Difficulties, strategies, and recent research and development of layered sodium transition metal oxide cathode materials for high-energy sodium-ion batteries

Energy-storage systems and their production have attracted significant interest for practical applications.Batteries are the foundation of sustainable energy sources for electric vehicles(EVs),portable electronic devices(PEDs),etc.In recent decades,Lithium-ion batteries(LIBs) have been extensively utilized in largescale energy storage devices owing to their long cycle life and high energy density.However,the high cost and limited availability of Li are the two main obstacles for LIBs.In this regard,sodium-ion batteries(SIBs) are attractive alternatives to LIBs for large-scale energy storage systems because of the abundance and low cost of sodium materials.Cathode is one of the most important components in the battery,which limits cost and performance of a battery.Among the classified cathode structures,layered structure materials have attracted attention because of their high ionic conductivity,fast diffusion rate,and high specific capacity.Here,we present a comprehensive review of the classification of layered structures and the preparation of layered materials.Furthermore,the review article discusses extensively about the issues of the layered materials,namely(1) electrochemical degradation,(2) irreversible structural changes,and(3) structural instability,and also it provides strategies to overcome the issues such as elemental phase composition,a small amount of elemental doping,structural design,and surface alteration for emerging SIBs.In addition,the article discusses about the recent research development on layered unary,binary,ternary,quaternary,quinary,and senary-based O3-and P2-type cathode materials for high-energy SIBs.This review article provides useful information for the development of high-energy layered sodium transition metal oxide P2 and O3-cathode materials for practical SIBs.

Moiré superlattices arising from growth induced by screw dislocations in layered materials

Moiré superlattices(MSLs) are modulated structures produced from homogeneous or heterogeneous two-dimensional layers stacked with a twist angle and/or lattice mismatch. Enriching the methods for fabricating MSL and realizing the unique emergent properties are key challenges in its investigation. Here we recommend that the spiral dislocation driven growth is another optional method for the preparation of high quality MSL samples. The spiral structure stabilizes the constant out-of-plane lattice distance, causing the variations in electronic and optical properties. Taking SnS_(2) MSL as an example, we find prominent properties including large band gap reduction(~ 0.4 e V) and enhanced optical activity. Firstprinciples calculations reveal that these unusual properties can be ascribed to the locally enhanced interlayer interaction associated with the Moiré potential modulation. We believe that the spiral dislocation driven growth would be a powerful method to expand the MSL family and broaden their scope of application.

Recent Progress and Regulation Strategies of Layered Materials as Cathode of Aqueous Zinc-Ion Batteries

Aqueous zinc-ion batteries(ZIBs)have shown great potential in the fields of wearable devices,consumer electronics,and electric vehicles due to their high level of safety,low cost,and multiple electron transfer.The layered cathode materials of ZIBs hold a stable structure during charge and discharge reactions owing to the ultrafast and straightforward(de)intercalation-type storage mechanism of Zn^(2+)ions in their tunable interlayer spacing and their abilities to accommodate other guest ions or molecules.Nevertheless,the challenges of inadequate energy density,dissolution of active materials,uncontrollable byproducts,increased internal pressure,and a large de-solvation penalty have been deemed an obstacle to the development of ZIBs.In this review,recent strategies on the structure regulation of layered materials for aqueous zinc-ion energy storage devices are systematically summarized.Finally,critical science challenges and future outlooks are proposed to guide and promote the development of advanced cathode materials for ZIBs.

Recent progress in Ni-rich layered oxides and related cathode materials for Li-ion cells

Undoubtedly,the enormous progress observed in recent years in the Ni-rich layered cathode materials has been crucial in terms of pushing boundaries of the Li-ion battery(LIB)technology.The achieved improvements in the energy density,cyclability,charging speed,reduced costs,as well as safety and stability,already contribute to the wider adoption of LIBs,which extends nowadays beyond mobile electronics,power tools,and electric vehicles,to the new range of applications,including grid storage solutions.With numerous published papers and broad reviews already available on the subject of Ni-rich oxides,this review focuses more on the most recent progress and new ideas presented in the literature references.The covered topics include doping and composition optimization,advanced coating,concentration gradient and single crystal materials,as well as innovations concerning new electrolytes and their modification,with the application of Ni-rich cathodes in solid-state batteries also discussed.Related cathode materials are briefly mentioned,with the high-entropy approach and zero-strain concept presented as well.A critical overview of the still unresolved issues is given,with perspectives on the further directions of studies and the expected gains provided.

Cycling performance of layered oxide cathode materials for sodium-ion batteries

Layered oxide is a promising cathode material for sodium-ion batteries because of its high-capacity,high operating voltage,and simple synthesis.Cycling performance is an important criterion for evaluating the application prospects of batteries.However,facing challenges,including phase transitions,ambient stability,side reactions,and irreversible anionic oxygen activity,the cycling performance of layered oxide cathode materials still cannot meet the application requirements.Therefore,this review proposes several strategies to address these challenges.First,bulk doping is introduced from three aspects:cationic single doping,anionic single doping,and multi-ion doping.Second,homogeneous surface coating and concentration gradient modification are reviewed.In addition,methods such as mixed structure design,particle engineering,high-entropy material construction,and integrated modification are proposed.Finally,a summary and outlook provide a new horizon for developing and modifying layered oxide cathode materials.

Recent progress in flexible sensors based on 2D materials

With the rapid development of the internet of things(IoT)and wearable electronics,the role of flexible sensors is becoming increasingly irreplaceable,due to their ability to process and convert information acquisition.Two-dimensional(2D)materials have been widely welcomed by researchers as sensitive layers,which broadens the range and application of flexible sensors due to the advantages of their large specific surface area,tunable energy bands,controllable thickness at the atomic level,stable mechanical properties,and excellent optoelectronic properties.This review focuses on five different types of 2D materials for monitoring pressure,humidity,sound,gas,and so on,to realize the recognition and conversion of human body and environmental signals.Meanwhile,the main problems and possible solutions of flexible sensors based on 2D materials as sensitive layers are summarized.

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.

Thermodynamically Revealing the Essence of Order and Disorder Structures in Layered Cathode Materials

Layered transition metal(TM) oxides are one of the most widely used cathode materials in lithium-ion batteries. The atomic configuration in TM layer of these materials is often known to be random when multiple TM elements co-exist in the layer(e.g. Ni, Co and Mn). By contrast, the configuration tends to be ordered if the elements are Li and Mn. Here, by using special quasi-random structures(SQS) algorithm, the essential reasons of the ordering in a promising Li-rich Mn-based cathode material Li2MnO3 are investigated. The difference of internal energy and entropy between ordered and disordered materials is calculated. As a result, based on the Gibbs free energy, it is found that Li2MnO3 should have an ordered structure in TM layer. In comparison, structures with Ni-Mn ratio of 2:1 are predicted to have a disordered TM layer, because the entropy terms have larger impact on the structural ordering than internal energy terms.

Recent progress and prospective on layered anode materials for potassium-ion batteries

Potassium-ion batteries(PIBs),also known as“novel post-lithium-ion batteries,”have promising energy storage and utilization prospects due to their abundant and inexpensive raw materials.Appropriate anode materials are critical for realizing high-performance PIBs because they are an important component determining the energy and power densities.Two-dimensional(2D)layered anode materials with increased interlayer distances,specific surface areas,and more active sites are promising candidates for PIBs,which have a high reversible capacity in the energetic pathway.In this review,we briefly summarize K+storage behaviors in 2D layered carbon,transition metal chalcogenides,and MXene materials and provide some suggestions on how to select and optimize appropriate 2D anode materials to achieve ideal electrochemical performance.

Intercalation Assembly Method and Intercalation Process Control of Layered Intercalated Functional Materials

Layered intercalated functional materials of layered double hydroxide type are an important class of functional materials developed in recent years. Based on long term studies on these materials in the State Key Laboratory of Chemical Resource Engineering in Beiiing University of Chemical Technology, the orinciole for the design of controlled intercalation processes in the light of tuture production processing requirements has been developed. Intercalation assembly methods and technologies have been invented to control the intercalation process for preparing layered intercalated materials with various structures and functions.

2D materials modulating layered double hydroxides for electrocatalytic water splitting

Exploring highly efficient electrochemical water splitting catalysts has recently attracted extensive research interest from both fundamental researches and practical applications.Transition metal‐based layered double hydroxides(LDHs)have been proved to be one of the most efficient materials for oxygen evolution reaction(OER),however,still suffered from low conductivity and sluggish kinetics for hydrogen evolution reaction(HER),which largely inhibited the overall water splitting efficiency.To address this dilemma,enormous approaches including doping regulation,intercalation tuning and defect engineering are therefore rationally designed and developed.Herein,we focus on the recent exciting progress of LDHs hybridization with other two‐dimensional(2D)materials for water splitting reactions,not barely for enhancing OER efficiency but also for boosting HER activity.Particularly,the structural features,morphologies,charge transfer and synergistic effects for the heterostructure/heterointerface that influence the electrocatalytic performance are discussed in details.The hybrid 2D building blocks not only serve as additional conductivity and structural supported but also promote electron transfer at the interfaces and further enhance the electrocatalytic performance.The construction and application of the nanohybrid materials will guide a new direction in developing multifunctional materials based on LDHs,which will contribute to energy conversion and storage.

Synthesis and Characterization of Novel Layered Lithium Sodium Silicate (Silinaite) and the Mesoporous Materials from Silinaite

Novel layered silinaite has been synthesized using an aqueous mixture of water glass, LiOH and NaOH under hydrothermal crystallization. Subsequently transformation of silinaite into mesoporous materials （SDM） was achieved at mild condition using cetyltfimethylammonium bromide as structure-directing agents. The resulting samples were characterized by XRD, SEM, FTIR nitrogen adsorption-desorption isotherms and catalytic performance in bulky molecular involved reaction. The results revealed that synthesized mesoporous materials derived from the silinaite exhibited an ordered hexagonal crystal structure with average pore diameter 2.7 nm and BET surface area 817m^2/g. The SDM-supported ZnCl2 catalyst, prepared by impregnationevaporation method, retained the mesoporous structure and showed high selectivity in alkylation of benzene with benzyl chloride.

Recent Progress and Prospects of Layered Cathode Materials for Potassium-ion Batteries

Layered materials with two-dimensional ion diffusion channels and fast kinetics are attractive as cathode materials for secondary batteries.However,one main challenge in potassium-ion batteries is the large ion size of K^(+),along with the strong K^(+)-K^(+)electrostatic repulsion.This strong interaction results in initial K deficiency,greater voltage slope,and lower specific capacity between set voltage ranges for layered transition metal oxides.In this review,a comprehensive review of the latest advancements in layered cathode materials for potassium-ion batteries is presented.Except for layered transition metal oxides,some polyanionic compounds,chalcogenides,and organic materials with the layered structure are introduced separately.Furthermore,summary and personal perspectives on future optimization and structural design of layered cathode materials are constructively discussed.We strongly appeal to the further exploration of layered polyanionic compounds and have demonstrated a series of novel layered structures including layered K_(3)V_(2)(PO_(4))_(3).

Recent advances in the electrochemistry of layered post-transition metal chalcogenide nanomaterials for hydrogen evolution reaction

Layered two-dimensional(2 D)materials have received tremendous attention due to their unique physical and chemical properties when downsized to single or few layers.Several types of layered materials,especially transition metal dichalcogenides(TMDs)have been demonstrated to be good electrode materials due to their interesting physical and chemical properties.Apart from TMDs,post-transition metal chalcogenides(PTMCs)recently have emerged as a family of important semiconducting materials for electrochemical studies.PTMCs are layered materials which are composed of post-transition metals raging from main group IIIA to group VA(Ga,In,Ge,Sn,Sb and Bi)and group VI chalcogen atoms(S,selenium(Se)and tellurium(Te)).Although a large number of literatures have reviewed the electrochemical and electrocatalytic applications of TMDs,less attention has been focused on PTMCs.In this review,we focus our attention on PTMCs with the aim to provide a summary to describe their fundamental electrochemical properties and electrocatalytic activity towards hydrogen evolution reaction(HER).The characteristic chemical compositions and crystal structures of PTMCs are firstly discussed,which are different from TMDs.Then,inherent electrochemistry of PTMCs is discussed to unveil the well-defined redox behaviors of PTMCs,which could potentially affect their efficiency when applied as electrode materials.Following,we focus our attention on electrocatalytic activity of PTMCs towards HER including novel synthetic strategies developed for the optimization of their HER activity.This review ends with the perspectives for the future research direction in the field of PTMC based electrocatalysts.

Synthesis and electrochemical characterization of layered Li[Ni_(1/3)Co_(1/3)Mn_(1/3)]O_2 cathode materialfor Li-ion batteries

Layered LiNi1/3Co1/3Mn1/3O2 materials were synthesized using a nickel-cobalt-manganese carbonate precursor obtained by chemical co-precipitation. The [Ni1/3Co1/3Mn1/3]CO3 precursor and the LiNi1/3Co1/3Mn1/3O2 powders were characterized by X-ray diffraction（XRD） and scanning electron micrograph（SEM）. The SEM analysis shows that these particles possess uniform and spherical morphology. The electrochemical properties of the (LiNi1/3-)(Co1/3Mn1/3O2) cathode material for rechargeable lithium-ion batteries such as the galvanostatic charge-discharge performance and cyclic voltammetry（CV） were measured. The results show that an initial discharge capacity of 190.29mA·h·g-1 is obtained in the voltage range of 2.54.6V and at a current rate of 0.1C at 25℃.The discharge capacity increases linearly with the increase of the upper cut-off voltage limit.

Intercalation Assembly and Chemical Product Engineering of Layered Intercalated Functional Materials Based on Efficient Utilization of Magnesium Resources in Salt Lakes

1 Introduction Magnesium salts are very important by-product of salt lake industry in West China.Nearly 200 million cubic meters of waste brine are released to the environment

Experiments and computer simulation analysis of impact behaviors of micro-sized abrasive in waterjet cutting of thin multiple layered materials

The abrasive waterjet (AWJ) is now widely used in the advanced cutting processes of polymers,metals,glass,ceramics and composite materials like thin multiple-layered material (TMM).Various research and development efforts have recently been made to understand the science of AWJ.However,the interaction mechanism between a workpiece and high-velocity abrasive particles still remains a complicated problem.In this work,the material removal mechanisms of AWJ such as micro penetration and micro dent were experimentally investigated.In addition,a new computer simulation model considering high strain rate effect was proposed to understand the micro impact behavior of high-velocity micro-sized abrasives in AWJ cutting.

Approximate Electromagnetic Cloaking of a Dielectric Sphere Using Homogeneous Isotropic Multi-Layered Materials

In cloaking, a body is hidden from detection by surrounding it by a coating consisting of an unusual anisotropic nonhomogeneous material. The permittivity and permeability of such a cloak are determined by the coordinate transformation of compressing a hidden body into a point or a line. The radially-dependent spherical cloaking shell can be approximately discretized into many homogeneous anisotropic layers;each anisotropic layer can be replaced by a pair of equivalent isotropic sub-layers, where the effective medium approximation is used to find the parameters of these two equivalent sub-layers. In this work, the scattering properties of cloaked dielectric sphere is investigated using a combination of approximate cloaking, where the dielectric sphere is transformed into a small sphere rather than to a point, together with discretizing the cloaking material using pairs of homogeneous isotropic sub-layers. The back-scattering normalized radar cross section, the scattering patterns are studied and the total scattering cross section against the frequency for different number of layers and transformed radius.

Examination of the Thermal Cloaking Effectiveness with Layered Engineering Materials

The concentrically layered thermal cloaks with isotropic materials could realize the equivalent thermal cloaking effect with Pendry＇s cloak, while the effectiveness is scarcely investigated quantitatively. Here we examine the cloaking effectiveness quantitatively by evaluating the standard deviation of the temperature difference between the simulated plane with the layered thermal cloak and Pendry＇s thermal cloak. The design rules for the isotropic materials in terms of thermal conductivity and layer thickness are presented. The present method could quan- titatively evaluate the cloaking effectiveness, and could open avenues for analyzing the cloaking effect, detecting the （anti-） cloaks, etc.

Recent advances in two-dimensional layered and non-layered materials hybrid heterostructures

With the development of Moore's law, the future trend of devices will inevitably be shrinking and integration to further achieve size reduction. The emergence of new two-dimensional non-layered materials(2DNLMs) not only enriches the 2D material family to meet future development, but also stimulates the global enthusiasm for basic research and application technologies in the 2D field. Van der Waals(vd W) heterostructures, in which two-dimensional layered materials(2DLMs)are physically stacked layer by layer, can also occur between 2DLMs and 2DNLMs hybrid heterostructures, providing an alternative platform for nanoelectronics and optoelectronic applications. Here, we outline the recent developments of2DLMs/2DNLMs hybrid heterostructures, with particular emphasis on major advances in synthetic methods and applications. And the categories and crystal structures of 2DLMs and 2DNLMs are also shown. We highlight some promising applications of the heterostructures in electronics, optoelectronics, and catalysis. Finally, we provide conclusions and future prospects in the 2D materials field.