Cobalt sulphides attract much attention as anode materials for Li-ion batteries(LIBs).However,its poor conductivity,low initial column efficiency and large volume changes during cycling have hindered its further devel...Cobalt sulphides attract much attention as anode materials for Li-ion batteries(LIBs).However,its poor conductivity,low initial column efficiency and large volume changes during cycling have hindered its further development.Herein,novel interlaced CoS nanosheets were firstly prepared on Carbon Fiber Cloth(CFC)by two hydrothermal reactions followed with carbon coating via carbonizing dopamine(CoS NS@C/CFC).As a freestanding anode,the nanosheet structure of CoS not only accommodates the volume variation,but also provides a large interface area to proceed the charge transfer reaction.In addition,CFC works as both a three-dimensional skeleton and an active substance which can further improve the areal capacity of the resulting electrode.Furthermore,the coated carbon combined with the CFC work as a 3D conductive network to facilitate the electron conduction.The obtained CoS NS@C/CFC,and the contrast sample prepared with the same procedure but without carbon coating(CoS NS/CFC),are characterized with XRD,SEM,TEM,XPS and electrochemical measurements.The results show that the CoS NS@C/CFC possesses much improved electrochemical performance due to the synergistic effect of nanosheet CoS,the coated carbon and the CFC substrate,exhibiting high initial columbic efficiency(~87%),high areal capacity(2.5 at 0.15 mA cm−2),excellent rate performance(1.6 at 2.73 mA cm−2)and improved cycle stability(87.5%capacity retention after 300 cycles).This work may provide a new route to explore freestanding anodes with high areal specific capacity for LIBs.展开更多
MoOnanocrystals(NCs) on Ni foam were simply synthesized via a facile hydrothermal method and a dip-coating method. It was worth noting that ultrafine interconnected MoOnanocrystals(about 10 nm) were uniformly anchored...MoOnanocrystals(NCs) on Ni foam were simply synthesized via a facile hydrothermal method and a dip-coating method. It was worth noting that ultrafine interconnected MoOnanocrystals(about 10 nm) were uniformly anchored on Ni foam to fabricate a particular three-dimensional architecture, which may provide more active sites and shorter transmission pathways for lithium ions. As binder-free anode, MoONCs on Ni foam deliver a high initial discharge capacity of 990 mAh·gand retain a reversible capacity of 924 mAh· g(-1) after 100 cycles at a current density of 0.1 C. More importantly, when the current density returns from 2 C to 0.1 C, the capacity recovers to 910 mAh·g(-1)(about 92% of the original high capacity), suggesting excellent cycling stability and rate capability. The particular 3 D electrode as binder-free anode makes it a promising anode candidate for high-performance lithium-ion batteries.展开更多
Generally,the practical capacity of an electrode should include the weight of non-active components such as current collector,polymer binder,and conductive additives,which were as high as 70 wt%in current reported wor...Generally,the practical capacity of an electrode should include the weight of non-active components such as current collector,polymer binder,and conductive additives,which were as high as 70 wt%in current reported works,seriously limiting the practical capacity.This work pioneered the usage of ultralight reduced graphene fiber(rGF)fabrics as conductive scaffolds,aiming to reduce the weight of nonactive components and enhance the practical capacity.Ultrathin SnS2 nanosheets/rGF hybrids were prepared and used as binder-free electrodes of sodium-ion batteries(SIBs).The interfused graphene fibers endow the electrode a porous,continuous,and conductive network.The in situ phase transformation from SnO2 to SnS2 could preserve the strong interfacial interactions between SnS2 and graphene.Benefitting from these,the designed binder-free electrode delivers a high specific capacity of 500 mAh g?1 after 500 cycles at a current rate of 0.5 A g?1 with almost 100%Coulombic efficiency.Furthermore,the weight percentage of SnS2 in the whole electrode could reach up to 67.2 wt%,much higher than that of common electrode configurations using Cu foil,Al foil,or carbon cloth,significantly highlighting the ultralight characters and advantages of the rGF fabrics for using as binder-free electrodes of SIBs.展开更多
Molybdenum sulfide(MoS_(2))with well-designed porous structure has the potential to be great electrode materials in sodium-ion batteries due to its high theoretical capacity and abundant resource,however,hindered by i...Molybdenum sulfide(MoS_(2))with well-designed porous structure has the potential to be great electrode materials in sodium-ion batteries due to its high theoretical capacity and abundant resource,however,hindered by its intrinsic low conductivity and stability.Herein,MoS_(2) with 3 D macroporous foam structure and high conductivity was obtained through SiO_(2) templates and integrated with carbon paper(3 D FMoS_(2)/CP).It has showed superior specific capacity(225 m A h g^(-1),0.4–3 V)and cycling stability(1000 cycles)at high rate(2000 m A g^(-1)),with a low decay rate(0.033%per cycle)in sodium-ion batteries.The excellent electrochemical performance may originate from its unique integrated structure:3 D MoS_(2) macropores providing high surface area and abundant transfer channels while carbon paper enhancing the conductivity of MoS_(2) and avoiding unnecessary side reactions brought by binder addition.展开更多
Antimony-based materials are considered as promising anodes for potassium ion batteries due to their high theoretical capacity and low electrode potential. However, the aggregation and bulk expansion of Sb particles i...Antimony-based materials are considered as promising anodes for potassium ion batteries due to their high theoretical capacity and low electrode potential. However, the aggregation and bulk expansion of Sb particles in cycling will cause capacity attenuation and poor rate performance. In this paper, Sb nanoplates were designed to be embedded in flexible porous N-dopped carbon nanofibers(Sb@PCNFs)by a simple electrospinning deposition(ESD) method. In this structural design, Sb nanoplates of high capacity were employed as active materials, N-dopped carbon nanofibers were used to improve conductivity and structural stability. The introduction of pore-forming agent enables the nanofibers to possess porous structure, thus buffering the huge volume change and promoting the transfer of electrolyte/ions.More importantly, the freestanding film can be directly used as a working electrode, reducing the redundancy in the battery and the cost. Benefitting from the favorable structure, the freestanding flexible Sb@PCNFs electrode shows excellent potassium storage performance with a capacity of 314 m Ah/g after 2000 cycles at 500 m A/g. This strategy of employing active material with high capacity in porous and conductive flexible nanofibers represents an effective method of achieving binder-free electrode with good electrochemical performance towards wearable energy storage devices.展开更多
Eliminating the usage of metal current collectors and binders in traditional battery electrode configuration is an effective strategy to significantly improve the capacities of lithium ion batteries (LIBs). Herein, we...Eliminating the usage of metal current collectors and binders in traditional battery electrode configuration is an effective strategy to significantly improve the capacities of lithium ion batteries (LIBs). Herein, we demonstrate the construction of porous vanadium nitride (VN) nanosheet network in situ grown on nitrogen-rich (N-rich) carbon textile (N-C@P-VN) as lightweight and binder-free anode for LIBs. The N-rich carbon textile is used both as the current collector and host to store Li^(+), thus improving the specific capacities of binder-free VN anode and meanwhile reducing the inert mass of the whole cell. Moreover, the open spaces in carbon textile and vertically aligned pores in VN nanosheet network can not only provide an expressway for Li+ and e− transport, but also afford more active sites. As a result, the binder-free N-C@P-VN anode maintains a specific capacity of 1,040 mAh·g^(−1) (or an areal capacity of 2.6 mAh·cm^(−2)) after 100 cycles at 0.1 mA·cm^(−2) in half cell. Moreover, in an assembled N-C@P-VN//LiFePO4 full cell, it exhibits an areal capacity of 1.7 mAh·cm^(−2) after 300 cycles at 0.1 C. The synergistic strategy of N-C substrate and porous VN network could be applied to guide rational design of similar N-C@nitride or sulfide hybrid systems with corresponding sulfur-doped carbon textile as the substrate.展开更多
Metal-air battery is an environmental friendly energy storage system with unique open structure.Magnesium(Mg)and its alloys have been extensively attempted as anodes for air batteries due to high theoretical energy de...Metal-air battery is an environmental friendly energy storage system with unique open structure.Magnesium(Mg)and its alloys have been extensively attempted as anodes for air batteries due to high theoretical energy density,low cost,and recyclability.However,the study on Mg-air battery(MAB)is still at the laboratory level currently,mainly owing to the low anodic efficiency caused by the poor corrosion resistance.In order to reduce corrosion losses and achieve optimal utilization efficiency of Mg anode,the design strategies are reviewed from microstructure perspectives.Firstly,the corrosion behaviors have been discussed,especially the negative difference effect derived by hydrogen evolution.Special attention is given to the effect of anode micro-structures on the MAB,which includes grain size,grain orientation,second phases,crystal structure,twins,and dislocations.For further improvement,the discharge performance,long period stacking ordered phase and its enhancing effect are considered.Meanwhile,given the current debates over Mg dendrites,the potential risk,the impact on discharge,and the elimination strategies are discussed.Microstructure control and single crystal would be promising ways for MAB anode.展开更多
Zinc-ion batteries(ZIBs) are recognized as potential energy storage devices due to their advantages of low cost, high energy density, and environmental friendliness. However, zinc anodes are subject to unavoidable zin...Zinc-ion batteries(ZIBs) are recognized as potential energy storage devices due to their advantages of low cost, high energy density, and environmental friendliness. However, zinc anodes are subject to unavoidable zinc dendrites, passivation, corrosion, and hydrogen evolution reactions during the charging and discharging of batteries, becoming obstacles to the practical application of ZIBs. Appropriate zinc metal-free anodes provide a higher working potential than metallic zinc anodes, effectively solving the problems of zinc dendrites, hydrogen evolution, and side reactions during the operation of metallic zinc anodes. The improvement in the safety and cycle life of batteries creates conditions for further commercialization of ZIBs. Therefore, this work systematically introduces the research progress of zinc metal-free anodes in “rocking chair” ZIBs. Zinc metal-free anodes are mainly discussed in four categories: transition metal oxides,transition metal sulfides, MXene(two dimensional transition metal carbide) composites, and organic compounds, with discussions on their properties and zinc storage mechanisms. Finally, the outlook for the development of zinc metal-free anodes is proposed. This paper is expected to provide a reference for the further promotion of commercial rechargeable ZIBs.展开更多
As the anode active substance of lithium ions battery(LIB),the low conductivity/ion diffusivity and large volume changes of tungsten oxide(WO_(3))lead to its serious polarization during the lithiation/delithiation pro...As the anode active substance of lithium ions battery(LIB),the low conductivity/ion diffusivity and large volume changes of tungsten oxide(WO_(3))lead to its serious polarization during the lithiation/delithiation process,decreasing the cycling stability.To address these challenges,a binder-free anode consisting of nitrogen-doped tungsten oxide nanosheets,encapsulated in carbon layers(N-doped WO_(3)@CL)and entangled with carbon nanotubes macro-films(CMF),was successfully synthesized through a combination of hydrothermal and online assembly method.Compared with the pristine tungsten oxide entangled with carbon nanotubes macro-films(WO_(3)@CMF),the synthesized N-doped WO_(3)@CL@CMF as a binder-free LIB anode demonstrated better electrochemical performance,which could be attributed to(1)surface defects of WO_(3)created by N dopant providing more channels to improve Li^(+)diffusion,(2)the N-doped WO_(3)@CL with a flower-like structure shortening the diffusion length of Li^(+)ions and further leading to high Li^(+)incorporation,and(3)carbon layers and carbon nanotubes synergistically alleviating the large volume change of the N-doped WO_(3)@CL@CMF electrode during the charging and discharging process.The present study offers insights into employing nitrogen dopant and a carbon matrix to mediate the conductivity and wrapped structure in the WO_(3)semiconductor powder,which provides an important strategy for large-scale design of the binder-free LIB anode with high performance.展开更多
Free-standing silicon anodes with high proportion of active materials have aroused great attention;however,the mechanical stability and electrochemical performance are severely suppressed.Herein,to resolve the appeal ...Free-standing silicon anodes with high proportion of active materials have aroused great attention;however,the mechanical stability and electrochemical performance are severely suppressed.Herein,to resolve the appeal issues,a free-standing anode with a"corrugated paper"shape on micro-scale and a topological crosslinking network on the submicron and nano-scale is designed.Essentially,an integrated three-dimensional electrode structure is constructed based on robust carbon nanotubes network with firmly anchored SiNPs via forming interlocking junctions.In which,the hierarchical interlocking structure is achieved by directional induction of the binder,which ensures well integration during cycling so that significantly enhances mechanical stability as well as electronic and ionic conductivity of electrodes.Benefiting from it,this anode exhibits outsta nding performance under harsh service conditions including high Si loading,ultrahigh areal capacity(33.2 mA h cm^(-2)),and high/low temperatures(-15-60℃),which significantly extends its practical prospect.Furthermore,the optimization mechanism of this electrode is explored to verify the crack-healing and structure-integration maintaining along cycling via a unique self-stabilization process.Thus,from both the fundamental and engineering views,this strategy offers a promising path to produce high-performance free-standing electrodes for flexible device applications especially facing volume effect challenges.展开更多
With graphite currently leading as the most viable anode for potassium-ion batteries(KIBs),other materials have been left relatively underexamined.Transition metal oxides are among these,with many positive attributes ...With graphite currently leading as the most viable anode for potassium-ion batteries(KIBs),other materials have been left relatively underexamined.Transition metal oxides are among these,with many positive attributes such as synthetic maturity,longterm cycling stability and fast redox kinetics.Therefore,to address this research deficiency we report herein a layered potassium titanium niobate KTiNbO5(KTNO)and its rGO nanocomposite(KTNO/rGO)synthesised via solvothermal methods as a high-performance anode for KIBs.Through effective distribution across the electrically conductive rGO,the electrochemical performance of the KTNO nanoparticles was enhanced.The potassium storage performance of the KTNO/rGO was demonstrated by its first charge capacity of 128.1 mAh g^(−1) and reversible capacity of 97.5 mAh g^(−1) after 500 cycles at 20 mA g^(−1),retaining 76.1%of the initial capacity,with an exceptional rate performance of 54.2 mAh g^(−1)at 1 A g^(−1).Furthermore,to investigate the attributes of KTNO in-situ XRD was performed,indicating a low-strain material.Ex-situ X-ray photoelectron spectra further investigated the mechanism of charge storage,with the titanium showing greater redox reversibility than the niobium.This work suggests this lowstrain nature is a highly advantageous property and well worth regarding KTNO as a promising anode for future high-performance KIBs.展开更多
Over the years,zinc-ion batteries(ZIBs)have attracted attention as a promising next-generation energy storage technology because of their excellent safety,long cycling performance,eco-friendliness,and high-power densi...Over the years,zinc-ion batteries(ZIBs)have attracted attention as a promising next-generation energy storage technology because of their excellent safety,long cycling performance,eco-friendliness,and high-power density.However,issues,such as the corrosion and dissolution of the Zn anode,limited wet-tability,and lack of sufficient nucleation sites for Zn plating,have limited their practical application.The introduction of a protective layer comprising of tellurium(Te)nanobelts onto the surface of Zn anode has emerged as a promising approach to overcome these limitations and improve the electrochemical behav-ior by enhancing the safety and wettability of ZIBs,as well as providing numerous nucleation sites for Zn plating.In the presence of a Te-based protective layer,the energy power density of the surface-engineered Zn anode improved significantly(ranging from 310 to 144 W h kg^(-1),over a power density range of 270 to 1,800 W kg^(-1)),and the lifespan capability was extended.These results demonstrate that the proposed strategy of employing Te nanobelts as a protective layer holds great promise for enhancing the energy storage performance of zIBs,making them even more attractive as a viable energy storage solution forthefuture.展开更多
The severe degradation of electrochemical performance for lithium-ion batteries(LIBs)at low temperatures poses a significant challenge to their practical applications.Consequently,extensive efforts have been contribut...The severe degradation of electrochemical performance for lithium-ion batteries(LIBs)at low temperatures poses a significant challenge to their practical applications.Consequently,extensive efforts have been contributed to explore novel anode materials with high electronic conductivity and rapid Li^(+)diffusion kinetics for achieving favorable low-temperature performance of LIBs.Herein,we try to review the recent reports on the synthesis and characterizations of low-temperature anode materials.First,we summarize the underlying mechanisms responsible for the performance degradation of anode materials at subzero temperatures.Second,detailed discussions concerning the key pathways(boosting electronic conductivity,enhancing Li^(+)diffusion kinetics,and inhibiting lithium dendrite)for improving the low-temperature performance of anode materials are presented.Third,several commonly used low-temperature anode materials are briefly introduced.Fourth,recent progress in the engineering of these low-temperature anode materials is summarized in terms of structural design,morphology control,surface&interface modifications,and multiphase materials.Finally,the challenges that remain to be solved in the field of low-temperature anode materials are discussed.This review was organized to offer valuable insights and guidance for next-generation LIBs with excellent low-temperature electrochemical performance.展开更多
Zinc-ion batteries(ZIBs)are considered to be one of the most promising candidates to replace lithium-ion batteries(LIBs)due to the high theoretical capacity,low cost and intrinsic safety.However,zinc dendrites,hydroge...Zinc-ion batteries(ZIBs)are considered to be one of the most promising candidates to replace lithium-ion batteries(LIBs)due to the high theoretical capacity,low cost and intrinsic safety.However,zinc dendrites,hydrogen evolution reaction,surface passivation and other side reactions will inevitably occur during the charging and discharging process of Zn anode,which will seriously affect the cycle stability of the battery and hinder its practical application.The etching strategy of Zn anode has attracted wide attention because of its simple operation and broad commercial prospects,and the etched Zn anode can effectively improve its electrochemical performance.However,there is no comprehensive review of the etching strategy of Zn anode.This review first summarizes the challenges faced by Zn anode,then puts forward the etching mechanisms and properties of acid,salt and other etchants.Finally,based on the above discussion,the challenges and opportunities of Zn anode etching strategy are proposed.展开更多
The recycling of graphite from spent lithium-ion batteries(LIBs)is overlooked due to its relatively low added value and the lack of efficient recovering methods.To reuse the spent graphite anodes,we need to eliminate ...The recycling of graphite from spent lithium-ion batteries(LIBs)is overlooked due to its relatively low added value and the lack of efficient recovering methods.To reuse the spent graphite anodes,we need to eliminate their useless components(mainly the degraded solid electrolyte interphase,SEI)and reconstruct their damaged structure.Herein,a facile and efficient strategy is proposed to recycle the spent graphite on the basis of the careful investigation of the composition of the cycled graphite anodes and the rational design of the regeneration processes.The regenerated graphite,which is revitalized by calcination treatment and acid leaching,delivers superb rate performance and a high specific capacity of 370 mAh g^(-1)(~99% of its theoretical capacity)after 100 cycles at 0.1 C,superior to the commercial graphite anodes.The improved electrochemical performance could be attributed to unchoked Li^(+) transport channels and enhanced charge transfer reaction due to the effective destruction of the degraded SEI and the full recovery of the damaged structure of the spent graphite.This work clarifies that the electrochemical performance of the regenerated graphite could be deteriorated by even a trace amount of the residual“impurity”and provides a facile method for the efficient regeneration of graphite anodes.展开更多
Graphite interfaces are an important part of the anode in lithium-ion batteries(LIBs),significantly influencing Li intercalation kinetics.Graphite anodes adopt different stacking sequences depending on the concentrati...Graphite interfaces are an important part of the anode in lithium-ion batteries(LIBs),significantly influencing Li intercalation kinetics.Graphite anodes adopt different stacking sequences depending on the concentration of the intercalated Li ions.In this work,we performed first-principles calculations to comprehensively address the energetics and dynamics of Li intercalation and Li vacancy diffusion near the no n-basal edges of graphite,namely the armchair and zigzag-edges,at high Li concentration.We find that surface effects persist in stage-Ⅱ that bind Li strongly at the edge sites.However,the pronounced effect previously identified at the zigzag edge of pristine graphite is reduced in LiC_(12),penetrating only to the subsurface site,and eventually disappearing in LiC_(6).Consequently,the distinctive surface state at the zigzag edge significantly impacts and restrains the charging rate at the initial lithiation of graphite anodes,whilst diminishes with an increasing degree of lithiation.Longer diffusion time for Li hopping to the bulk site from either the zigzag edge or the armchair edge in LiC_(6) was observed during high state of charge due to charge repulsion.Effectively controlling Li occupation and diffusion kinetics at this stage is also crucial for enhancing the charge rate.展开更多
Metallic lithium(Li)is considered the“Holy Grail”anode material for the nextgeneration of Li batteries with high energy density owing to the extraordinary theoretical specific capacity and the lowest negative electr...Metallic lithium(Li)is considered the“Holy Grail”anode material for the nextgeneration of Li batteries with high energy density owing to the extraordinary theoretical specific capacity and the lowest negative electrochemical potential.However,owing to inhomogeneous Li-ion flux,Li anodes undergo uncontrollable Li deposition,leading to limited power output and practical applications.Carbon materials and their composites with controllable structures and properties have received extensive attention to guide the homogeneous growth of Li to achieve high-performance Li anodes.In this review,the correlation between the behavior of Li anode and the properties of carbon materials is proposed.Subsequently,we review emerging strategies for rationally designing high-performance Li anodes with carbon materials,including interface engineering(stabilizing solid electrolyte interphase layer and other functionalized interfacial layer)and architecture design of host carbon(constructing three-dimension structure,preparing hollow structure,introducing lithiophilic sites,optimizing geometric effects,and compositing with Li).Based on the insights,some prospects on critical challenges and possible future research directions in this field are concluded.It is anticipated that further innovative works on the fundamental chemistry and theoretical research of Li anodes are needed.展开更多
Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes th...Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes the electrode structure instability,leading to poor cyclic stability.What’s worse,the natural Al2O3 layer on commercial Al pellets is always existed as a robust insulating barrier for elec-trons,which brings the voltage dip and results in low reversible capacity.Herein,this work synthesized core-shell Al@C-Sn pellets for LIBs by a plus-minus strategy.In this proposal,the natural Al2O3 passivation layer is eliminated when annealing the pre-introduced SnCl2,meanwhile,polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alle-viate the volume swellings.Benefiting from the addition of C-Sn shell and the elimination of the Al2O3 passivation layer,the as-prepared Al@C-Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g^(-1) at 0.1 A·g^(-1) and 295.0 mAh·g^(-1) at 2.0 A·g^(-1)(after 1000 cycles),respectively.Moreover,its diffusion-controlled capacity is muchly improved compared to those of its counterparts,confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.展开更多
Silicon monoxide(SiO)(silicon[Si]mixed with silicon dioxide[SiO_(2)])/graphite(Gr)composite material is one of the most commercially promising anode materials for the next generation of high-energy-density lithium-ion...Silicon monoxide(SiO)(silicon[Si]mixed with silicon dioxide[SiO_(2)])/graphite(Gr)composite material is one of the most commercially promising anode materials for the next generation of high-energy-density lithium-ion batteries.The major bottleneck for SiO/Gr composite anode is the poor cyclability arising from the stress/strain behaviors due to the mismatch between two heterogenous materials during the lithiation/delithiation process.To date,a meticulous and quantitative understanding of the highly nonlinear coupling behaviors of such materials is still lacking.Herein,an electro–chemo–mechanics-coupled detailed model containing particle geometries is established.The underlying mechanism of the regulation between SiO and Gr components during electrochemical cycling is quantitatively revealed.We discover that increasing the SiO weight percentage(wt%)reduces the utilization efficiency of the active materials at the same 1C rate charging and enhances the hindering effects of stress-driven flux on diffusion.In addition,the mechanical constraint demonstrates a balanced effect on the overall performance of cells and the local behaviors of particles.This study provides new insights into the fundamental interactions between SiO and Gr materials and advances the investigation methodology for the design and evaluation of next-generation high-energydensity batteries.展开更多
Zincophilic property and high electrical conductivity are both very important parameters to design novel Zn anode for aqueous Zn-ion batteries(AZIBs).However,single material is difficult to exhibit zincophilic propert...Zincophilic property and high electrical conductivity are both very important parameters to design novel Zn anode for aqueous Zn-ion batteries(AZIBs).However,single material is difficult to exhibit zincophilic property and high electrical conductivity at the same time.Herein,originating from theoretical calculation,a zincophilic particle regulation strategy is proposed to address these limitations and carbon coated Na_(3)V_(2)(PO_(4))_(3)is taken as an example to be a protective layer on zinc metal(NVPC@Zn).Na_(3)V_(2)(PO_(4))_(3)(NVP)is a common cathode material for Zn-ion batteries,which is zincophilic.Carbon materials not only offer an electron pathway to help Zn deposition onto NVPC surface,but also enhance the zinc nucleophilicity of Na_(3)V_(2)(PO_(4))_(3).Hence,this hybrid coating layer can tune zinc deposition and resist side reactions such as hydrogen generation and Zn metal corrosion.Experimentally,a symmetrical battery with NVPC@Zn electrode displays highly reversible plating/stripping behavior with a long cycle lifespan over 1800 h at2 mA cm^(-2),much better than carbon and Na_(3)V_(2)(PO_(4))_(3)solely modified Zn electrodes.When the Na_(3)V_(2)(PO_(4))_(3)is replaced with zincophobic Al2O3or zincophilic V2O3,the stability of the modified zinc anodes is also prolonged.This strategy expands the option of zincophilic materials and provides a general and effective way to stabilize the Zn electrode.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos.21573109,21206069)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).
文摘Cobalt sulphides attract much attention as anode materials for Li-ion batteries(LIBs).However,its poor conductivity,low initial column efficiency and large volume changes during cycling have hindered its further development.Herein,novel interlaced CoS nanosheets were firstly prepared on Carbon Fiber Cloth(CFC)by two hydrothermal reactions followed with carbon coating via carbonizing dopamine(CoS NS@C/CFC).As a freestanding anode,the nanosheet structure of CoS not only accommodates the volume variation,but also provides a large interface area to proceed the charge transfer reaction.In addition,CFC works as both a three-dimensional skeleton and an active substance which can further improve the areal capacity of the resulting electrode.Furthermore,the coated carbon combined with the CFC work as a 3D conductive network to facilitate the electron conduction.The obtained CoS NS@C/CFC,and the contrast sample prepared with the same procedure but without carbon coating(CoS NS/CFC),are characterized with XRD,SEM,TEM,XPS and electrochemical measurements.The results show that the CoS NS@C/CFC possesses much improved electrochemical performance due to the synergistic effect of nanosheet CoS,the coated carbon and the CFC substrate,exhibiting high initial columbic efficiency(~87%),high areal capacity(2.5 at 0.15 mA cm−2),excellent rate performance(1.6 at 2.73 mA cm−2)and improved cycle stability(87.5%capacity retention after 300 cycles).This work may provide a new route to explore freestanding anodes with high areal specific capacity for LIBs.
基金Funded by the National Natural Science Foundation of China(51506155)
文摘MoOnanocrystals(NCs) on Ni foam were simply synthesized via a facile hydrothermal method and a dip-coating method. It was worth noting that ultrafine interconnected MoOnanocrystals(about 10 nm) were uniformly anchored on Ni foam to fabricate a particular three-dimensional architecture, which may provide more active sites and shorter transmission pathways for lithium ions. As binder-free anode, MoONCs on Ni foam deliver a high initial discharge capacity of 990 mAh·gand retain a reversible capacity of 924 mAh· g(-1) after 100 cycles at a current density of 0.1 C. More importantly, when the current density returns from 2 C to 0.1 C, the capacity recovers to 910 mAh·g(-1)(about 92% of the original high capacity), suggesting excellent cycling stability and rate capability. The particular 3 D electrode as binder-free anode makes it a promising anode candidate for high-performance lithium-ion batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.21503025,21503178 and 21603019)Fundamental Research Funds for the Central Universities(Nos.0903005203377 and 106112016CDJZR325520)+3 种基金Key Program for International Science and Technology Cooperation Projects of Ministry of Science and Technology of China(No.2016YFE0125900)Venture and Innovation Support Program for Chongqing Overseas Returnees(cx2017060 and cx2017115)Chongqing Research Program of Basic Research and Frontier Technology(No.cstc2016jcyjA1059)Hundred Talents Program of Chongqing University.
文摘Generally,the practical capacity of an electrode should include the weight of non-active components such as current collector,polymer binder,and conductive additives,which were as high as 70 wt%in current reported works,seriously limiting the practical capacity.This work pioneered the usage of ultralight reduced graphene fiber(rGF)fabrics as conductive scaffolds,aiming to reduce the weight of nonactive components and enhance the practical capacity.Ultrathin SnS2 nanosheets/rGF hybrids were prepared and used as binder-free electrodes of sodium-ion batteries(SIBs).The interfused graphene fibers endow the electrode a porous,continuous,and conductive network.The in situ phase transformation from SnO2 to SnS2 could preserve the strong interfacial interactions between SnS2 and graphene.Benefitting from these,the designed binder-free electrode delivers a high specific capacity of 500 mAh g?1 after 500 cycles at a current rate of 0.5 A g?1 with almost 100%Coulombic efficiency.Furthermore,the weight percentage of SnS2 in the whole electrode could reach up to 67.2 wt%,much higher than that of common electrode configurations using Cu foil,Al foil,or carbon cloth,significantly highlighting the ultralight characters and advantages of the rGF fabrics for using as binder-free electrodes of SIBs.
基金supported financially by the National Key R&D Program of China(No.2016YFA0204100,2016YFA0200200)the National Natural Science Foundation of China(No.21890753,21988101,21905035)+1 种基金the Danish company Haldor Tops?e A/S,Liaoning Revitalization Talents Program(XLYC1907093)the Liaoning Natural Science Foundation(20180510043)。
文摘Molybdenum sulfide(MoS_(2))with well-designed porous structure has the potential to be great electrode materials in sodium-ion batteries due to its high theoretical capacity and abundant resource,however,hindered by its intrinsic low conductivity and stability.Herein,MoS_(2) with 3 D macroporous foam structure and high conductivity was obtained through SiO_(2) templates and integrated with carbon paper(3 D FMoS_(2)/CP).It has showed superior specific capacity(225 m A h g^(-1),0.4–3 V)and cycling stability(1000 cycles)at high rate(2000 m A g^(-1)),with a low decay rate(0.033%per cycle)in sodium-ion batteries.The excellent electrochemical performance may originate from its unique integrated structure:3 D MoS_(2) macropores providing high surface area and abundant transfer channels while carbon paper enhancing the conductivity of MoS_(2) and avoiding unnecessary side reactions brought by binder addition.
基金the financial support from the National Natural Science Foundation of China (Nos. 51872071, 52172173)Anhui Provincial Natural Science Foundation for Distinguished Young Scholar(No. 2108085J25)Natural Science Research Projects of Universities in Anhui Province (No. KJ2020A0021)。
文摘Antimony-based materials are considered as promising anodes for potassium ion batteries due to their high theoretical capacity and low electrode potential. However, the aggregation and bulk expansion of Sb particles in cycling will cause capacity attenuation and poor rate performance. In this paper, Sb nanoplates were designed to be embedded in flexible porous N-dopped carbon nanofibers(Sb@PCNFs)by a simple electrospinning deposition(ESD) method. In this structural design, Sb nanoplates of high capacity were employed as active materials, N-dopped carbon nanofibers were used to improve conductivity and structural stability. The introduction of pore-forming agent enables the nanofibers to possess porous structure, thus buffering the huge volume change and promoting the transfer of electrolyte/ions.More importantly, the freestanding film can be directly used as a working electrode, reducing the redundancy in the battery and the cost. Benefitting from the favorable structure, the freestanding flexible Sb@PCNFs electrode shows excellent potassium storage performance with a capacity of 314 m Ah/g after 2000 cycles at 500 m A/g. This strategy of employing active material with high capacity in porous and conductive flexible nanofibers represents an effective method of achieving binder-free electrode with good electrochemical performance towards wearable energy storage devices.
基金This work was supported by the National Natural Science Foundation of China(No.21872008)the Natural Science Foundation of Beijing,China(No.2212019)Beijing Institute of Technology Research Fund Program for Young Scholars(Nos.3100011182019 and 3100011182128).We would also thank the Analysis&Testing Center of Beijing Institute of Technology measurements.
文摘Eliminating the usage of metal current collectors and binders in traditional battery electrode configuration is an effective strategy to significantly improve the capacities of lithium ion batteries (LIBs). Herein, we demonstrate the construction of porous vanadium nitride (VN) nanosheet network in situ grown on nitrogen-rich (N-rich) carbon textile (N-C@P-VN) as lightweight and binder-free anode for LIBs. The N-rich carbon textile is used both as the current collector and host to store Li^(+), thus improving the specific capacities of binder-free VN anode and meanwhile reducing the inert mass of the whole cell. Moreover, the open spaces in carbon textile and vertically aligned pores in VN nanosheet network can not only provide an expressway for Li+ and e− transport, but also afford more active sites. As a result, the binder-free N-C@P-VN anode maintains a specific capacity of 1,040 mAh·g^(−1) (or an areal capacity of 2.6 mAh·cm^(−2)) after 100 cycles at 0.1 mA·cm^(−2) in half cell. Moreover, in an assembled N-C@P-VN//LiFePO4 full cell, it exhibits an areal capacity of 1.7 mAh·cm^(−2) after 300 cycles at 0.1 C. The synergistic strategy of N-C substrate and porous VN network could be applied to guide rational design of similar N-C@nitride or sulfide hybrid systems with corresponding sulfur-doped carbon textile as the substrate.
基金supported by National Natural Science Foundation of China(52371095)Innovation Research Group of Universities in Chongqing(CXQT21030)+2 种基金Chongqing Talents:Exceptional Young Talents Project(CQYC201905100)Chongqing Youth Expert Studio,Chongqing Overseas Chinese Entrepreneurship and Innovation Support Program(cx2023117)Chongqing Natural Science Foundation Innovation and Development Joint Fund(CSTB 2022NS CQLZX0054)。
文摘Metal-air battery is an environmental friendly energy storage system with unique open structure.Magnesium(Mg)and its alloys have been extensively attempted as anodes for air batteries due to high theoretical energy density,low cost,and recyclability.However,the study on Mg-air battery(MAB)is still at the laboratory level currently,mainly owing to the low anodic efficiency caused by the poor corrosion resistance.In order to reduce corrosion losses and achieve optimal utilization efficiency of Mg anode,the design strategies are reviewed from microstructure perspectives.Firstly,the corrosion behaviors have been discussed,especially the negative difference effect derived by hydrogen evolution.Special attention is given to the effect of anode micro-structures on the MAB,which includes grain size,grain orientation,second phases,crystal structure,twins,and dislocations.For further improvement,the discharge performance,long period stacking ordered phase and its enhancing effect are considered.Meanwhile,given the current debates over Mg dendrites,the potential risk,the impact on discharge,and the elimination strategies are discussed.Microstructure control and single crystal would be promising ways for MAB anode.
基金financially supported by the National Natural Science Foundation of China (Nos.51872090 and51772097)the Hebei Natural Science Fund for Distinguished Young Scholar,China (No.E2019209433)+2 种基金the Youth Talent Program of Hebei Provincial Education Department,China (No.BJ2018020)the Natural Science Foundation of Hebei Province,China (No.E2020209151)the Science and Technology Project of Hebei Education Department,China (No.SLRC2019028)。
文摘Zinc-ion batteries(ZIBs) are recognized as potential energy storage devices due to their advantages of low cost, high energy density, and environmental friendliness. However, zinc anodes are subject to unavoidable zinc dendrites, passivation, corrosion, and hydrogen evolution reactions during the charging and discharging of batteries, becoming obstacles to the practical application of ZIBs. Appropriate zinc metal-free anodes provide a higher working potential than metallic zinc anodes, effectively solving the problems of zinc dendrites, hydrogen evolution, and side reactions during the operation of metallic zinc anodes. The improvement in the safety and cycle life of batteries creates conditions for further commercialization of ZIBs. Therefore, this work systematically introduces the research progress of zinc metal-free anodes in “rocking chair” ZIBs. Zinc metal-free anodes are mainly discussed in four categories: transition metal oxides,transition metal sulfides, MXene(two dimensional transition metal carbide) composites, and organic compounds, with discussions on their properties and zinc storage mechanisms. Finally, the outlook for the development of zinc metal-free anodes is proposed. This paper is expected to provide a reference for the further promotion of commercial rechargeable ZIBs.
基金This study was financially supported by the National Natural Science Foundation of China[Grant No.22062008]Supported by the program of Qingjiang Excellent Young Talents,Jiangxi University of Science and Technology[Grant No.JXUSTQJBJ2020008]+2 种基金the Special Fund for Postgraduate Innovation of Jiangxi Province[Grant No.YC2020-S458 and YC2021-S569]National Training Program for College Students’Innovation and Entrepreneurship[Grant No.202110407005X]the Postdoctoral Science Foundation of Jiangxi Province[Grant No.2019KY56 and 2018RC02].
文摘As the anode active substance of lithium ions battery(LIB),the low conductivity/ion diffusivity and large volume changes of tungsten oxide(WO_(3))lead to its serious polarization during the lithiation/delithiation process,decreasing the cycling stability.To address these challenges,a binder-free anode consisting of nitrogen-doped tungsten oxide nanosheets,encapsulated in carbon layers(N-doped WO_(3)@CL)and entangled with carbon nanotubes macro-films(CMF),was successfully synthesized through a combination of hydrothermal and online assembly method.Compared with the pristine tungsten oxide entangled with carbon nanotubes macro-films(WO_(3)@CMF),the synthesized N-doped WO_(3)@CL@CMF as a binder-free LIB anode demonstrated better electrochemical performance,which could be attributed to(1)surface defects of WO_(3)created by N dopant providing more channels to improve Li^(+)diffusion,(2)the N-doped WO_(3)@CL with a flower-like structure shortening the diffusion length of Li^(+)ions and further leading to high Li^(+)incorporation,and(3)carbon layers and carbon nanotubes synergistically alleviating the large volume change of the N-doped WO_(3)@CL@CMF electrode during the charging and discharging process.The present study offers insights into employing nitrogen dopant and a carbon matrix to mediate the conductivity and wrapped structure in the WO_(3)semiconductor powder,which provides an important strategy for large-scale design of the binder-free LIB anode with high performance.
基金sponsored by the National Natural Science Foundation of China(21905221,21805221)the Suzhou Technological innovation of key industries-research and development of key technologies(SGC2021118)。
文摘Free-standing silicon anodes with high proportion of active materials have aroused great attention;however,the mechanical stability and electrochemical performance are severely suppressed.Herein,to resolve the appeal issues,a free-standing anode with a"corrugated paper"shape on micro-scale and a topological crosslinking network on the submicron and nano-scale is designed.Essentially,an integrated three-dimensional electrode structure is constructed based on robust carbon nanotubes network with firmly anchored SiNPs via forming interlocking junctions.In which,the hierarchical interlocking structure is achieved by directional induction of the binder,which ensures well integration during cycling so that significantly enhances mechanical stability as well as electronic and ionic conductivity of electrodes.Benefiting from it,this anode exhibits outsta nding performance under harsh service conditions including high Si loading,ultrahigh areal capacity(33.2 mA h cm^(-2)),and high/low temperatures(-15-60℃),which significantly extends its practical prospect.Furthermore,the optimization mechanism of this electrode is explored to verify the crack-healing and structure-integration maintaining along cycling via a unique self-stabilization process.Thus,from both the fundamental and engineering views,this strategy offers a promising path to produce high-performance free-standing electrodes for flexible device applications especially facing volume effect challenges.
基金Y.X.acknowledges the financial support of the Engineering and Physical Sciences Research Council(EP/X000087/1,EP/V000152/1)Leverhulme Trust(RPG-2021-138)Royal Society(IEC\NSFC\223016).
文摘With graphite currently leading as the most viable anode for potassium-ion batteries(KIBs),other materials have been left relatively underexamined.Transition metal oxides are among these,with many positive attributes such as synthetic maturity,longterm cycling stability and fast redox kinetics.Therefore,to address this research deficiency we report herein a layered potassium titanium niobate KTiNbO5(KTNO)and its rGO nanocomposite(KTNO/rGO)synthesised via solvothermal methods as a high-performance anode for KIBs.Through effective distribution across the electrically conductive rGO,the electrochemical performance of the KTNO nanoparticles was enhanced.The potassium storage performance of the KTNO/rGO was demonstrated by its first charge capacity of 128.1 mAh g^(−1) and reversible capacity of 97.5 mAh g^(−1) after 500 cycles at 20 mA g^(−1),retaining 76.1%of the initial capacity,with an exceptional rate performance of 54.2 mAh g^(−1)at 1 A g^(−1).Furthermore,to investigate the attributes of KTNO in-situ XRD was performed,indicating a low-strain material.Ex-situ X-ray photoelectron spectra further investigated the mechanism of charge storage,with the titanium showing greater redox reversibility than the niobium.This work suggests this lowstrain nature is a highly advantageous property and well worth regarding KTNO as a promising anode for future high-performance KIBs.
基金supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)grant funded by the Korea government(MOTIE)(RS-2023-00303581,Multiscale Simulation-Driven Development of Cost-Effective and Stable Aqueous Zn Ion Battery with Energy Density of 110 Wh/L for Energy Storage Systems:A Korea-USA Collaboration)。
文摘Over the years,zinc-ion batteries(ZIBs)have attracted attention as a promising next-generation energy storage technology because of their excellent safety,long cycling performance,eco-friendliness,and high-power density.However,issues,such as the corrosion and dissolution of the Zn anode,limited wet-tability,and lack of sufficient nucleation sites for Zn plating,have limited their practical application.The introduction of a protective layer comprising of tellurium(Te)nanobelts onto the surface of Zn anode has emerged as a promising approach to overcome these limitations and improve the electrochemical behav-ior by enhancing the safety and wettability of ZIBs,as well as providing numerous nucleation sites for Zn plating.In the presence of a Te-based protective layer,the energy power density of the surface-engineered Zn anode improved significantly(ranging from 310 to 144 W h kg^(-1),over a power density range of 270 to 1,800 W kg^(-1)),and the lifespan capability was extended.These results demonstrate that the proposed strategy of employing Te nanobelts as a protective layer holds great promise for enhancing the energy storage performance of zIBs,making them even more attractive as a viable energy storage solution forthefuture.
基金supported by the National Key Research and Development Program of China(No.2019YFA0705601)the National Natural Science Foundation of China(No.U23A20122,52101267)the Key Science and Technology Special Project of Henan Province(No.201111311400).
文摘The severe degradation of electrochemical performance for lithium-ion batteries(LIBs)at low temperatures poses a significant challenge to their practical applications.Consequently,extensive efforts have been contributed to explore novel anode materials with high electronic conductivity and rapid Li^(+)diffusion kinetics for achieving favorable low-temperature performance of LIBs.Herein,we try to review the recent reports on the synthesis and characterizations of low-temperature anode materials.First,we summarize the underlying mechanisms responsible for the performance degradation of anode materials at subzero temperatures.Second,detailed discussions concerning the key pathways(boosting electronic conductivity,enhancing Li^(+)diffusion kinetics,and inhibiting lithium dendrite)for improving the low-temperature performance of anode materials are presented.Third,several commonly used low-temperature anode materials are briefly introduced.Fourth,recent progress in the engineering of these low-temperature anode materials is summarized in terms of structural design,morphology control,surface&interface modifications,and multiphase materials.Finally,the challenges that remain to be solved in the field of low-temperature anode materials are discussed.This review was organized to offer valuable insights and guidance for next-generation LIBs with excellent low-temperature electrochemical performance.
基金supported by the Science and Technology Research Project of the Education Department of Jilin Province (JJKH20230803KJ)。
文摘Zinc-ion batteries(ZIBs)are considered to be one of the most promising candidates to replace lithium-ion batteries(LIBs)due to the high theoretical capacity,low cost and intrinsic safety.However,zinc dendrites,hydrogen evolution reaction,surface passivation and other side reactions will inevitably occur during the charging and discharging process of Zn anode,which will seriously affect the cycle stability of the battery and hinder its practical application.The etching strategy of Zn anode has attracted wide attention because of its simple operation and broad commercial prospects,and the etched Zn anode can effectively improve its electrochemical performance.However,there is no comprehensive review of the etching strategy of Zn anode.This review first summarizes the challenges faced by Zn anode,then puts forward the etching mechanisms and properties of acid,salt and other etchants.Finally,based on the above discussion,the challenges and opportunities of Zn anode etching strategy are proposed.
基金supported by the National Key R&D Program of China(2021YFB2400300)Key R&D Program of Hubei Province of China(2020BAB088)+2 种基金National Natural Science Foundation of China(52002277)the Fundamental Research Funds for the Central Universities(2021GCRC001)Guangdong Basic and Applied Basic Reuter Foundation(2021A1515011748).
文摘The recycling of graphite from spent lithium-ion batteries(LIBs)is overlooked due to its relatively low added value and the lack of efficient recovering methods.To reuse the spent graphite anodes,we need to eliminate their useless components(mainly the degraded solid electrolyte interphase,SEI)and reconstruct their damaged structure.Herein,a facile and efficient strategy is proposed to recycle the spent graphite on the basis of the careful investigation of the composition of the cycled graphite anodes and the rational design of the regeneration processes.The regenerated graphite,which is revitalized by calcination treatment and acid leaching,delivers superb rate performance and a high specific capacity of 370 mAh g^(-1)(~99% of its theoretical capacity)after 100 cycles at 0.1 C,superior to the commercial graphite anodes.The improved electrochemical performance could be attributed to unchoked Li^(+) transport channels and enhanced charge transfer reaction due to the effective destruction of the degraded SEI and the full recovery of the damaged structure of the spent graphite.This work clarifies that the electrochemical performance of the regenerated graphite could be deteriorated by even a trace amount of the residual“impurity”and provides a facile method for the efficient regeneration of graphite anodes.
基金financial support from the National Natural Science Foundation of China(52203303)the International Partnership Program of the Chinese Academy of Sciences(321GJHZ2023189FN)+2 种基金the Natural Science Foundation of Guangdong Province(2022A1515010076)the Shenzhen Science and Technology Program(SGDX20211123151002003)the Shenzhen International Cooperation Program(GJHZ20220913142812025)。
文摘Graphite interfaces are an important part of the anode in lithium-ion batteries(LIBs),significantly influencing Li intercalation kinetics.Graphite anodes adopt different stacking sequences depending on the concentration of the intercalated Li ions.In this work,we performed first-principles calculations to comprehensively address the energetics and dynamics of Li intercalation and Li vacancy diffusion near the no n-basal edges of graphite,namely the armchair and zigzag-edges,at high Li concentration.We find that surface effects persist in stage-Ⅱ that bind Li strongly at the edge sites.However,the pronounced effect previously identified at the zigzag edge of pristine graphite is reduced in LiC_(12),penetrating only to the subsurface site,and eventually disappearing in LiC_(6).Consequently,the distinctive surface state at the zigzag edge significantly impacts and restrains the charging rate at the initial lithiation of graphite anodes,whilst diminishes with an increasing degree of lithiation.Longer diffusion time for Li hopping to the bulk site from either the zigzag edge or the armchair edge in LiC_(6) was observed during high state of charge due to charge repulsion.Effectively controlling Li occupation and diffusion kinetics at this stage is also crucial for enhancing the charge rate.
基金supported by the China Petrochemical Corporation(222260).
文摘Metallic lithium(Li)is considered the“Holy Grail”anode material for the nextgeneration of Li batteries with high energy density owing to the extraordinary theoretical specific capacity and the lowest negative electrochemical potential.However,owing to inhomogeneous Li-ion flux,Li anodes undergo uncontrollable Li deposition,leading to limited power output and practical applications.Carbon materials and their composites with controllable structures and properties have received extensive attention to guide the homogeneous growth of Li to achieve high-performance Li anodes.In this review,the correlation between the behavior of Li anode and the properties of carbon materials is proposed.Subsequently,we review emerging strategies for rationally designing high-performance Li anodes with carbon materials,including interface engineering(stabilizing solid electrolyte interphase layer and other functionalized interfacial layer)and architecture design of host carbon(constructing three-dimension structure,preparing hollow structure,introducing lithiophilic sites,optimizing geometric effects,and compositing with Li).Based on the insights,some prospects on critical challenges and possible future research directions in this field are concluded.It is anticipated that further innovative works on the fundamental chemistry and theoretical research of Li anodes are needed.
基金supported by the National Natural Science Foundation of China(No.62105277)the Natural Science Foundation of Henan Province(No.232300420139)the Internationalization Training of High-Level Talents of Henan Province,and Nanhu Scholars Program for Young Scholars of XYNU.
文摘Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes the electrode structure instability,leading to poor cyclic stability.What’s worse,the natural Al2O3 layer on commercial Al pellets is always existed as a robust insulating barrier for elec-trons,which brings the voltage dip and results in low reversible capacity.Herein,this work synthesized core-shell Al@C-Sn pellets for LIBs by a plus-minus strategy.In this proposal,the natural Al2O3 passivation layer is eliminated when annealing the pre-introduced SnCl2,meanwhile,polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alle-viate the volume swellings.Benefiting from the addition of C-Sn shell and the elimination of the Al2O3 passivation layer,the as-prepared Al@C-Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g^(-1) at 0.1 A·g^(-1) and 295.0 mAh·g^(-1) at 2.0 A·g^(-1)(after 1000 cycles),respectively.Moreover,its diffusion-controlled capacity is muchly improved compared to those of its counterparts,confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.
文摘Silicon monoxide(SiO)(silicon[Si]mixed with silicon dioxide[SiO_(2)])/graphite(Gr)composite material is one of the most commercially promising anode materials for the next generation of high-energy-density lithium-ion batteries.The major bottleneck for SiO/Gr composite anode is the poor cyclability arising from the stress/strain behaviors due to the mismatch between two heterogenous materials during the lithiation/delithiation process.To date,a meticulous and quantitative understanding of the highly nonlinear coupling behaviors of such materials is still lacking.Herein,an electro–chemo–mechanics-coupled detailed model containing particle geometries is established.The underlying mechanism of the regulation between SiO and Gr components during electrochemical cycling is quantitatively revealed.We discover that increasing the SiO weight percentage(wt%)reduces the utilization efficiency of the active materials at the same 1C rate charging and enhances the hindering effects of stress-driven flux on diffusion.In addition,the mechanical constraint demonstrates a balanced effect on the overall performance of cells and the local behaviors of particles.This study provides new insights into the fundamental interactions between SiO and Gr materials and advances the investigation methodology for the design and evaluation of next-generation high-energydensity batteries.
基金financially supported by the National Key Research and Development Program of China(2022YFB3803600)the Fundamental Research Funds for the Central Universities(30106200463 and CCNU22CJ017)+1 种基金the National Natural Science Foundation of China(U20A20246)the Graduate Education Innovation Grant from Central China Normal University,China(20210407032)。
文摘Zincophilic property and high electrical conductivity are both very important parameters to design novel Zn anode for aqueous Zn-ion batteries(AZIBs).However,single material is difficult to exhibit zincophilic property and high electrical conductivity at the same time.Herein,originating from theoretical calculation,a zincophilic particle regulation strategy is proposed to address these limitations and carbon coated Na_(3)V_(2)(PO_(4))_(3)is taken as an example to be a protective layer on zinc metal(NVPC@Zn).Na_(3)V_(2)(PO_(4))_(3)(NVP)is a common cathode material for Zn-ion batteries,which is zincophilic.Carbon materials not only offer an electron pathway to help Zn deposition onto NVPC surface,but also enhance the zinc nucleophilicity of Na_(3)V_(2)(PO_(4))_(3).Hence,this hybrid coating layer can tune zinc deposition and resist side reactions such as hydrogen generation and Zn metal corrosion.Experimentally,a symmetrical battery with NVPC@Zn electrode displays highly reversible plating/stripping behavior with a long cycle lifespan over 1800 h at2 mA cm^(-2),much better than carbon and Na_(3)V_(2)(PO_(4))_(3)solely modified Zn electrodes.When the Na_(3)V_(2)(PO_(4))_(3)is replaced with zincophobic Al2O3or zincophilic V2O3,the stability of the modified zinc anodes is also prolonged.This strategy expands the option of zincophilic materials and provides a general and effective way to stabilize the Zn electrode.