ni cathode materials.It also summarizes recent research developments related to the following modifications,aims to provide notable points and directions for post-studies,and provides valuable references for the commercialization of stable high-energy-density cathode materials.

Functionally gradient materials for sustainable and high-energy rechargeable lithium batteries:Design principles,progress,and perspectives

Rechargeable lithium batteries with high-capacity cathodes/anodes promise high energy densities for nextgeneration electrochemical energy storage.However,the associated limitations at various scales greatly hinder their practical applications.Functional gradient material(FGM)design endows the electrode materials with property gradient,thus providing great opportunities to address the kinetics and stability obstacles.To date,still no review or perspective has covered recent advancements in gradient design at multiple scales for boosting lithium battery performances.To fill this void,this work provides a timely and comprehensive overview of this exciting and sustainable research field.We begin by overviewing the fundamental features of FGM and the rationales of gradient design for improved electrochemical performance.Then,we comprehensively review FGM design for rechargeable lithium batteries at various scales,including natural or artificial solid electrolyte interphase(SEI)at the nanoscale,micrometer-scale electrode particles,and macroscale electrode films.The link between gradient structure design and improved electrochemical performance is particularly highlighted.The most recent research into constructing novel functional gradients,such as valence and temperature gradients,has also been explored.Finally,we discussed the current constraints and future scope of FGM in rechargeable lithium batteries,aiming to inspire the development of novel FGM for next-generation high-performance lithium batteries.

Theoretical Study of the N-NO_2 Bond Dissociation Energies for Energetic Materials with Density Functional Theory

The N-NO2 bond dissociation energies （BDEs） for 7 energetic materials were computed by means of accurate density functional theory （B3LYP, B3PW91 and B3P86） with 6-31G＊＊ and 6-311G＊＊ basis sets. By comparing the computed energies and experimental results, we find that the B3P86/6-311G＊＊ method can give good results of BDE, which has the mean absolute deviation of 1.30kcal/mol. In addition, substituent effects were also taken into account. It is noted that the Hammett constants of substituent groups are related to the BDEs of the N-NO2 bond and the bond dissociation energies of the energetic materials studied decrease when increasing the number of NO2 group.

Screener3D:a gaseous time projection chamber for ultra-low radioactive material screening

In experiments searching for rare signals,background events from the detector itself are some of the major factors limiting search sensitivity.Screening for ultra-low radioactive detector materials is becoming ever more essential.We propose to develop a gaseous time projection chamber(TPC)with a Micromegas readout for radio screening.The TPC records three-dimensional trajectories of charged particles emitted from a flat sample placed in the active volume of the detector.The detector can distinguish the origin of an event and identify the particle types with information from trajectories,which significantly increases the screening sensitivity.For a particles from the sample surface,we observe that our proposed detector can reach a sensitivity higher than 100 l Bq m-2 within two days.

Closed-form solution for shock wave propagation in density-graded cellular material under impact

Density-graded cellular materials have tremendous potential in structural applications where impact resistance is required.Cellular materials subjected to high impact loading result in a compaction type deformation,usually modeled using continuum-based shock theory.The resulting governing differential equation of the shock model is nonlinear,and the density gradient further complicates the problem.Earlier studies have employed numerical methods to obtain the solution.In this study,an analytical closed-form solution is proposed to predict the response of density-graded cellular materials subjected to a rigid body impact.Solutions for the velocity of the impinging rigid body mass,energy absorption capacity of the cellular material,and the incident stress are obtained for a single shock propagation.The results obtained are in excellent agreement with the existing numerical solutions found in the literature.The proposed analytical solution can be potentially used for parametric studies and for effectively designing graded structures to mitigate impact.

New carbon-nitrogen-oxygen compounds as high energy density materials

Molecular crystals are complex systems exhibiting various crystal structures,and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure.Here,we perform an extensive structure search of ternary carbon-nitrogen-oxygen(CNO)compound under high pressure with the CALYPSO method and first principles calculations,and successfully identify three polymeric CNO compounds with Pbam,C2/m and I4m2symmetries under 100 GPa.More interestingly,these structures are also dynamically stable at ambient pressure,and are potential high energy density materials(HEDMs).The energy densities of Pbam,C2/m and I4m2 phases of CNO are about2.30 kJ/g,1.37 kJ/g and 2.70 kJ/g,respectively,with the decompositions of graphitic carbon and molecular carbon dioxide andα-N(molecular N_(2))at ambient pressure.The present results provide in-depth insights into the structural evolution and physical properties of CNO compounds under high pressures,which offer crucial insights for designs and syntheses of novel HEDMs.

Compressive Strength of Polymer Grouting Material at Different Temperatures

In order to study the influence of temperature on compressive strength of polymer grouting material,the compression specimen injection mold is self-made,and the uniaxial compressive test was carried out in the temperature control box under different temperatures.The change regularity of compressive strength of polymer grouting material under different temperatures and the law of volume changes of polymer samples were obtained.The experimental results show that：the compressive strength of polymer material increases with the increase of density;the temperature change has a certain influence on the compressive strength of polymer grouting material;the compressive strength decreases with temperature increases under the same density,but the compressive strength is not significantly affected by temperature when the density is less than 0.4 g/cm3;the volume change of the samples accords with the law of thermal expansion and contraction when temperature changes,and the increase of the volume is obvious when it is under high temperature.The achievements will provide an important basis to the application of the polymer grouting material.

On the hydro-mechanical behaviour of MX80 bentonite-based materials

Bentonite-based materials have been considered in many countries as engineered barrier/backfilling materials in deep geological disposal of high-level radioactive waste.During the long period of waste storage,these materials will play an essential role in ensuring the integrity of the storage system that consists of the waste canisters,the engineered barrier/backfill,the retaining structures as well as the geological barrier.Thus,it is essential to well understand the hydro-mechanical behaviours of these bentonite-based materials.This review paper presents the recent advances of knowledge on MX80 bentonite-based materials,in terms of water retention properties,hydraulic behaviour and mechanical behaviour.Emphasis is put on the effect of technological voids and the role of the dry density of bentonite.The swelling anisotropy is also discussed based on the results from swelling tests with measurements of both axial and radial swelling pressures on a sand-bentonite mixture compacted at different densities.Microstructure observation was used to help the interpretation of macroscopic hydromechanical behaviour.Also,the evolution of soil microstructure thus the soil density over time is discussed based on the results from mock-up tests.This evolution is essential for understanding the longterm hydro-mechanical behaviour of the engineered barrier/backfill.

Surface-engineering of layered LiNi_(0.815)Co_(0.15)Al_(0.035)O_2 cathode material for high-energy and stable Li-ion batteries

Surface engineering is an effective strategy to restrain the generation of rocksalt NiO phase on surface of layered LiNi0.815Co0.15Al0.035O2（NCA） primary nanoparticles, a representative Ni-rich layered oxides cathode materials. Herein, we demonstrate the kilogram-scale synthesis of few-layer reduced graphene oxide（rGO） conformably coated NCA primary nanoparticles cathode materials by a mechanical wet ball-milling strategy. The lightening rGO coating layer effectively avoids the direct contact of electrolyte and NCA with rapid electrons transfer. As a result, the as-obtained NCA@rGO hybrids with only 1.0 wt% rGO content can deliver a high specific capacity（196 mAh g-1 at 0.2 C） and fast charge/discharge capability（127 mAh g-1 at 5 C）, which is much higher than the corresponding NCA nanoparticles（95 mAh g-1 at 5 C）. Even after100 cycles at 1 C, 91.7% of initial reversible capacity is still maintained. Furthermore, a prismatic pouch cell（240 mAh） is also successfully assembled with the commercial graphite anode.

Particle breakage of granular materials during sample preparation

Particle breakage is commonly observed in granular materials when subjected to external loads. It was found that particle breakage would occur during both sample preparation and loading stages. However,main attention was usually paid to the particle breakage behaviour of samples during loading stage. This study attempts to explore the breakage behaviour of granular materials during sample preparation.Triaxial samples of rockfill aggregates are prepared by layered compaction method to achieve different relative densities. Extents of particle breakage based on the gradings before and after test are presented and analysed. It is found that particle breakage during sample preparation cannot be ignored. Gradings after test are observed to shift away from the initial grading. Aggregates with larger size that appear to break are more than the smaller-sized ones. Irrespective of the initial gradings, an increase in the extent of particle breakage with the increasing relative density is observed during sample preparation.

Nitrogen-doped carbon stabilized Li Fe0.5Mn0.5PO4/rGO cathode materials for high-power Li-ion batteries

Exploring high ion/electron conductive olivine-type transition metal phosphates is of vital significance to broaden their applicability in rapid-charging devices.Herein,we report an interface engineered Li Fe0.5Mn0.5PO4/rGO@C cathode material by the synergistic effects of r GO and polydopamine-derived N-doped carbon.The well-distributed Li Fe0.5Mn0.5PO4nanoparticles are tightly anchored on r GO nanosheet benefited by the coating of N-doped carbon layer.The design of such an architecture can effectively suppress the agglomeration of nanoparticles with a shortened Li+transfer path.Meantime,the high-speed conducting network has been constructed by r GO and N-doped carbon,which exhibits the face-to-face contact with Li Fe0.5Mn0.5PO4nanoparticles,guaranteeing the rapid electron transfer.These profits endow the Li Fe0.5Mn0.5PO4/rGO@C hybrids with a fast charge-discharge ability,e.g.a high reversible capacity of 105 m Ah·g^-1at 10 C,much higher than that of the Li Fe0.5Mn0.5PO4@C nanoparticles(46 mA·h·g^-1).Furthermore,a 90.8%capacity retention can be obtained even after cycling 500 times at 2 C.This work gives a new avenue to fabricate transition metal phosphate with superior electrochemical performance for high-power Li-ion batteries.

First-principles study of high performance lithium/sodium storage of Ti3C2T2 nanosheets as electrode materials

Ti3C2Tx nanosheet,the first synthesized MXene with high capacity performance and charge/discharge rate,has attracted increasingly attention in renewable energy storage applications.By performing systematic density functional theory calculations,the theoretical capacity of the intrinsic structure of single-and multi-layered Ti3C2T2(T=F or O)corresponding to M(M=Li and Na)atoms are investigated.Theoretical volumetric capacity and gravimetric capacity are obtained,which are related to the stacking degree.The optimal ratios of capacity to structure are determined under different stacking degrees for understanding the influence of surface functional groups on energy storage performance.Its performance can be tuned by performing surface modification and increasing the interlayer distance.In addition,the reason for theoretical capacity differences of M atoms is analyzed,which is attributed to difference in interaction between the M-ions and substrate and the difference in electrostatic exclusion between adsorbed M-ions.These results provide an insight into the understanding of the method of efficiently increasing the energy storage performance,which will be useful for designing and using high performance electrode materials.

Giant Magnetostrictive Material Loudspeaker System Acoustic Radiation Simulation

An infinite panel model of giant magnetostrictive material loudspeaker system （GMMLS） is proposed by making use of finite element method（FEM）. Bending wave eigenfunction is introduced to describe the acoustic radiation condition of the panel. Far-field response in different conditions is calculated by changing the mass surface density. Conclusion is obtained by analyzing the curves simulated, that panel which has larger mass surface density can hardly generate far-field acoustic radiation for lower frequency, while the panel has smaller mass surface density generates far-field acoustic radiation for lower frequency evenly and stronger.

Accurate machine learning models based on small dataset of energetic materials through spatial matrix featurization methods

A large database is desired for machine learning(ML) technology to make accurate predictions of materials physicochemical properties based on their molecular structure.When a large database is not available,the development of proper featurization method based on physicochemical nature of target proprieties can improve the predictive power of ML models with a smaller database.In this work,we show that two new featurization methods,volume occupation spatial matrix and heat contribution spatial matrix,can improve the accuracy in predicting energetic materials' crystal density(ρ_(crystal)) and solid phase enthalpy of formation(H_(f,solid)) using a database containing 451 energetic molecules.Their mean absolute errors are reduced from 0.048 g/cm~3 and 24.67 kcal/mol to 0.035 g/cm~3 and 9.66 kcal/mol,respectively.By leave-one-out-cross-validation,the newly developed ML models can be used to determine the performance of most kinds of energetic materials except cubanes.Our ML models are applied to predict ρ_(crystal) and H_(f,solid) of CHON-based molecules of the 150 million sized PubChem database,and screened out 56 candidates with competitive detonation performance and reasonable chemical structures.With further improvement in future,spatial matrices have the potential of becoming multifunctional ML simulation tools that could provide even better predictions in wider fields of materials science.

Anode materials for potassium-ion batteries: Current status and prospects

Potassium-ion batteries(KIBs)as one of the most promising alternatives to lithium-ion batteries have been highly valued in recent years.However,progress in KIBs is largely restricted by the sluggish development in anode materials.Therefore,it is imperative to systematically outline and evaluate the recent research advances in the field of anode materials for KIBs toward promoting the development of high-performance anode materials for KIBs.In this review,the recent achievements in anode materials for KIBs are summarized.The electrochemical properties(ie.charge storage mechanism,capacity,rate performance,and cycling stability)of these reported anode materials,as well as their advantages/disadvantages,are discerned and analyzed,enabling high-performance KIBs to meet the requirements for practical applications.Finally,technological developments,scientific challenges,and future research opportunities of anode materials for KIBs are briefly reviewed.

Computational screening of doping schemes for LiTi2(PO4)3 as cathode coating materials

In all-solid-state lithium batteries,the impedance at the cathode/electrolyte interface shows close relationship with the cycle performance.Cathode coatings are helpful to reduce the impedance and increase the stability at the interface effectively.LiTi2(PO4)3(LTP),a fast ion conductor with high ionic conductivity approaching 10^(-3)S·cm^(-1),is adopted as the coating materials in this study.The crystal and electronic structures,as well as the Li^+ion migration properties are evaluated for LTP and its doped derivatives based on density functional theory(DFT)and bond valence(BV)method.Substituting part of Ti sites with element Mn,Fe,or Mg in LTP can improve the electronic conductivity of LTP while does not decrease its high ionic conductivity.In this way,the coating materials with both high ionic conductivities and electronic conductivities can be prepared for all-solid-state lithium batteries to improve the ion and electron transport properties at the interface.