Machine learning in metal-ion battery research: Advancing material prediction, characterization, and status evaluation

Metal-ion batteries(MIBs),including alkali metal-ion(Li^(+),Na^(+),and K^(3)),multi-valent metal-ion(Zn^(2+),Mg^(2+),and Al^(3+)),metal-air,and metal-sulfur batteries,play an indispensable role in electrochemical energy storage.However,the performance of MIBs is significantly influenced by numerous variables,resulting in multi-dimensional and long-term challenges in the field of battery research and performance enhancement.Machine learning(ML),with its capability to solve intricate tasks and perform robust data processing,is now catalyzing a revolutionary transformation in the development of MIB materials and devices.In this review,we summarize the utilization of ML algorithms that have expedited research on MIBs over the past five years.We present an extensive overview of existing algorithms,elucidating their details,advantages,and limitations in various applications,which encompass electrode screening,material property prediction,electrolyte formulation design,electrode material characterization,manufacturing parameter optimization,and real-time battery status monitoring.Finally,we propose potential solutions and future directions for the application of ML in advancing MIB development.

Application of deep learning for informatics aided design of electrode materials in metal-ion batteries

To develop emerging electrode materials and improve the performances of batteries,the machine learning techniques can provide insights to discover,design and develop battery new materials in high-throughput way.In this paper,two deep learning models are developed and trained with two feature groups extracted from the Materials Project datasets to predict the battery electrochemical performances including average voltage,specific capacity and specific energy.The deep learning models are trained with the multilayer perceptron as the core.The Bayesian optimization and Monte Carlo methods are applied to improve the prediction accuracy of models.Based on 10 types of ion batteries,the correlation coefficients are maintained above 0.9 compared to DFT calculation results and the mean absolute error of the prediction results for voltages of two models can reach 0.41 V and 0.20 V,respectively.The electrochemical performance prediction times for the two trained models on thousands of batteries are only 72.9 ms and 75.7 ms.Besides,the two deep learning models are applied to approach the screening of emerging electrode materials for sodium-ion and potassium-ion batteries.This work can contribute to a high-throughput computational method to accelerate the rational and fast materials discovery and design.

The design and engineering strategies of metal tellurides for advanced metal-ion batteries

Owning various crystal structures and high theoretical capacity,metal tellurides are emerging as promising electrode materials for high-performance metal-ion batteries(MBs).Since metal telluride-based MBs are quite new,fundamental issues raise regarding the energy storage mechanism and other aspects affecting electrochemical performance.Severe volume expansion,low intrinsic conductivity and slow ion diffusion kinetics jeopardize the performance of metal tellurides,so that rational design and engineering are crucial to circumvent these disadvantages.Herein,this review provides an in-depth discussion of recent investigations and progresses of metal tellurides,beginning with a critical discussion on the energy storage mechanisms of metal tellurides in various MBs.In the following,recent design and engineering strategies of metal tellurides,including morphology engineering,compositing,defect engineering and heterostructure construction,for high-performance MBs are summarized.The primary focus is to present a comprehensive understanding of the structural evolution based on the mechanism and corresponding effects of dimension control,composition,electron configuration and structural complexity on the electrochemical performance.In closing,outlooks and prospects for future development of metal tellurides are proposed.This work also highlights the promising directions of design and engineering strategies of metal tellurides with high performance and low cost.

Design strategies for rechargeable aqueous metal-ion batteries

Rechargeable aqueous metal-ion batteries(AMBs)have attracted extensive scientific and commercial interest due to their potential for cost-effective,highly safe,and scalable stationary energy storage.However,their limited output voltage,inadequate energy density,and poor reversibility of ambiguous electrode reactions in aqueous electrolytes strongly limit their practical viability.This review aims to elucidate the challenges of existing AMBs from the material design to whole device applications.We summarize the emerging electrochemistry,fundamental properties,and key issues in interfacial behaviors of various classes of prevailing AMBs,including aqueous alkali metal-ion batteries and multivalent-ion batteries,and present an appraisal of recent advances for addressing the performance deficiency.Specifically,the progress of zinc-ion batteries is highlighted to provide a ubiquitous guideline for their commercialization in the grid-scale energy storage.Finally,we figure out the dominating general challenges for achieving high-performance AMBs,laying out a perspective for future breakthroughs.

Osteolysis in total hip arthroplasty in relation to metal ion release: Comparison between monolithic prostheses and different modularities

BACKGROUND Among the various complications associated with total hip arthroplasty(THA)periprosthetic osteolysis and wear phenomena due to the release of metal particles,are two of the most common and have been reported to be correlated because of inflammatory responses directed towards released particles that generally activate macrophagic osteolytic effects.Therein,new masses known as pseudotumors can appear in soft tissues around a prosthetic implant.To date,there is paucity of reliable data from studies investigating for any association between the above mentioned adverse events.AIM To investigate for the existence of any association between serum and urine concentrations of metal-ions released in THA and periprosthetic osteolysis for modular neck and monolithic implants.METHODS Overall,76 patients were divided into three groups according to the type of hip prosthesis implants:Monoblock,modular with metal head and modular with ceramic head.With an average f-up of 4 years,we conducted a radiological evaluation in order to detect any area of osteolysis around the prosthesis of both the femur and the acetabulum.Moreover,serum and urinary tests were performed to assess the values of Chromium and Cobalt released.Statistical analysis was performed to determine any association between the ion release and osteolysis.RESULTS For the 3 study groups,the monolithic,modular ceramic-headed and modular metal-headed implants had different incidences of osteolysis events,which were higher for the modular implants.Furthermore,the most serious of these(grade 3)were detected almost exclusively for the modular implants with metal heads.A mapping of the affected areas was performed revealing that the highest incidences of osteolysis were evidenced in the pertrochanteric region at the femur level,and in the supero-external region at the acetabular level.Regarding the evaluation of the release of metals-ions from wear processes,serum and urinary chromium and cobalt values were found to be higher in cases of modularity,and even more so for those with metal head.Statistical linear correlation test results suggested positive correlations between increasing metal concentrations and incidences areas of osteolysis.However,no cases of pseudo-tumor were detected.CONCLUSION Future studies are needed to identify risk factors that increase peri-prosthetic metal ion levels and whether these factors might be implicated in the triggering of local events,including osteolysis and aseptic loosening.

Molecular insights on Ca^(2+)/Na+separation via graphene-based nanopores:The role of electrostatic interactions to ionic dehydration

Ca^(2+)/Na+separation is a common problem in industrial applications,biological and medical fields.However,Ca^(2+)and Na+have similar ionic radii and hydration radii,thus Ca^(2+)/Na+separation is challenging.Inspired by biological channels,group modification is one of the effective methods to improve the separation performance.In this work,molecular dynamics simulations were performed to investigate the effects of different functional groups(COO,NH3+)on the separation performance of Ca^(2+)and Na+through graphene nanopores under an electric field.The pristine graphene nanopore was used for comparison.Results showed that three types of nanopores preferred Ca^(2+)to Na+,and Ca^(2+)/Na+selectivity followed the order of GE-COO(4.06)>GE(1.85)>GE-NH3+(1.63).Detailed analysis of ionic hydration microstructure shows that different nanopores result in different hydration factors for the second hydration layer of Ca^(2+)and the first layer of Na+.Such different hydration factors corresponding to the dehydration ability can effectively evaluate the separation performance.In addition,the breaking of hydrogen bonds between water molecules due to electrostatic effects can directly affect the dehydration ability.Therefore,the electrostatic effect generated by group modification will affect the ionic hydration microstructure,thus reflecting the differences in dehydration ability.This in turn affects the permeable and separation performance of cations.The results of this work provide perceptive guidelines for the application of graphene-based membranes in ion separation.

DFT‑Guided Design and Fabrication of Carbon‑Nitride‑Based Materials for Energy Storage Devices:A Review

Carbon nitrides(including CN,C2N,C3N,C3N4,C4N,and C5N)are a unique family of nitrogen-rich carbon materials with multiple beneficial properties in crystalline structures,morphologies,and electronic configurations.In this review,we provide a comprehensive review on these materials properties,theoretical advantages,the synthesis and modification strategies of different carbon nitride-based materials(CNBMs)and their application in existing and emerging rechargeable battery systems,such as lithium-ion batteries,sodium and potassium-ion batteries,lithium sulfur batteries,lithium oxygen batteries,lithium metal batteries,zinc-ion batteries,and solid-state batteries.The central theme of this review is to apply the theoretical and computational design to guide the experimental synthesis of CNBMs for energy storage,i.e.,facilitate the application of first-principle studies and density functional theory for electrode material design,synthesis,and characterization of different CNBMs for the aforementioned rechargeable batteries.At last,we conclude with the challenges,and prospects of CNBMs,and propose future perspectives and strategies for further advancement of CNBMs for rechargeable batteries.

Recent progress in COF-based electrode materials for rechargeable metal-ion batteries

Covalent organic frameworks(COFs)have emerged as promising electrode materials for rechargeable metal-ion batteries and have gained much attention in recent years due to their high specific surface area,inherent porosity,tunable molecular structure,robust framework,abundant active sites.Moreover,compared with inorganic materials and small organic molecules,COFs have the advantages of multi-electron transfer,short pathways,high cycling stability.Although great progress on COF-based electrodes has been made,the corresponding electrochemical performance is still far from satisfactory for practical applications.In this review,we first summarize the fundamental background of COFs,including the species of COFs(different active covalent bonds)and typical synthesis methods of COFs.Then,the key challenges and the latest research progress of COF-based cathodes and anodes for metal-ion batteries are reviewed,including Li-ion batteries,Na-ion batteries,K-ion batteries,Zn-ion batteries,et al.Moreover,the effective strategies to enhance electrochemical performance of COF-based electrodes are presented.Finally,this review also covers the typical superiorities of COFs used in energy devices,as well as providing some perspectives and outlooks in this field.We hope this review can provide fundamental guidance for the development of COFbased electrodes for metal-ion batteries in the further research.

Covalent organic frameworks as electrode materials for rechargeable metal-ion batteries

Covalent organic frameworks(COFs),as a class of crystalline porous polymers,featuring designable structures,tunable frameworks,well-defined channels,and tailorable functionalities,have emerged as promising organic electrode materials for rechargeable metal-ion batteries in recent years.Tremendous efforts have been devoted to improving the electrochemical performance of COFs.However,although significant achievements have been made,the electrochemical behaviors of developed COFs are far away from the desirable performance for practical batteries owing to intrinsic problems,such as poor electronic conductivity,the trade-off relationship between capacity and redox potential,and unfavorable micromorphology.In this review,the recent progress in the development of COFs for rechargeable metal-ion batteries is presented,including Li,Na,K,and Zn ion batteries.Various research strategies for improving the electrochemical performance of COFs are summarized in terms of the molecular-level design and the material-level modification.Finally,the major challenges and perspectives of COFs are also discussed in the aspect of large-scale production and electrochemical performance improvements.

Recent Advances in Covalent Organic Framework Electrode Materials for Alkali Metal-Ion Batteries

Owing to the shortcomings of traditional electrode materials in alkalimetal-ion batteries(AIBs),such as limited reversible specific capacity,low power density,and poor cycling performance,it is particularly important to develop new electrode materials.Covalent organic frameworks(COFs)are crystalline porous polymers that incorporate organic building blocks into their periodic structures through dynamic covalent bonds.COFs are superior to organic materials because of their high designability,regular channels,and stable topology.Since the first report of D_(TP)-A_(NDI)-COF as a cathode material for lithium-ion batteries in 2015,research on COF electrode materials has made continuous progress and breakthroughs.This review briefly introduces the characteristics and current challenges associated with COF electrode materials.Furthermore,we summarize the basic reaction types and active sites according to the categories of covalent bonds,including B–O,C=N,C–N,and C=C.Finally,we emphasize the perspectives on basic structure and morphology design,dimension and size design,and conductivity improvement of COFs based on the latest progress in AIBs.We believe that this review provides important guidelines for the development of high-efficiency COF electrode materials and devices for AIBs.

Carbon materials for metal-ion batteries

Metal-ion(Li-,Na-,Zn-,K-,Mg-,and Al-ion)batteries(MIBs)play an important role in realizing the goals of“emission peak and carbon neutralization”because of their green production techniques,lower pollution,high voltage,and large energy density.Carbon-based materials are indispensable for developing MIBs and are widely adopted as active or auxiliary materials in the anodes and cathodes.For example,carbon-based materials,includ-ing graphite,Si/C and hard carbon,have been used as anode materials for Li-and Na-ion batteries.Carbon can also be used as a conductive coating for cathodes,such as in LiFePO 4/C,to achieve better performance.In addition,as new high-valence MIBs(Zn-,Al-,and Mg-ion)have emerged,a growing number of novel carbon-based mate-rials have been utilized to construct high-performance MIBs.Herein,we discuss the recent development trends in advanced carbon-based materials for MIBs.The impact of the structure properties of advanced carbon-based materials on energy storage is addressed,and a perspective on their development is also proposed.

Self-healing Ga-based liquid metal/alloy anodes for rechargeable batteries

With the rapid development of electronics,electric vehicles,and grid energy storage stations,higher requirements have been put forward for advanced secondary batteries.Liquid metal/alloy electrodes have been considered as a promising development direction to achieve excellent electrochemical performance in metal-ion batteries,due to their specific advantages including the excellent electrode kinetics and self-healing ability against microstructural electrode damage.For conventional liquid batteries,high temperatures are needed to keep electrode liquid and ensure the high conductivity of molten salt electrolytes,which also brings the corrosion and safety issues.Ga-based metal/alloys,which can be operated at or near room temperature,are potential candidates to circumvent the above problems.In this review,the properties and advantages of Ga-based metal/alloys are summarized.Then,Ga-based liquid metal/alloys as anodes in various metal-ion batteries are reviewed in terms of their self-healing ability,battery configurations,working mechanisms,and so on.Furthermore,some views on the future development of Ga-based electrodes in batteries are provided.

Electrolytic alloy-type anodes for metal-ion batteries

Alloy-type metals/alloys hold the promise of increasing the energy density of metal-ion batteries(MIBs)because of their theoretical high gravimetrical capacities.Semimetals and semimetal-analogs are typical alloy-type anodes.Currently,the large-scale extraction of semimetals(Si,Ge)and semimetal-analogs(Sb,Bi,Sn)by traditional metallurgical routes highly relies on using reducing agents(e.g.,carbon,hydrogen,reactive metals),which consumes a large number of fossil fuels and produces greenhouse gas emissions.In addition,the common metallurgical methods for extracting semimetals involve relatively high operating temperatures and therefore produce bulk metal ingots solidified from the liquid metals.However,the commonly used electrode materials in batteries are fine powders.Thus,directly producing semimetal powders would be more energy efficient.In addition,semimetals are good candidates to host alkali/alkaline-earth ions through the alloying process because the electronegativity of semimetals is high.Therefore,preparing semimetal powders via an environment-sound manner is of great interest to provide sustainable anode materials for MIBs while reducing the ecological footprint.Low-cost and high-output capacity anode powder materials,as well as straightforward and environmental-benign synthetic methods,play key roles in enabling the energy conversion and storage technologies for real applications of MIBs.Electrochemical technologies offer new strategies to extract semimetals using electrons as the reducing agent that comes from renewable energies.Besides,the morphologies and structures of the electrolytic products can be rationally tailored by tuning the electrode potentials,electrolytes,and operating temperatures.In this regard,using the one-step green electrochemical method to prepare high-capacity and cheaper alloy-type metalloids for MIB anodes can fulfill the requirements for developing MIBs.This review critically overviews recent developments and advances in the electrochemical extraction of semimetals(Si,Ge)and semimetal-analogs(Sb,Bi,Sn)for MIBs,including basic electrochemical principles,thermodynamic analysis,manufacture strategies and applications in lithium-ion batteries(LIBs),sodium-ion batteries(SIBs),potassium-ion batteries(PIBs),magnesium-ion batteries(Mg-ion batteries),and liquid metal batteries(LMBs).It also presents challenges and prospects of employing electrochemical approaches for preparing alloy-type anode materials directly from inexpensive ore-originated feedstocks.

Advanced carbon-based materials for Na,K,and Zn ion hybrid capacitors

Developing electrochemical energy storage devices with high energy and power densities,long cycling life,as well as low cost is of great significance.Hybrid metal-ion capacitors(MICs),commonly consisting of high energy battery-type anodes and high power capacitor-type cathodes,have become a trade-off between batteries and supercapacitors.Tremendous efforts have been devoted to searching for high-performance electrode materials due to poor rate capability of anodes,low capacity of cathodes,and interior sluggish kinetic match.Carbon materials with large surface area,good electrical conductivity and stability have been considered to be ideal candidates for electrodes of MICs.In this review,the advanced carbon materials directly as cathodes and anodes of MICs are systematically summarized.Then,the key structural/chemical factors including the structure engineering,porous characteristics,and heteroatom incorporation for improving electrochemical performance of carbon materials are highlighted.Additionally,the challenges and opportunities for future research on carbon materials in MICs are also proposed.

MoS_(2)/MoO_(2) nanosheets anchored on carbon cloth for high-performance magnesium-and sodium-ion storage

Developing new types of rechargeable metal-ion batteries beyond lithium-ions,including alkaline ion(such as Na+,K+)and multivalent ion(such as Mg 2+,Zn 2+,Ca 2+and Al 3+)batteries,is progressing quickly towards large-scale energy storage systems.However,the major obstacle to their large-scale applications has been a lack of appropriate electrode materials with reversible metal ions insertion/extraction be-havior,resulting in inferior electrochemical performance.Here we develop a well-designed MoS_(2)/MoO_(2) hybrid nanosheets anchored on carbon cloth(MoS_(2)/MoO_(2)/CC)as electrode materials.This rational de-sign can effectively shorten ion diffusion distance,increase electric conductivity of the electrode,and buffer volume change.Benefiting from the synergistic effect of structural and compositional features,the MoS_(2)/MoO_(2)/CC electrode exhibits high initial reversible capacities(326 mA h g^(−1) at 0.1 A g^(−1) in magnesium-ion storage;1270 mA h g^(−1) at 0.1 A g^(−1) in sodium-ion storage),excellent rate capacities(57 mA h g^(−1) at 10 A g^(−1) in magnesium-ion storage;335 mA h g^(−1) at 5 A g^(−1) in sodium-ion storage)and long-term cycling stability(105 mA h g^(−1) after 600 cycle at 1 A g^(−1) in magnesium-ion storage;208 mA h g^(−1) after 600 cycles at 5 A g^(−1) in sodium-ion storage).We expect that the multi-engineering strategy will provide some valuable insights for the development of other advanced electrode materials for high-performance metal-ion batteries.

2020 roadmap on pore materials for energy and environmental applications

Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized with other materials into functional composites with superior properties.The high specific area of porous materials offer them the advantage as hosts to conduct catalytic and electrochemical reactions.On one hand,catalytic reactions include photocatalytic,p ho toe lectrocatalytic and electrocatalytic reactions over some gases.On the other hand,they can be used as electrodes in various batteries,such as alkaline metal ion batteries and electrochemical capacitors.So far,both catalysis and batteries are extremely attractive topics.There are also many obstacles to overcome in the exploration of these porous materials.The research related to porous materials for energy and environment applications is at extremely active stage,and this has motivated us to contribute with a roadmap on ’porous materials for energy and environment applications’.

2020 roadmap on two-dimensional materials for energy storage and conversion

Energy storage and conversion have attained significant intere st owing to its important applications that reduce CO2 emission through employing green energy.Some promising technologies are included metalair batteries,metal-sulfur batteries,metal-ion batteries,electrochemical capacitors,etc.Here,metal elements are involved with lithium,sodium,and magnesium.For these devices,electrode materials are of importance to obtain high performance.Two-dimensional(2 D) materials are a large kind of layered structured materials with promising future as energy storage materials,which include graphene,black phosporu s,MXenes,covalent organic frameworks(COFs),2 D oxides,2 D chalcogenides,and others.Great progress has been achieved to go ahead for 2 D materials in energy storage and conversion.More researchers will join in this research field.Under the background,it has motivated us to contribute with a roadmap on ’two-dimensional materials for energy storage and conversion.

Self-supported transition metal oxide electrodes for electrochemical energy storage

Electrode materials are of decisive importance in determining the performance of electrochemical energy storage(EES)devices.Typically,the electrode materials are physically mixed with polymer binders and conductive additives,which are then loaded on the current collectors to function in real devices.Such a configuration inevitably reduces the content of active species and introduces quite some undesired interfaces that bring down the energy densities and power capabilities.One viable solution to address this issue is to construct self-supported electrodes where the active species,for example transition metal oxides(TMOs),are directly integrated with conductive substrates without polymer binders and conductive additives.In this review,the recent progress of self-supported TMO-based electrodes for EES devices including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs),aluminum-ion batteries(AIBs),metal-air batteries,and supercapacitors(SCs),is discussed in great detail.The focused attention is firstly concentrated on their structural design and controllable synthesis.Then,the mechanism understanding of the enhanced electrochemical performance is presented.Finally,the challenges and prospects of self-supported TMO-based electrodes are summarized to end this review.

Sodium vanadium oxides:From nanostructured design to high-performance energy storage materials

Developing high-capacity and low-cost cathode materials for metal-ion rechargeable batteries is the mainstream trend and is also the key to providing breakthroughs in making high-energy rechargeable batteries.Vanadium has a variety of valence states and can form a variety of vanadate structures.As a typical positive electrode material,vanadate has abundant ion adsorption sites,a unique“pillar”framework,and a typical layered structure.Therefore,it has the advantages of high specific capacity and excellent rate performance,possessing the prospect of being a large-capacity energy storage material.In this review,we focus on applications of sodium vanadium oxides(NVO)in electrical energy storage(EES)devices and summarize sodium vanadate materials from three aspects,including crystal structure,electrochemical performance,and energy storage mechanism.The recent progress of NVO-based highperformance energy storage materials along with nanostructured design strategies was provided and discussed as well.This review is intended to serve as general guidance for researchers to develop desirable sodium vanadate materials.