The low yield of MXene is normally related to the delaminating step,contributing to the key technical challenges in moving toward industrial applications.Here,a shearing-force-driven strategy is proposed for re-exfoli...The low yield of MXene is normally related to the delaminating step,contributing to the key technical challenges in moving toward industrial applications.Here,a shearing-force-driven strategy is proposed for re-exfoliating waste MXene residue to prepare oxidatively stable MXene composites in a low-cost manner,where the strong shear stress in the assisted solvent,such as carbon nanotubes(CNTs),chitosan(CS),and polyacrylamide(PAM)aqueous solutions,acts on the surface of MXene(Ti_(3)C_(2)T_(x))through coordination between hydroxyl and Ti atoms,resulting in a rapid and efficient exfoliation of waste Ti_(3)C_(2)T_(x)residue under stirring.Furthermore,this formed coordinate bond helps to stabilize the low-valent Ti atoms on the surface of MXene,thereby enhancing the oxidative stability of Ti_(3)C_(2)T_(x).Besides,the CNT@MXene composite is selected to construct a free-standing membrane to encapsulate Si nanoparticles,achieving a high and reversible capacity after 50 cycles.This work supports the concept of valorizing waste and adopts a fluid shear forceassisted method to re-exfoliate waste residues,which greatly reduces the cost of processing and improves the chemical stability of MXene.More importantly,this work has uncovered a new direction for the commercialization of MXene composites and has significantly improved the realworld applications of MXene-based materials.展开更多
Silicon(Si)is considered as one of the most promising anode materials for advanced lithium-ion batteries due to its high theoretical capacity,environmental friendliness,and widespread availability.However,great challe...Silicon(Si)is considered as one of the most promising anode materials for advanced lithium-ion batteries due to its high theoretical capacity,environmental friendliness,and widespread availability.However,great challenges such as volumetric expansion,limited ionic/electronic conductivity properties and complex manufacturing processes hinder its practical applications.Herein,a novel plasma-enhanced reduced graphene oxide fibers/Si(PrGOFs/Si)composite anode is first proposed by using wet-spinning technology followed by plasma-enhanced reduction method.The PrGOFs provide large space to accommodate the volume expansion of Si nanoparticles(SiNPs)by forming a flexible 3D conductive network.Compared to the conventional thermally reduced graphene oxide fibers/Si(TrGOFs/Si)sample,the PrGOFs/Si anodes demonstrate higher conductivity,specific surface area,and superior fabrication efficiency.Accordingly,the Pr GOFs/Si anodes exhibit a reversible capacity of 698.3 mA h/g,and maintain a specific capacity of 602.5m Ah/g at a current density of 200 m A/g after 100 cycles,superior to conventional Tr GOFs/Si counterparts.This research presents a novel strategy for the preparation of high-performance Si/carbon anodes for energy storage applications.展开更多
A commentary on pressure-induced pre-lithiation towards Si anodes in allsolid-state Li-ion batteries(ASSLIBs)using sulfide electrolytes(SEs)is presented.First,feasible pre-lithiation technologies for Si anodes in SE-b...A commentary on pressure-induced pre-lithiation towards Si anodes in allsolid-state Li-ion batteries(ASSLIBs)using sulfide electrolytes(SEs)is presented.First,feasible pre-lithiation technologies for Si anodes in SE-based ASSLIBs especially the significant pressure-induced pre-lithiation strategies are briefly reviewed.Then,a recent achievement by Meng et al.in this field is elaborated in detail.Finally,the significance of Meng’s work is discussed.展开更多
Micron-sized silicon(μSi)is a promising anode material for next-generation lithium-ion batteries due to its high specific capacity,low cost,and abundant reserves.However,the volume expansion that occurs during cyclin...Micron-sized silicon(μSi)is a promising anode material for next-generation lithium-ion batteries due to its high specific capacity,low cost,and abundant reserves.However,the volume expansion that occurs during cycling leads to the accumulation of undesirable stresses,resulting in pulverization of silicon microparticles and shortened lifespan of the batteries.Herein,a composite film of Cu-PET-Cu is proposed as the current collector(CC)forμSi anodes to replace the conventional Cu CC.Cu-PET-Cu CC is prepared by depositing Cu on both sides of a polyethylene terephthalate(PET)film.The PET layer promises good ductility of the film,permitting the Cu-PET-Cu CC to accommodate the volumetric changes of silicon microparticles and facilitates the stress release through ductile deformation.As a result,theμSi electrode with Cu-PET-Cu CC retains a high specific capacity of 2181 mA h g^(-1),whereas theμSi electrode with Cu CC(μSi/Cu)exhibits a specific capacity of 1285 mA h g^(-1)after 80 cycles.The stress relieving effect of CuPET-Cu was demonstrated by in-situ fiber optic stress monitoring and multi-physics simulations.This work proposes an effective stress relief strategy at the electrode level for the practical implementation ofμSi anodes.展开更多
Silicon(Si)is a promising anode material for rechargeable batteries due to its high theoretical capacity and abundance,but its practical application is hindered by the continuous growth of porous solid-electrolyte int...Silicon(Si)is a promising anode material for rechargeable batteries due to its high theoretical capacity and abundance,but its practical application is hindered by the continuous growth of porous solid-electrolyte interphase(SEI),leading to capacity fade.Herein,a LiF-Pie structured SEI is proposed,with LiF nanodomains encapsulated in the inner layer of the organic cross-linking silane matrix.A series of advanced techniques such as cryogenic electron microscopy,time-of-flight secondary ion mass spectrometry,and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry have provided detailed insights into the formation mechanism,nanostructure,and chemical composition of the interface.With such SEI,the capacity retention of LiCoO_(2)||Si is significantly improved from 49.6%to 88.9%after 300 cycles at 100 mA g^(-1).These findings provide a desirable interfacial design principle with enhanced(electro)chemical and mechanical stability,which are crucial for sustaining Si anode functionality,thereby significantly advancing the reliability and practical application of Si-based anodes.展开更多
Solid-state lithium-ion batteries(SSLIBs) offer significant advantages over traditional liquid-electrolytebased batteries,including improved safety,higher energy density,and better thermal stability.Among various anod...Solid-state lithium-ion batteries(SSLIBs) offer significant advantages over traditional liquid-electrolytebased batteries,including improved safety,higher energy density,and better thermal stability.Among various anode materials,silicon(Si)-based anodes have attracted significant attention due to their ultrahigh theoretical capacity(~4200 mAh/g) and abundant resources.However,widespread adoption of Si-based anodes in SSLIBs is still restricted by some critical challenges such as severe volume expansion,low electronic and ionic conductivity,high interfacial impedance,and low initial Coulombic efficiency(ICE).This review mainly focuses on the design strategies of Si-based anode for SSLIBs at the material,electrode and cell levels including nanostructuring,Si alloys,Si-carbon composites,conductive additives,advanced binder,external pressure,electrolyte infiltration,and prelithiation.The insights provided here aim to inspire future research and accelerate commercialization of high-performance Si-based anodes in next-generation SSLIBs.展开更多
While silicon/carbon(Si/C)is considered one of the most promising anode materials for the next generation of high-energy lithium-ion batteries(LIBs),the industrialization of Si/C anodes is hampered by high-cost and lo...While silicon/carbon(Si/C)is considered one of the most promising anode materials for the next generation of high-energy lithium-ion batteries(LIBs),the industrialization of Si/C anodes is hampered by high-cost and low product yield.Herein,a high-yield strategy is developed in which photovoltaic waste silicon is converted to cost-effective graphitic Si/C composites(G-Si@C)for LIBs.The introduction of a binder improves the dispersion and compatibility of silicon and graphite,enhances particle sphericity,and significantly reduces the loss rate of the spray prilling process(from about 25%to 5%).As an LIB anode,the fabricated G-Si@C composites exhibit a capacity of 605 mAh g^(-1) after 1200 cycles.The cost of manufacturing Si/C anode materials has been reduced to approximately$7.47 kg^(-1),which is close to that of commercial graphite anode materials($5.0 kg^(-1)),and significantly lower than commercial Si/C materials(ca.$20.74 kg^(-1)).Moreover,the G-Si@C material provides approximately 81.0 Ah/$of capacity,which exceeds the current best commercial graphite anodes(70.0 Ah/$)and Si/C anodes(48.2 Ah/$).The successful implementation of this pathway will significantly promote the industrialization of high-energydensity Si/C anode materials.展开更多
The ever-increasing environmental/energy crisis as well as the rapid upgrading of mobile devices had stimulated intensive research attention on promising alternative energy storage and conversion devices.Among these d...The ever-increasing environmental/energy crisis as well as the rapid upgrading of mobile devices had stimulated intensive research attention on promising alternative energy storage and conversion devices.Among these devices,alkali metal ion batteries,such as lithium-ion batteries(LIBs) had attracted increasing research attention due to its several advantages including,environmental friendliness,high power density,long cycle life and excellent reversibility.It had been widely used in consumer electronics,electric vehicles,and large power grids et ac.Silicon-based(silicon and their oxides,carbides) anodes had been widely studied.Its several advantages including low cost,high theoretical capacity,natural abundance,and environmental friendliness,which shows great potential as anodes of LIBs.In this review,we summarized the recently progress in the synthetic method of silicon matrix composites.The empirical method for prelithiation of silicon-based materials were also provided.Further,we also reviewed some novel characterization methods.Finally,the new design,preparation methods and properties of these nano materials were reviewed and compared.We hoped that this review can provide a general overview of recent progress and we briefly highlighted the current challenges and prospects,and will clarify the future trend of silicon anode LIBs research.展开更多
Silicon(Si)is a promising anode material for lithium‐ion batteries(LIBs)owing to its tremendously high theoretical storage capacity(4200 mAh g−1),which has the potential to elevate the energy of LIBs.However,Si anode...Silicon(Si)is a promising anode material for lithium‐ion batteries(LIBs)owing to its tremendously high theoretical storage capacity(4200 mAh g−1),which has the potential to elevate the energy of LIBs.However,Si anodes exhibit severe volume change during lithiation/delithiation processes,resulting in anode pulverization and delamination with detrimental growth of solid electrolyte interface layers.As a result,the cycling stability of Si anodes is insufficient for commercialization in LIBs.Polymeric binders can play critical roles in Si anodes by affecting their cycling stability,although they occupy a small portion of the electrodes.This review introduces crucial factors influencing polymeric binders'properties and the electrochemical performance of Si anodes.In particular,we emphasize the structure–property relationships of binders in the context of molecular design strategy,functional groups,types of interactions,and functionalities of binders.Furthermore,binders with additional functionalities,such as electrical conductivity and self‐healability,are extensively discussed,with an emphasis on the binder design principle.展开更多
To mitigate the massive volume expansion of Si-based anode during the charge/discharge cycles,we synthesized a superstructure of Si@Co±NC composite via the carbonization of zeolite imidazolate frameworks incorpor...To mitigate the massive volume expansion of Si-based anode during the charge/discharge cycles,we synthesized a superstructure of Si@Co±NC composite via the carbonization of zeolite imidazolate frameworks incorporated with Si nanoparticles.The Si@Co±NC is comprised of Sinanoparticle core and N-doped/Co-incorporated carbon shell,and there is void space between the core and the shell.When using as anode material for LIBs,Si@Co±NC displayed a super performance with a charge/discharge capacity of 191.6/191.4 mA h g^(-1)and a coulombic efficiency of 100.1%at 1000 mA g^(-1)after 3000 cycles,and the capacity loss rate is 0.022%per cycle only.The excellent electrochemical property of Si@Co±NC is because its electronic conductivity is enhanced by doping the carbon shell with N atoms and by incorporating with Co particles,and the pathway of lithium ions transmission is shortened by the hollow structure and abundant mesopores in the carbon shell.Also,the volume expansion of Si nanoparticles is well accommodated in the void space and suppressed by the carbon host matrix.This work shows that,through designing a superstructure for the anode materials,we can synergistically reduce the work function and introduce the confinement effect,thus significantly enhancing the anode materials’electrochemical performance in LIBs.展开更多
The commercialized binder carboxymethyl cellulose sodium(CMC-Na)is considered unsuitable for micro-sized SiO_(x) anode as it cannot endure the large volume change to retain the conductive network during repeated charg...The commercialized binder carboxymethyl cellulose sodium(CMC-Na)is considered unsuitable for micro-sized SiO_(x) anode as it cannot endure the large volume change to retain the conductive network during repeated charge/discharge cycles.Herein,a small amount of silicon nanoparticles(SiNPs)is added during slurry preparation process as“nano-combs”to unfold the convoluted CMC-Na polymer chains so that they undergo a coilto-stretch transition by interaction between polar groups(e.g.,-OH,-COONa)of polymer and SiNPs’large surface.Through maximizing the utilization of binders,a uniform conductive network is constructed with increased interfacial contact with micro-sized SiO_(x).As a result,the SiO_(x) electrode with optimized(10 wt%)SiNPs addition shows significantly improved initial capacity and cycling performance.Through revisiting CMCNa,a currently deemed unqualified binder in SiO_(x) anode,this work gives a brand-new perspective on the failing mechanism of Si-based anode materials and an improving strategy for electrode preparation.展开更多
Silicon(Si)holds promise as an anode material for lithium-ion batteries(LIBs)as it is widely avail-able and characterized by high specific capacity and suitable working potential.However,the relatively low electrical ...Silicon(Si)holds promise as an anode material for lithium-ion batteries(LIBs)as it is widely avail-able and characterized by high specific capacity and suitable working potential.However,the relatively low electrical conductivity of Si and the significantly high extent of volume expansion realized dur-ing lithiation hinder its practical application.We prepared N-doped carbon polyhedral micro cage en-capsulated Si nanoparticles derived from Co-Mo bimetal metal-organic framework(MOFs)(denoted as Si/CoMo@NCP)and explored their lithium storage performance as anode materials to address these prob-lems.The Si/CoMo@NCP anode exhibited a high reversible lithium storage capacity(1013 mAh g^(−1)at 0.5 A g^(−1)after 100 cycles),stable cycle performance(745 mAh g^(−1)at 1 A g^(−1)after 400 cycles),and excellent rate performance(723 mAh g^(−1)at 2 A g^(−1)).Also,the constructed the full-cell NCM 811//Si/CoMo@NCP exhibited well reversible capacity.The excellent electrochemical performances of Si/CoMo@NCP were at-tributed to two unique properties.The encapsulation of NCP with doped nitrogen and porous structural carbon improves the electrical conductivity and cycling stability of the molecules.The introductions of metallic cobalt and its oxides help to improve the rate capability and lithiation capacity of the materials following multi-electron reaction mechanisms.展开更多
Si anode is of paramount importance for advanced energy-dense lithium-ion batteries(LIBs).However,the large volume change as well as stress generates during its lithiation-delithiation process poses a great challenge ...Si anode is of paramount importance for advanced energy-dense lithium-ion batteries(LIBs).However,the large volume change as well as stress generates during its lithiation-delithiation process poses a great challenge to the long-term cycling and hindering its application.Herein this work,a composite binder is prepared with a soft component,guar gum(GG),and a rigid linear polymer,anionic polyacrylamide(APAM).Rich hydroxy,carboxyl,and amide groups on the polymer chains not only enable intermolecular crosslinking to form a web-like binder,A2G1,but also realize strong chemical binding as well as physical encapsulating to Si particles.The resultant electrode shows limited thickness change of merely 9%on lithiation and almost recovers its original thickness on delithiation.It demonstrates high reversible capacity of 2104.3 mAh g^(-1)after 100 cycles at a current density of 1800 mA g^(-1),and in constant capacity(1000 mAh g^(-1))test,it also shows a long life of 392 cycles.Therefore,this soft-hard combining web-like binder illustrates its great potential in the future applications.展开更多
Silicon is recognized as the most advantageous next-generation anode material for LIBs in terms of its extremely high theoretical capacity and appropriate operating voltage.However,the application of Si anode is limit...Silicon is recognized as the most advantageous next-generation anode material for LIBs in terms of its extremely high theoretical capacity and appropriate operating voltage.However,the application of Si anode is limited by huge volume expansion emerging with cycling,which in turn induces the collapse of the electrode structure,resulting in rapid capacity decay.Here,we report a strategy using self-swelling artificial laponite to prepare a laponite/MXene/CNT composite framework with both rigidity and flexibility,which can excellently address these challenges of Si anode.The self-swelling artificial laponite participates in the construction of hierarchical and porous structures,providing sufficient buffer space to mitigate the volume expansion of the LixSi alloying reaction.Meanwhile,tough and tightly cross-linked silicate nanosheets can improve the mechanical strength of the framework for strong structural stability.More importantly,the negative charge between the layers of artificial laponite can effectively promote fast Li-ion transport in the electrode.This free-standing silicon anode enables the preparation of high areal capacity electrodes to further enhance the energy density of LIBs and a higher reversible capacity of 2381.8 mAh/g at 0.1 C after 50 cycles with an initial coulombic of 85.6%.This work provides a simple and practical fabrication strategy for developing high-performance Si-based batteries,which can speed up their commercialization.展开更多
Replacing the conventional carbonate electrolyte by solid-state electrolyte (SSE) will offer improved safety for lithium-ion batteries.To further improve the energy density,Silicon (Si) is attractive for next generati...Replacing the conventional carbonate electrolyte by solid-state electrolyte (SSE) will offer improved safety for lithium-ion batteries.To further improve the energy density,Silicon (Si) is attractive for next generation solid-state battery (SSB) because of its high specific capacity and low cost.High energy density and safe Si-based SSB,however,is plagued by large volume change that leads to poor mechanical stability and slow lithium ions transportation at the multiple interfaces between Si and SSE.Herein,we designed a self-integrated and monolithic Si/two dimensional layered T_(3)C_(2)T_(x)(MXene,T_(x) stands for terminal functional groups) electrode architecture with interfacial nitrogen engineering.During a heat treatment process,the polyacrylonitrile not only converts into amorphous carbon (a-C) that shells Si but also forms robust interfacial nitrogen chemical bonds that anchors Si and MXene.During repeated lithiation and delithiation processes,the robust interfacial engineered Si/MXene configuration enhances the mechanical adhesion between Si and MXene that improves the structure stability but also contributes to form stable solid-electrolyte interphase (SEI).In addition,the N-MXene provides fast lithium ions transportation pathways.Consequently,the Si/MXene with interfacial nitrogen engineering (denoted as Si-N-MXene) deliveres high-rate performance with a specific capacity of 1498 m Ah g^(-1) at a high current of 6.4 A g^(-1).A Si-N-MXene/NMC full cell exhibited a capacity retention of 80.5%after 200 cycles.The Si-N-MXene electrode is also applied to SSB and shows a relative stable cycling over 100 cycles,demonstrating the versatility of this concept.展开更多
Silicon nanowires(Si NWs)have been widely researched as the best alternative to graphite anodes for the next-generation of high-performance lithium-ion batteries(LIBs)owing to their high capacity and low discharge pot...Silicon nanowires(Si NWs)have been widely researched as the best alternative to graphite anodes for the next-generation of high-performance lithium-ion batteries(LIBs)owing to their high capacity and low discharge potential.However,growing binder-free Si NW anodes with adequate mass loading and stable capacity is severely limited by the low surface area of planar current collectors(CCs),and is particularly challenging to achieve on standard pure-Cu substrates due to the ubiquitous formation of Li+inactive silicide phases.Here,the growth of densely-interwoven In-seeded Si NWs is facilitated by a thin-film of copper-silicide(CS)network in situ grown on a Cu-foil,allowing for a thin active NW layer(<10μm thick)and high areal loading(≈1.04 mg/cm^(2))binder-free electrode architecture.The electrode exhibits an average Coulombic efficiency(CE)of>99.6%and stable performance for>900 cycles with≈88.7%capacity retention.More significantly,it delivers a volumetric capacity of≈1086.1 m A h/cm^(3)at 5C.The full-cell versus lithium manganese oxide(LMO)cathode delivers a capacity of≈1177.1 m A h/g at 1C with a stable rate capability.This electrode architecture represents significant advances toward the development of binder-free Si NW electrodes for LIB application.展开更多
Inspired by the natural corn structure,a Si@hollow graphene shell@graphene(Si@GS@G)anode material was prepared in which silicon nanoparticles were preliminarily anchored onto the surface of an elastic graphene shell a...Inspired by the natural corn structure,a Si@hollow graphene shell@graphene(Si@GS@G)anode material was prepared in which silicon nanoparticles were preliminarily anchored onto the surface of an elastic graphene shell and further constrained using graphene sheets.Hollow graphene oxide shells with abundant surficial hydrogen bonds,which were synthesized using a novel bottom-up method,were used as an intermediate material to anchor positively charged silicon nanoparticles via electrostatic attraction and achieve a rational spatial distribution.The inner hollow graphene shell anchorage and outer graphene constraint synergistically constituted a porous and robust conductive corn-like structure.The as-fabricated Si@GS@G anode afforded efficient electron and ion transport pathways and improved structural stability,thereby enhancing Li+storage capability(505 mAh·g^(−1)at 10 A·g^(−1))and extending the lifespan compared to the single hollow graphene shell or graphene sheet-protected Si anode(72%capacity retention after 500 cycles).The improved kinetics of the Si@GS@G anode were investigated using electro impedance spectroscopy,galvanostatic intermittent titration,and pseudocapacitance contribution rate analysis,and the structural evolution was analyzed using ex situ electron microscopy.This study proposes a novel hollow graphene oxide shell as an activated intermediate material for designing a porous electrode structure that facilitates an enhanced electrochemical performance.展开更多
Silicon is being investigated extensively as an anodic material for next-generation lithium ion batteries for portable energy storage and electric vehicles.However,the large changes in volume during cycling lead to th...Silicon is being investigated extensively as an anodic material for next-generation lithium ion batteries for portable energy storage and electric vehicles.However,the large changes in volume during cycling lead to the breakdown of the conductive network in Si anodes and the formation of an unstable solid-electrolyte interface,resulting in capacity fading.Here,we demonstrate nanoparticles with a Si@Mn22.6Si5.4C4@C double-shell structure and the formation of self-organized Si-Mn-C nanocomposite anodes during the lithiation/delithiation process.The anode consists of amorphous Si particles less than 10 nm in diameter and separated by an interconnected conductive/buffer network,which exhibits excellent charge transfer kinetics and charge/discharge performances.A stable specific capacity of 1100 mAh·g-1 at 100 mA·g-1 and a coulombic efficiency of 99.2%after 30 cycles are achieved.Additionally,a rate capacity of 343 mAh·g-1 and a coulombic efficiency of 99.4%at 12000 mA·g-1 are also attainable.Owing to its simplicity and applicability,this strategy for improving electrode performance paves a way for the development of high-performance Si-based anodic materials for lithium ion batteries.展开更多
Silicon anodes are promising for high-energy-density lithium-ion batteries.Nevertheless,unsatisfied initial Coulombic efficiency(ICE)and structure collapse are two barriers still hindering their application.Here,we re...Silicon anodes are promising for high-energy-density lithium-ion batteries.Nevertheless,unsatisfied initial Coulombic efficiency(ICE)and structure collapse are two barriers still hindering their application.Here,we report a 5 at.%-vanadium hybriding strategy to stabilize Si film anode,which delivers a high initial Coulombic efficiency of 92.1%with a discharge capacity of 2434.9 mAh·g^(−1) and a desirable capacity retention of 80%after 100 cycles at 1 A·g^(−1).Physical and electrochemical analyses demonstrate the Li_(x)PO_(y)F_(z)-rich inorganic solid-electrolyte interphase(SEI)and the low film internal strain are two advantageous factors for the desirable Li-ion storage reversibility and stability.A full battery with a LiFePO_(4) cathode delivers the energy densities of 291.9 and 194.6 Wh·kg^(−1) under power densities of 145.9 and 389.2 W·kg^(−1),respectively.This result on Si anodes may pave the way to next-generation highenergy-density lithium-ion batteries.展开更多
The application of Si as the anode materials for lithium-ion batteries(LIBs) is still severely hindered by the rapid capacity decay due to the structural damage caused by large volume change(> 300%) during cycling....The application of Si as the anode materials for lithium-ion batteries(LIBs) is still severely hindered by the rapid capacity decay due to the structural damage caused by large volume change(> 300%) during cycling. Herein, a three-dimensional(3 D) aerogel anode of Si@carbon@graphene(SCG) is rationally constructed via a polydopamine-assisted strategy. Polydopamine is coated on Si nanoparticles to serve as an interface linker to initiate the assembly of Si and graphene oxide, which plays a crucial role in the successful fabrication of SCG aerogels. After annealing the polydopamine is converted into N-doped carbon(N-carbon) coatings to protect Si materials. The dual protection from N-carbon and graphene aerogels synergistically improves the structural stability and electronic conductivity of Si, thereby leading to the significantly improved lithium storage properties. Electrochemical tests show that the SCG with optimized graphene content delivers a high capacity(712 m Ah/g at 100 m A/g) and robust cycling stability(402 m Ah/g at 1 A/g after 1500 cycles). Furthermore, the full cell using SCG aerogels as anode exhibits a reversible capacity of 187.6 m Ah/g after 80 cycles at 0.1 A/g. This work provides a plausible strategy for developing Si anode in LIBs.展开更多
基金financially supported by the National Natural Science Foundation of China(No.52102470)the Natural Science Foundation of Jiangsu Province(No.BK20200047)+1 种基金General Project of Natural Science Research in Jiangsu Universities(22KJB15003)Scientific Research Project for Doctor Degree Teachers of Jiangsu Normal University(21XSRX003)。
文摘The low yield of MXene is normally related to the delaminating step,contributing to the key technical challenges in moving toward industrial applications.Here,a shearing-force-driven strategy is proposed for re-exfoliating waste MXene residue to prepare oxidatively stable MXene composites in a low-cost manner,where the strong shear stress in the assisted solvent,such as carbon nanotubes(CNTs),chitosan(CS),and polyacrylamide(PAM)aqueous solutions,acts on the surface of MXene(Ti_(3)C_(2)T_(x))through coordination between hydroxyl and Ti atoms,resulting in a rapid and efficient exfoliation of waste Ti_(3)C_(2)T_(x)residue under stirring.Furthermore,this formed coordinate bond helps to stabilize the low-valent Ti atoms on the surface of MXene,thereby enhancing the oxidative stability of Ti_(3)C_(2)T_(x).Besides,the CNT@MXene composite is selected to construct a free-standing membrane to encapsulate Si nanoparticles,achieving a high and reversible capacity after 50 cycles.This work supports the concept of valorizing waste and adopts a fluid shear forceassisted method to re-exfoliate waste residues,which greatly reduces the cost of processing and improves the chemical stability of MXene.More importantly,this work has uncovered a new direction for the commercialization of MXene composites and has significantly improved the realworld applications of MXene-based materials.
基金supported by Natural Science Foundation for Distinguished Young Scholars of Zhejiang Province(No.LR20E020001)National Natural Science Foundation of China(Nos.52372235,52073252,22379020,52002052,U20A20253,21972127,22279116)+3 种基金Science and Technology Department of Zhejiang Province(Nos.2023C01231,Q23E020046,LD22E020006,and LY21E020005)Key Research and Development Project of Science and Technology Department of Sichuan Province(No.2022YFSY0004)Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology),Ministry of Education(No.KFM 202202)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEEKF202206),Fuzhou University。
文摘Silicon(Si)is considered as one of the most promising anode materials for advanced lithium-ion batteries due to its high theoretical capacity,environmental friendliness,and widespread availability.However,great challenges such as volumetric expansion,limited ionic/electronic conductivity properties and complex manufacturing processes hinder its practical applications.Herein,a novel plasma-enhanced reduced graphene oxide fibers/Si(PrGOFs/Si)composite anode is first proposed by using wet-spinning technology followed by plasma-enhanced reduction method.The PrGOFs provide large space to accommodate the volume expansion of Si nanoparticles(SiNPs)by forming a flexible 3D conductive network.Compared to the conventional thermally reduced graphene oxide fibers/Si(TrGOFs/Si)sample,the PrGOFs/Si anodes demonstrate higher conductivity,specific surface area,and superior fabrication efficiency.Accordingly,the Pr GOFs/Si anodes exhibit a reversible capacity of 698.3 mA h/g,and maintain a specific capacity of 602.5m Ah/g at a current density of 200 m A/g after 100 cycles,superior to conventional Tr GOFs/Si counterparts.This research presents a novel strategy for the preparation of high-performance Si/carbon anodes for energy storage applications.
基金supported by grants from the National Natural Science Foundation of China(Grant Nos.52072136,52272201,52172229,51972257)Yanchang Petroleum-WHUT Joint Program(yc-whlg-2022ky-05)Fundamental Research Funds for the Central Universities(104972024RSCrc0006)for financial support.
文摘A commentary on pressure-induced pre-lithiation towards Si anodes in allsolid-state Li-ion batteries(ASSLIBs)using sulfide electrolytes(SEs)is presented.First,feasible pre-lithiation technologies for Si anodes in SE-based ASSLIBs especially the significant pressure-induced pre-lithiation strategies are briefly reviewed.Then,a recent achievement by Meng et al.in this field is elaborated in detail.Finally,the significance of Meng’s work is discussed.
基金supported by the the National Key R&D Program of China(2022YFB3803500)the Natural Science Foundation of Hubei Province(2021CFA066).
文摘Micron-sized silicon(μSi)is a promising anode material for next-generation lithium-ion batteries due to its high specific capacity,low cost,and abundant reserves.However,the volume expansion that occurs during cycling leads to the accumulation of undesirable stresses,resulting in pulverization of silicon microparticles and shortened lifespan of the batteries.Herein,a composite film of Cu-PET-Cu is proposed as the current collector(CC)forμSi anodes to replace the conventional Cu CC.Cu-PET-Cu CC is prepared by depositing Cu on both sides of a polyethylene terephthalate(PET)film.The PET layer promises good ductility of the film,permitting the Cu-PET-Cu CC to accommodate the volumetric changes of silicon microparticles and facilitates the stress release through ductile deformation.As a result,theμSi electrode with Cu-PET-Cu CC retains a high specific capacity of 2181 mA h g^(-1),whereas theμSi electrode with Cu CC(μSi/Cu)exhibits a specific capacity of 1285 mA h g^(-1)after 80 cycles.The stress relieving effect of CuPET-Cu was demonstrated by in-situ fiber optic stress monitoring and multi-physics simulations.This work proposes an effective stress relief strategy at the electrode level for the practical implementation ofμSi anodes.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFB2502200)the National Natural Science Foundation of China(NSFC nos.52172257 and 22409211)+2 种基金the China Postdoctoral Science Foundation(No.2023M743739)the Postdoctoral Fellowship Program of CPSF(No.GZC20232939)CAS Youth Interdisciplinary Team。
文摘Silicon(Si)is a promising anode material for rechargeable batteries due to its high theoretical capacity and abundance,but its practical application is hindered by the continuous growth of porous solid-electrolyte interphase(SEI),leading to capacity fade.Herein,a LiF-Pie structured SEI is proposed,with LiF nanodomains encapsulated in the inner layer of the organic cross-linking silane matrix.A series of advanced techniques such as cryogenic electron microscopy,time-of-flight secondary ion mass spectrometry,and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry have provided detailed insights into the formation mechanism,nanostructure,and chemical composition of the interface.With such SEI,the capacity retention of LiCoO_(2)||Si is significantly improved from 49.6%to 88.9%after 300 cycles at 100 mA g^(-1).These findings provide a desirable interfacial design principle with enhanced(electro)chemical and mechanical stability,which are crucial for sustaining Si anode functionality,thereby significantly advancing the reliability and practical application of Si-based anodes.
基金financially supported by the National Natural Science Foundation of China(Nos.22366032,52072119)Hunan Intelligent Rehabilitation Robot and Auxiliary Equipment Engineering Technology Research Center(No.2025SH301)。
文摘Solid-state lithium-ion batteries(SSLIBs) offer significant advantages over traditional liquid-electrolytebased batteries,including improved safety,higher energy density,and better thermal stability.Among various anode materials,silicon(Si)-based anodes have attracted significant attention due to their ultrahigh theoretical capacity(~4200 mAh/g) and abundant resources.However,widespread adoption of Si-based anodes in SSLIBs is still restricted by some critical challenges such as severe volume expansion,low electronic and ionic conductivity,high interfacial impedance,and low initial Coulombic efficiency(ICE).This review mainly focuses on the design strategies of Si-based anode for SSLIBs at the material,electrode and cell levels including nanostructuring,Si alloys,Si-carbon composites,conductive additives,advanced binder,external pressure,electrolyte infiltration,and prelithiation.The insights provided here aim to inspire future research and accelerate commercialization of high-performance Si-based anodes in next-generation SSLIBs.
基金supported by the Major Science and Technology Projects in Yunnan Province(Grant No.202402AF080005)National Natural Science Foundation of China(Grant Nos.52274408,22468029,52274412)+2 种基金Yunnan Fundamental Research Projects(Grant No.202201AW070014)the Program for Innovative Research Team in University of Ministry of Education of China(Grant No.IRT 17R48)the German Research Foundation(DFG,Project number 501766751).
文摘While silicon/carbon(Si/C)is considered one of the most promising anode materials for the next generation of high-energy lithium-ion batteries(LIBs),the industrialization of Si/C anodes is hampered by high-cost and low product yield.Herein,a high-yield strategy is developed in which photovoltaic waste silicon is converted to cost-effective graphitic Si/C composites(G-Si@C)for LIBs.The introduction of a binder improves the dispersion and compatibility of silicon and graphite,enhances particle sphericity,and significantly reduces the loss rate of the spray prilling process(from about 25%to 5%).As an LIB anode,the fabricated G-Si@C composites exhibit a capacity of 605 mAh g^(-1) after 1200 cycles.The cost of manufacturing Si/C anode materials has been reduced to approximately$7.47 kg^(-1),which is close to that of commercial graphite anode materials($5.0 kg^(-1)),and significantly lower than commercial Si/C materials(ca.$20.74 kg^(-1)).Moreover,the G-Si@C material provides approximately 81.0 Ah/$of capacity,which exceeds the current best commercial graphite anodes(70.0 Ah/$)and Si/C anodes(48.2 Ah/$).The successful implementation of this pathway will significantly promote the industrialization of high-energydensity Si/C anode materials.
基金financially supported by the International Science & Technology Cooperation Program of China under 2019YFE0100200the NSAF (Grant No. U1930113)+2 种基金the Beijing Natural Science Foundation (Grant No. L182022)the 13th Five-Year Plan of Advance Research and Sharing Techniques by the Equipment Department (41421040202)the SAST (2018-114).
文摘The ever-increasing environmental/energy crisis as well as the rapid upgrading of mobile devices had stimulated intensive research attention on promising alternative energy storage and conversion devices.Among these devices,alkali metal ion batteries,such as lithium-ion batteries(LIBs) had attracted increasing research attention due to its several advantages including,environmental friendliness,high power density,long cycle life and excellent reversibility.It had been widely used in consumer electronics,electric vehicles,and large power grids et ac.Silicon-based(silicon and their oxides,carbides) anodes had been widely studied.Its several advantages including low cost,high theoretical capacity,natural abundance,and environmental friendliness,which shows great potential as anodes of LIBs.In this review,we summarized the recently progress in the synthetic method of silicon matrix composites.The empirical method for prelithiation of silicon-based materials were also provided.Further,we also reviewed some novel characterization methods.Finally,the new design,preparation methods and properties of these nano materials were reviewed and compared.We hoped that this review can provide a general overview of recent progress and we briefly highlighted the current challenges and prospects,and will clarify the future trend of silicon anode LIBs research.
基金National Research Foundation,Grant/Award Number:2022R1A2C1092273。
文摘Silicon(Si)is a promising anode material for lithium‐ion batteries(LIBs)owing to its tremendously high theoretical storage capacity(4200 mAh g−1),which has the potential to elevate the energy of LIBs.However,Si anodes exhibit severe volume change during lithiation/delithiation processes,resulting in anode pulverization and delamination with detrimental growth of solid electrolyte interface layers.As a result,the cycling stability of Si anodes is insufficient for commercialization in LIBs.Polymeric binders can play critical roles in Si anodes by affecting their cycling stability,although they occupy a small portion of the electrodes.This review introduces crucial factors influencing polymeric binders'properties and the electrochemical performance of Si anodes.In particular,we emphasize the structure–property relationships of binders in the context of molecular design strategy,functional groups,types of interactions,and functionalities of binders.Furthermore,binders with additional functionalities,such as electrical conductivity and self‐healability,are extensively discussed,with an emphasis on the binder design principle.
基金financial supports by the National Natural Science Foundation of China(No.51772295)support of GTIIT for the collaboration,and the start-up fund provided by GTIIT
文摘To mitigate the massive volume expansion of Si-based anode during the charge/discharge cycles,we synthesized a superstructure of Si@Co±NC composite via the carbonization of zeolite imidazolate frameworks incorporated with Si nanoparticles.The Si@Co±NC is comprised of Sinanoparticle core and N-doped/Co-incorporated carbon shell,and there is void space between the core and the shell.When using as anode material for LIBs,Si@Co±NC displayed a super performance with a charge/discharge capacity of 191.6/191.4 mA h g^(-1)and a coulombic efficiency of 100.1%at 1000 mA g^(-1)after 3000 cycles,and the capacity loss rate is 0.022%per cycle only.The excellent electrochemical property of Si@Co±NC is because its electronic conductivity is enhanced by doping the carbon shell with N atoms and by incorporating with Co particles,and the pathway of lithium ions transmission is shortened by the hollow structure and abundant mesopores in the carbon shell.Also,the volume expansion of Si nanoparticles is well accommodated in the void space and suppressed by the carbon host matrix.This work shows that,through designing a superstructure for the anode materials,we can synergistically reduce the work function and introduce the confinement effect,thus significantly enhancing the anode materials’electrochemical performance in LIBs.
基金support from the National Key R&D Program of China(2016YFB0700600,2020YFB0704500)China Postdoctoral Science Foundation(2019M660317)+1 种基金Engineering and Physical Sciences Research Council,UK(EP/S000933/1)Shenzhen Science and Technology Program(Grant No.RCBS20200714114820077).
文摘The commercialized binder carboxymethyl cellulose sodium(CMC-Na)is considered unsuitable for micro-sized SiO_(x) anode as it cannot endure the large volume change to retain the conductive network during repeated charge/discharge cycles.Herein,a small amount of silicon nanoparticles(SiNPs)is added during slurry preparation process as“nano-combs”to unfold the convoluted CMC-Na polymer chains so that they undergo a coilto-stretch transition by interaction between polar groups(e.g.,-OH,-COONa)of polymer and SiNPs’large surface.Through maximizing the utilization of binders,a uniform conductive network is constructed with increased interfacial contact with micro-sized SiO_(x).As a result,the SiO_(x) electrode with optimized(10 wt%)SiNPs addition shows significantly improved initial capacity and cycling performance.Through revisiting CMCNa,a currently deemed unqualified binder in SiO_(x) anode,this work gives a brand-new perspective on the failing mechanism of Si-based anode materials and an improving strategy for electrode preparation.
基金the National Natural Science Foundation of China(NSFC,No.21203116)the Innovation Capability Support Plan of Shaanxi Province(Grant No.2022WGZJ-25)the Foundation of Shaanxi University of Science and Tech-nology(Grant No.210210031 and 210210032).
文摘Silicon(Si)holds promise as an anode material for lithium-ion batteries(LIBs)as it is widely avail-able and characterized by high specific capacity and suitable working potential.However,the relatively low electrical conductivity of Si and the significantly high extent of volume expansion realized dur-ing lithiation hinder its practical application.We prepared N-doped carbon polyhedral micro cage en-capsulated Si nanoparticles derived from Co-Mo bimetal metal-organic framework(MOFs)(denoted as Si/CoMo@NCP)and explored their lithium storage performance as anode materials to address these prob-lems.The Si/CoMo@NCP anode exhibited a high reversible lithium storage capacity(1013 mAh g^(−1)at 0.5 A g^(−1)after 100 cycles),stable cycle performance(745 mAh g^(−1)at 1 A g^(−1)after 400 cycles),and excellent rate performance(723 mAh g^(−1)at 2 A g^(−1)).Also,the constructed the full-cell NCM 811//Si/CoMo@NCP exhibited well reversible capacity.The excellent electrochemical performances of Si/CoMo@NCP were at-tributed to two unique properties.The encapsulation of NCP with doped nitrogen and porous structural carbon improves the electrical conductivity and cycling stability of the molecules.The introductions of metallic cobalt and its oxides help to improve the rate capability and lithiation capacity of the materials following multi-electron reaction mechanisms.
基金supported by the National Key Research and Development Program of China(No.2021YFB2500100)Science Fund for Creative Research Groupsof the National Natural Science Foundation of China(No.21921005)+1 种基金Beijing Natural Science Foundation(No.2222031)Hebei Natural Science Foundation(No.B2020103028)
文摘Si anode is of paramount importance for advanced energy-dense lithium-ion batteries(LIBs).However,the large volume change as well as stress generates during its lithiation-delithiation process poses a great challenge to the long-term cycling and hindering its application.Herein this work,a composite binder is prepared with a soft component,guar gum(GG),and a rigid linear polymer,anionic polyacrylamide(APAM).Rich hydroxy,carboxyl,and amide groups on the polymer chains not only enable intermolecular crosslinking to form a web-like binder,A2G1,but also realize strong chemical binding as well as physical encapsulating to Si particles.The resultant electrode shows limited thickness change of merely 9%on lithiation and almost recovers its original thickness on delithiation.It demonstrates high reversible capacity of 2104.3 mAh g^(-1)after 100 cycles at a current density of 1800 mA g^(-1),and in constant capacity(1000 mAh g^(-1))test,it also shows a long life of 392 cycles.Therefore,this soft-hard combining web-like binder illustrates its great potential in the future applications.
基金supported by the National Natural Science Foundation of China(No.51871113)Natural Science Foundation of Jiangsu Province(No.BK20200047).
文摘Silicon is recognized as the most advantageous next-generation anode material for LIBs in terms of its extremely high theoretical capacity and appropriate operating voltage.However,the application of Si anode is limited by huge volume expansion emerging with cycling,which in turn induces the collapse of the electrode structure,resulting in rapid capacity decay.Here,we report a strategy using self-swelling artificial laponite to prepare a laponite/MXene/CNT composite framework with both rigidity and flexibility,which can excellently address these challenges of Si anode.The self-swelling artificial laponite participates in the construction of hierarchical and porous structures,providing sufficient buffer space to mitigate the volume expansion of the LixSi alloying reaction.Meanwhile,tough and tightly cross-linked silicate nanosheets can improve the mechanical strength of the framework for strong structural stability.More importantly,the negative charge between the layers of artificial laponite can effectively promote fast Li-ion transport in the electrode.This free-standing silicon anode enables the preparation of high areal capacity electrodes to further enhance the energy density of LIBs and a higher reversible capacity of 2381.8 mAh/g at 0.1 C after 50 cycles with an initial coulombic of 85.6%.This work provides a simple and practical fabrication strategy for developing high-performance Si-based batteries,which can speed up their commercialization.
基金supported by the National Natural Science Foundation of China(51902165,12004145,52072323)the Natural Science Foundation of Jiangsu Province(BK20200800)+2 种基金the Natural Science Foundation of Jiangxi Province(20192ACBL20048)the Jiangxi Provincial Natural Science Foundation(20212BAB214032)the Nanjing Science&Technology Innovation Project for Personnel Studying Abroad。
文摘Replacing the conventional carbonate electrolyte by solid-state electrolyte (SSE) will offer improved safety for lithium-ion batteries.To further improve the energy density,Silicon (Si) is attractive for next generation solid-state battery (SSB) because of its high specific capacity and low cost.High energy density and safe Si-based SSB,however,is plagued by large volume change that leads to poor mechanical stability and slow lithium ions transportation at the multiple interfaces between Si and SSE.Herein,we designed a self-integrated and monolithic Si/two dimensional layered T_(3)C_(2)T_(x)(MXene,T_(x) stands for terminal functional groups) electrode architecture with interfacial nitrogen engineering.During a heat treatment process,the polyacrylonitrile not only converts into amorphous carbon (a-C) that shells Si but also forms robust interfacial nitrogen chemical bonds that anchors Si and MXene.During repeated lithiation and delithiation processes,the robust interfacial engineered Si/MXene configuration enhances the mechanical adhesion between Si and MXene that improves the structure stability but also contributes to form stable solid-electrolyte interphase (SEI).In addition,the N-MXene provides fast lithium ions transportation pathways.Consequently,the Si/MXene with interfacial nitrogen engineering (denoted as Si-N-MXene) deliveres high-rate performance with a specific capacity of 1498 m Ah g^(-1) at a high current of 6.4 A g^(-1).A Si-N-MXene/NMC full cell exhibited a capacity retention of 80.5%after 200 cycles.The Si-N-MXene electrode is also applied to SSB and shows a relative stable cycling over 100 cycles,demonstrating the versatility of this concept.
基金funded by the Science Foundation Ireland (SFI)under the Principal Investigator Program under contract No.11PI-1148,16/IA/4629 and SFI 16/M-ERA/3419funding under the European Union’s Horizon 2020 Research and Innovation Program+7 种基金grant agreement No.814464 (Si-DRIVE project)IRCLA/2017/285 and SFI Research Centres AMBER,Ma REI and CONFIRM 12/RC/2302_P2,12/RC/2278_P2,and 16/RC/3918SFI for SIRG grant No.18/SIRG/5484support from the Sustainable Energy Authority of Ireland through the Research Development and Demonstration Funding Program (Grant No.19/RDD/548)Enterprise Ireland through the Innovation Partnership Program (Grant No.IP 20190910)support from the SFI Research Centre Ma REI (award reference No.12/RC/2302_P2)support from the SFI Industry RD&I Fellowship Program (21/IRDIF/9876)the EU Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Individual Fellowship Grant (843621)。
文摘Silicon nanowires(Si NWs)have been widely researched as the best alternative to graphite anodes for the next-generation of high-performance lithium-ion batteries(LIBs)owing to their high capacity and low discharge potential.However,growing binder-free Si NW anodes with adequate mass loading and stable capacity is severely limited by the low surface area of planar current collectors(CCs),and is particularly challenging to achieve on standard pure-Cu substrates due to the ubiquitous formation of Li+inactive silicide phases.Here,the growth of densely-interwoven In-seeded Si NWs is facilitated by a thin-film of copper-silicide(CS)network in situ grown on a Cu-foil,allowing for a thin active NW layer(<10μm thick)and high areal loading(≈1.04 mg/cm^(2))binder-free electrode architecture.The electrode exhibits an average Coulombic efficiency(CE)of>99.6%and stable performance for>900 cycles with≈88.7%capacity retention.More significantly,it delivers a volumetric capacity of≈1086.1 m A h/cm^(3)at 5C.The full-cell versus lithium manganese oxide(LMO)cathode delivers a capacity of≈1177.1 m A h/g at 1C with a stable rate capability.This electrode architecture represents significant advances toward the development of binder-free Si NW electrodes for LIB application.
基金the National Natural Science Foundation of China(Nos.52071225 and 51672181)the Czech Republic through ERDF“Institute of Environmental Technology-Excellent Research”(No.CZ.02.1.01/0.0/0.0/16_019/0000853)M.H.R.acknowledges the Sino-German Research Institute for their support(Project GZ 1400).
文摘Inspired by the natural corn structure,a Si@hollow graphene shell@graphene(Si@GS@G)anode material was prepared in which silicon nanoparticles were preliminarily anchored onto the surface of an elastic graphene shell and further constrained using graphene sheets.Hollow graphene oxide shells with abundant surficial hydrogen bonds,which were synthesized using a novel bottom-up method,were used as an intermediate material to anchor positively charged silicon nanoparticles via electrostatic attraction and achieve a rational spatial distribution.The inner hollow graphene shell anchorage and outer graphene constraint synergistically constituted a porous and robust conductive corn-like structure.The as-fabricated Si@GS@G anode afforded efficient electron and ion transport pathways and improved structural stability,thereby enhancing Li+storage capability(505 mAh·g^(−1)at 10 A·g^(−1))and extending the lifespan compared to the single hollow graphene shell or graphene sheet-protected Si anode(72%capacity retention after 500 cycles).The improved kinetics of the Si@GS@G anode were investigated using electro impedance spectroscopy,galvanostatic intermittent titration,and pseudocapacitance contribution rate analysis,and the structural evolution was analyzed using ex situ electron microscopy.This study proposes a novel hollow graphene oxide shell as an activated intermediate material for designing a porous electrode structure that facilitates an enhanced electrochemical performance.
基金supported by the Major Program of Beijing Municipal Natural Science Foundation(No.2110001)the National Natural Science Foundation of China(No.11179001)the National High Technology Research and Development Program(No.2012AA052201)
文摘Silicon is being investigated extensively as an anodic material for next-generation lithium ion batteries for portable energy storage and electric vehicles.However,the large changes in volume during cycling lead to the breakdown of the conductive network in Si anodes and the formation of an unstable solid-electrolyte interface,resulting in capacity fading.Here,we demonstrate nanoparticles with a Si@Mn22.6Si5.4C4@C double-shell structure and the formation of self-organized Si-Mn-C nanocomposite anodes during the lithiation/delithiation process.The anode consists of amorphous Si particles less than 10 nm in diameter and separated by an interconnected conductive/buffer network,which exhibits excellent charge transfer kinetics and charge/discharge performances.A stable specific capacity of 1100 mAh·g-1 at 100 mA·g-1 and a coulombic efficiency of 99.2%after 30 cycles are achieved.Additionally,a rate capacity of 343 mAh·g-1 and a coulombic efficiency of 99.4%at 12000 mA·g-1 are also attainable.Owing to its simplicity and applicability,this strategy for improving electrode performance paves a way for the development of high-performance Si-based anodic materials for lithium ion batteries.
基金supported by the National Natural Science Foundation of China(Nos.22469010 and U24A2063)Yunnan Province Natural Science Fund(Nos.202501AT070331 and 202301AT070151)Yunnan Xingdian Young Talent Project(No.KKXX202452039).
文摘Silicon anodes are promising for high-energy-density lithium-ion batteries.Nevertheless,unsatisfied initial Coulombic efficiency(ICE)and structure collapse are two barriers still hindering their application.Here,we report a 5 at.%-vanadium hybriding strategy to stabilize Si film anode,which delivers a high initial Coulombic efficiency of 92.1%with a discharge capacity of 2434.9 mAh·g^(−1) and a desirable capacity retention of 80%after 100 cycles at 1 A·g^(−1).Physical and electrochemical analyses demonstrate the Li_(x)PO_(y)F_(z)-rich inorganic solid-electrolyte interphase(SEI)and the low film internal strain are two advantageous factors for the desirable Li-ion storage reversibility and stability.A full battery with a LiFePO_(4) cathode delivers the energy densities of 291.9 and 194.6 Wh·kg^(−1) under power densities of 145.9 and 389.2 W·kg^(−1),respectively.This result on Si anodes may pave the way to next-generation highenergy-density lithium-ion batteries.
基金financially supported by the National Natural Science Foundation of China (Nos. 51972182 and 61971252)the Shandong Provincial Natural Science Foundation (Nos. ZR2020JQ27 and ZR2019BF008)the Youth Innovation Team Project of Shandong Provincial Education Department (No. 2020KJN015)。
文摘The application of Si as the anode materials for lithium-ion batteries(LIBs) is still severely hindered by the rapid capacity decay due to the structural damage caused by large volume change(> 300%) during cycling. Herein, a three-dimensional(3 D) aerogel anode of Si@carbon@graphene(SCG) is rationally constructed via a polydopamine-assisted strategy. Polydopamine is coated on Si nanoparticles to serve as an interface linker to initiate the assembly of Si and graphene oxide, which plays a crucial role in the successful fabrication of SCG aerogels. After annealing the polydopamine is converted into N-doped carbon(N-carbon) coatings to protect Si materials. The dual protection from N-carbon and graphene aerogels synergistically improves the structural stability and electronic conductivity of Si, thereby leading to the significantly improved lithium storage properties. Electrochemical tests show that the SCG with optimized graphene content delivers a high capacity(712 m Ah/g at 100 m A/g) and robust cycling stability(402 m Ah/g at 1 A/g after 1500 cycles). Furthermore, the full cell using SCG aerogels as anode exhibits a reversible capacity of 187.6 m Ah/g after 80 cycles at 0.1 A/g. This work provides a plausible strategy for developing Si anode in LIBs.
