The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the che...The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the chemical prelithiation agent is difficult to dope active Li^(+) in silicon-based anodes because of their low working voltage and sluggish Li^(+) diffusion rate. By selecting the lithium–arene complex reagent with 4-methylbiphenyl as an anion ligand and 2-methyltetrahydrofuran as a solvent, the as-prepared micro-sized Si O/C anode can achieve an ICE of nearly 100%. Interestingly, the best prelithium efficiency does not correspond to the lowest redox half-potential(E_(1/2)), and the prelithiation efficiency is determined by the specific influencing factors(E_(1/2), Li^(+) concentration, desolvation energy, and ion diffusion path). In addition, molecular dynamics simulations demonstrate that the ideal prelithiation efficiency can be achieved by choosing appropriate anion ligand and solvent to regulate the solvation structure of Li^(+). Furthermore, the positive effect of prelithiation on cycle performance has been verified by using an in-situ electrochemical dilatometry and solid electrolyte interphase film characterizations.展开更多
Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utiliz...Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH) groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.展开更多
The inferior conductivity and drastic volume expansion of silicon still remain the bottleneck in achieving high energy density Lithium-ion Batteries(LIBs).The design of the three-dimensional structure of electrodes by...The inferior conductivity and drastic volume expansion of silicon still remain the bottleneck in achieving high energy density Lithium-ion Batteries(LIBs).The design of the three-dimensional structure of electrodes by compositing silicon and carbon materials has been employed to tackle the above challenges,however,the exorbitant costs and the uncertainty of the conductive structure persist,leaving ample room for improvement.Herein,silicon nanoparticles were innovatively composited with eco-friendly biochar sourced from cotton to fabricate a 3D globally consecutive conductive network.The network serves a dual purpose:enhancing overall electrode conductivity and serving as a scaffold to maintain electrode integrity.The conductivity of the network was further augmented by introducing P-doping at the optimum doping temperature of 350℃.Unlike the local conductive sites formed by the mere mixing of silicon and conductive agents,the consecutive network can affirm the improvement of the conductivity at a macro level.Moreover,first-principle calculations further validated that the rapid diffusion of Li^(+)is attributed to the tailored electronic microstructure and charge rearrangement of the fiber.The prepared consecutive conductive Si@P-doped carbonized cotton fiber anode outperforms the inconsecutive Si@Graphite anode in both cycling performance(capacity retention of 1777.15 mAh g^(-1) vs.682.56 mAh g^(-1) after 150 cycles at 0.3 C)and rate performance(1244.24 mAh g^(-1) vs.370.28 mAh g^(-1) at 2.0 C).The findings of this study may open up new avenues for the development of globally interconnected conductive networks in Si-based anodes,thereby enabling the fabrication of high-performance LIBs.展开更多
Silicon(Si)-based anodes have emerged as promising candidates for the next-generation lithium-ion batteries(LIBs)due to their high theoretical capacity(4200 mAh g^(-1)).However,their further application is hindered by...Silicon(Si)-based anodes have emerged as promising candidates for the next-generation lithium-ion batteries(LIBs)due to their high theoretical capacity(4200 mAh g^(-1)).However,their further application is hindered by critical challenges,including severe volume expansion(~300%),formation of unstable solid electrolyte interphase(SEI),and inherently low conductivity.While extensive research has sought to alleviate the substantial internal stress caused by volume expansion through the rational design of Si-based anode structures,the underlying mechanisms that govern these improvements remain insufficiently understood,leaving significant gaps in mechanical and interface electrical failure.To build a comprehensive understanding relationship between structural design and performance enhancement of Si-based anodes,this review first analyzes the characteristics of various Sibased anode structures and their associated internal stresses.Subsequently,it summarizes effective strategies to optimize the performance of Si-based anodes,including doping design,novel electrolyte design,and fu nctional binder design.Additionally,we assess emerging technologies with high commercial potential for structural design and interfacial modification,such as porous carbon carriers,chemical vapor deposition(CVD),spray granulation,and pre-lithiation.Finally,this work provides perspectives on the structural design of Si-based anodes.Overall,this review systematically summarizes modification strategies for Si-based anodes through structural regulation and interface engineering,thereby providing a foundation for advanced structural and interfacial design.展开更多
With the rapid advancement of technology and the growing demand for renewable energy,lithium-ion batteries have become the cornerstone of modern energy storage,particularly in electric vehicles.However,traditional gra...With the rapid advancement of technology and the growing demand for renewable energy,lithium-ion batteries have become the cornerstone of modern energy storage,particularly in electric vehicles.However,traditional graphite anodes limit further improvements in energy density and charging speed.Silicon,with its ultrahigh theoretical capacity,low cost,and environmental compatibility,has emerged as a promising alternative anode material.Nevertheless,its practical application is hindered by severe volume expansion during lithiation,unstable Solid-Electrolyte Interphase(SEI)formation,and low electrical conductivity.This study reviews and analyzes three mainstream strategies developed to address these challenges:(1)the design of silicon–carbon composite anodes to improve conductivity and structural stability;(2)the application of nano-engineered silicon architectures(0D to 3D)to buffer mechanical stress and enhance cycling performance;and(3)electrolyte modification to form more flexible and robust SEI layers.Through comparative analysis of multiple research teams,this paper summarizes how composite engineering,structural optimization,and electrolyte innovation collectively enhance silicon anode performance in terms of capacity retention,rate capability,and long-term stability.The findings indicate that hybrid approaches—combining chemical compositing,nanostructural design,and interfacial engineering—represent the most promising direction for achieving practical,scalable silicon-based anodes.With continued progress in low-cost synthesis and interface stabilization,silicon is expected to play a crucial role in next-generation high-energy lithium-ion batteries,meeting the growing global demand for efficient and sustainable energy storage.展开更多
Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth...Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth and side reactions.Existing Zn interfacial modification strategies based on single-component or homogeneous structure are insufficient to address these issues comprehensively.Herein,we rationally designed an organic-inorganic hybrid interfacial layer with rigid-to-soft graded structure for dendrite-free and stable Zn anodes.A liquid plasma-assisted oxidation technology is developed to rapidly construct a porous ZnO inner framework in situ.This ZnO layer offers high interfacial energy,mechanical robustness,and an open structure that facilitates ion transport while firmly anchoring a subsequently coated soft polymer layer.The resulting architecture presents a structurally graded and functionally complementary interface,enabling effective dendrite suppression,continuous Zn ion transport,and enhanced corrosion resistance.As a result,a long cycling stability of more than 6000 h can be achieved at 1 mA cm^(-2)for 1 mAh cm^(-2)in symmetric cells.When used as anodes for zinc-iodine full battery,the hybrid interlayer can effectively prevent the Zn anodes from the corrosion by polyiodine,enabling stable cycling and negligible capacity decay(~0.02‰per cycle)for over 10,000 cycles at 2.0 A g^(-1).This work demonstrates a promising interfacial design strategy and introduces a novel liquid plasma-assisted oxidation route for fabricating high-performance Zn anodes towards next-generation aqueous batteries.展开更多
The rapid expansion of the photovoltaic industry has generated heavily oxidized waste silicon(wSi),which hinders efficient recycling owing to its small particle size and uncontrolled surface oxidation.This study intro...The rapid expansion of the photovoltaic industry has generated heavily oxidized waste silicon(wSi),which hinders efficient recycling owing to its small particle size and uncontrolled surface oxidation.This study introduces a molten salt electrochemical strategy for converting photovoltaic wSi into NiSi_(2)-silicon nanorods(NiSi_(2)-SiNRs)as high-performance anode materials for lithium-ion batteries.A stable oxidized passivation layer is formed on the wSi surface via controlled oxidation,and further in situ generated highly active NiSi_(2) droplets.The molten salt electric field modulates the surface energy of silicon,while particle integration drives localized directional growth,enabling the self-assembly of NiSi_(2)-SiNRs composites.These NiSi_(2)-SiNRs anodes exhibit rapid ion transport and effective strain buffering.The high aspect ratio of SiNRs and the presence of retained NiSi_(2) facilitate both longitudinal and transverse Li^(+) diffusion.Owing to their robust structural design,the NiSi_(2)-SiNRs anode achieves an excellent initial Coulombic efficiency of 91.61%and retains 72.99%of its capacity after 800 cycles at 2 A·g^(−1).This study establishes a model system for investigating silicide/silicon interfaces in molten salt electrochemical synthesis and provides an effective strategy for upcycling photovoltaic wSi into high-performance lithium-ion battery anodes.展开更多
Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance i...Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.展开更多
Silicon(Si)is widely considered to be the most attractive candidate anode material for use in next-generation high-energy-density lithium(Li)-ion batteries(LIBs)because it has a high theoretical gravimetric Li storage...Silicon(Si)is widely considered to be the most attractive candidate anode material for use in next-generation high-energy-density lithium(Li)-ion batteries(LIBs)because it has a high theoretical gravimetric Li storage capacity,relatively low lithiation voltage,and abundant resources.Consequently,massive efforts have been exerted to improve its electrochemical performance.While some progress in this field has been achieved,a number of severe challenges,such as the element’s large volume change during cycling,low intrinsic electronic conductivity,and poor rate capacity,have yet to be solved.Methods to solve these problems have been attempted via the development of nanosized Si materials.Unfortunately,reviews summarizing the work on Si-based alloys are scarce.Herein,the recent progress related to Si-based alloy anode materials is reviewed.The problems associated with Si anodes and the corresponding strategies used to address these problems are first described.Then,the available Si-based alloys are divided into Si/Li-active and inactive systems,and the characteristics of these systems are discussed.Other special systems are also introduced.Finally,perspectives and future outlooks are provided to enable the wider application of Si-alloy anodes to commercial LIBs.展开更多
Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challen...Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challenged by its low conductivity and drastic volume variation during the Li uptake/release process. Tremendous efforts have been made on shrinking the particle size of Si into nanoscale so that the volume variation could be accommodated. However, the bare nano-Si material would still pulverize upon (de)lithiation. Moreover, it shows an excessive surface area to invite unlimited growth of solid electrolyte interface that hinders the transportation of charge carriers, and an increased interparticle resistance. As a result, the Si nanoparticles gradually lose their electrical contact during the cycling process, which accounts for poor thermodynamic stability and sluggish kinetics of the anode reaction versus Li. To address these problems and improve the Li storage performance of nano-Si anode, proper structural design should be applied on the Si anode. In this perspective, we will briefly review some strategies for improving the electrochemistry versus Li of nano-Si materials and their derivatives, and show opinions on the optimal design of nanostructured Si anode for advanced LIBs.展开更多
Conventional lithium-ion batteries(LIBs)with graphite anodes are approaching their theoretical limitations in energy density.Replacing the conventional graphite anodes with high-capacity Si-based anodes represents one...Conventional lithium-ion batteries(LIBs)with graphite anodes are approaching their theoretical limitations in energy density.Replacing the conventional graphite anodes with high-capacity Si-based anodes represents one of the most promising strategies to greatly boost the energy density of LIBs.However,the inherent huge volume expansion of Si-based materials after lithiation and the resulting series of intractable problems,such as unstable solid electrolyte interphase layer,cracking of electrode,and especially the rapid capacity degradation of cells,severely restrict the practical application of Sibased anodes.Over the past decade,numerous reports have demonstrated that polymer binders play a critical role in alleviating the volume expansion and maintaining the integrity and stable cycling of Si-based anodes.In this review,the state-of-the-art designing of polymer binders for Si-based anodes have been systematically summarized based on their structures,including the linear,branched,crosslinked,and conjugated conductive polymer binders.Especially,the comprehensive designing of multifunctional polymer binders,by a combination of multiple structures,interactions,crosslinking chemistries,ionic or electronic conductivities,soft and hard segments,and so forth,would be promising to promote the practical application of Si-based anodes.Finally,a perspective on the rational design of practical polymer binders for the large-scale application of Si-based anodes is presented.展开更多
Silicon(Si)-based solid-state batteries(Si-SSBs)are attracting tremendous attention because of their high energy density and unprecedented safety,making them become promising candidates for next-generation energy stor...Silicon(Si)-based solid-state batteries(Si-SSBs)are attracting tremendous attention because of their high energy density and unprecedented safety,making them become promising candidates for next-generation energy storage systems.Nevertheless,the commercialization of Si-SSBs is significantly impeded by enormous challenges including large volume variation,severe interfacial problems,elusive fundamental mechanisms,and unsatisfied electrochemical performance.Besides,some unknown electrochemical processes in Si-based anode,solid-state electrolytes(SSEs),and Si-based anode/SSE interfaces are still needed to be explored,while an in-depth understanding of solid–solid interfacial chemistry is insufficient in Si-SSBs.This review aims to summarize the current scientific and technological advances and insights into tackling challenges to promote the deployment of Si-SSBs.First,the differences between various conventional liquid electrolyte-dominated Si-based lithium-ion batteries(LIBs)with Si-SSBs are discussed.Subsequently,the interfacial mechanical contact model,chemical reaction properties,and charge transfer kinetics(mechanical–chemical kinetics)between Si-based anode and three different SSEs(inorganic(oxides)SSEs,organic–inorganic composite SSEs,and inorganic(sulfides)SSEs)are systemically reviewed,respectively.Moreover,the progress for promising inorganic(sulfides)SSE-based Si-SSBs on the aspects of electrode constitution,three-dimensional structured electrodes,and external stack pressure is highlighted,respectively.Finally,future research directions and prospects in the development of Si-SSBs are proposed.展开更多
Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilizati...Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilization,are crucially important for the development of a more sustainable world.In this study,we employed a straightforward direct carbonization method within the temperature range of 700-1000℃to convert the worthless solid waste CTR into economically valuable carbon materials as anodes for potassium-ion batteries(PIBs).The effect of carbonization temperature on the microstructure and the potassium ions storage properties of CTR-derived carbons(CTRCs)were systematically explored by structural and morphological characterization,alongside electrochemical performances assessment.Based on the co-regulation between the turbine layers,crystal structure,pore structure,functional groups,and electrical conductivity of CTR-derived carbon carbonized at 900℃(CTRC-900H),the electrode material with high reversible capacity of 265.6m Ah·g^(-1)at 50 m A·g^(-1),a desirable cycling stability with 93.8%capacity retention even after 100 cycles,and the remarkable rate performance for PIBs were obtained.Furthermore,cyclic voltammetry(CV)at different scan rates and galvanostatic intermittent titration technique(GITT)have been employed to explore the potassium ions storage mechanism and electrochemical kinetics of CTRCs.Results indicate that the electrode behavior is predominantly governed by surface-induced capacitive processes,particularly under high current densities,with the potassium storage mechanism characterized by an“adsorption-weak intercalation”mechanism.This work highlights the potential of CTR-based carbon as a promising electrode material category suitable for high-performance PIBs electrodes,while also provides valuable insights into the new avenues for the high value-added utilization of CTR.展开更多
In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid...In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid solution atoms in theα-Mg matrix without its second-phase generation,and at the same time facilitates grain refinement,dendritic segregation and Mg17Sr2-phases precipitation.During discharge operation,Sr modifies the film composition via its compounds and promoted the redeposition of In at the substrate/film interface;their co-deposition behavior on the anodic reaction surface enhances anode reaction kinetics,suppresses the negative difference effect(NDE)and mitigates the“chunk effect”(CE),which is contributed to uniform dissolution and low self-corrosion hydrogen evolution rate(HER).Therefore,Mg-Sr-xIn alloy anodes show excellent discharge performance,e.g.,0.5Sr-1.0In shows an average discharge voltage of 1.4234 V and a specific energy density of 1990.71 Wh kg^(-1)at 10 mA cm^(-2).Furthermore,the decisive factor(CE and self-discharge HE)for anodic efficiency are quantitively analyzed,the self-discharge is the main factor of cell efficiency loss.Surprisingly,all Mg-Sr-xIn anodes show anodic efficiency greater than 60%at high current density(≥10 mA cm^(-2)),making them excellent candidate anodes for Mg-Air cells at high-power output.展开更多
Sodium-ion batteries(SIBs) are promising electrochemical energy storage systems as lithium-ion batteries by virtue of their similar chemical properties and natural abundance and availability.However,the ionic radius o...Sodium-ion batteries(SIBs) are promising electrochemical energy storage systems as lithium-ion batteries by virtue of their similar chemical properties and natural abundance and availability.However,the ionic radius of Na^(+)is larger than that of Li^(+),leading to challenges in its insertion/extraction at anode side.As a class of anode materials,phosphorus allotropes(PAs,red,and black) and metal phosphides(MPs) have shown great prospects because of high theoretical gravimetric/volumetric capacity,high carrier mobility,and suitable redox potential.In this review,recent developments in the studies of PAs and MPs with particular emphasis on understanding sodium storage mechanisms,developing novel synthesis strategies,and performance validations have been manifested valuable solutions to address these challenges.We begin with the introduction and classification of the macroscopic sodiation mechanisms of PAs and MPs,and the various fabrication strategies of PAs and MPs are comprehensively summarized in second section.The third section thoroughly reviews the progresses on PAs and MPs-based advanced materials for their application in SIBs.Finally,we also discuss the significant challenges and outline a roadmap for future research directions.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
Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the sol...Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.展开更多
Aqueous zinc-ion batteries are regarded as promising electrochemical energy-storage systems for various applications because of their high safety,low costs,and high capacities.However,dendrite formation and side react...Aqueous zinc-ion batteries are regarded as promising electrochemical energy-storage systems for various applications because of their high safety,low costs,and high capacities.However,dendrite formation and side reactions during zinc plating or stripping greatly reduce the capacity and cycle life of a battery and subsequently limit its practical application.To address these issues,we modified the surface of a zinc anode with a functional bilayer composed of zincophilic Cu and flexible polymer layers.The zincophilic Cu interfacial layer was prepared through CuSO_(4)solution pretreatment to serve as a nucleation site to facilitate uniform Zn deposition.Meanwhile,the polymer layer was coated onto the Cu interface layer to serve as a protective layer that would prevent side reactions between zinc and electrolytes.Benefiting from the synergistic effect of the zincophilic Cu and protective polymer layers,the symmetric battery exhibits an impressive cycle life,lasting over 2900 h at a current density of 1 m A·cm^(-2)with a capacity of 1 m A·h·cm^(-2).Moreover,a full battery paired with a vanadium oxide cathode achieves a remarkable capacity retention of 72%even after 500 cycles.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
Recently,potassium-ion batteries(PIBs)have received significant attention in the energy storage field owing to their high-power output,fast charging capability,natural abundance,and environmental sustainability.Herein...Recently,potassium-ion batteries(PIBs)have received significant attention in the energy storage field owing to their high-power output,fast charging capability,natural abundance,and environmental sustainability.Herein,we comprehensively review recent advancements in the design and development of carbon-based anode materials for PIBs anodes,covering graphite,hard carbon,alloy and conversion materials with carbon,and carbon host for K metal deposition.Chemical strategies such as structural engineering,heteroatom-doping,and surface modifications are highlighted to improve electrochemical performances as well as to resolve technical challenges,such as electrode instability,low initial Coulombic efficiency,and electrolyte compatibility.Furthermore,we discuss the fundamental understanding of potassium-ion storage mechanisms of carbon-based materials and their correlation with electrochemical performance.Finally,we present the current challenges and future research directions for the practical implementation of carbon-based anodes to enhance their potential as next-generation energy storage materials for PIBs.This review aims to provide our own insights into innovative design strategies for advanced PIB's anode through the chemical and engineering strategies.展开更多
基金supported by the National Natural Science Foundation of China (21875107, U1802256, and 22209204)Leading Edge Technology of Jiangsu Province (BK20220009), the Natural Science Foundation of Jiangsu Province (BK20221140)+2 种基金the China Postdoctoral Science Foundation (2022M713364)Jiangsu Specially Appointed Professors ProgramPriority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)。
文摘The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the chemical prelithiation agent is difficult to dope active Li^(+) in silicon-based anodes because of their low working voltage and sluggish Li^(+) diffusion rate. By selecting the lithium–arene complex reagent with 4-methylbiphenyl as an anion ligand and 2-methyltetrahydrofuran as a solvent, the as-prepared micro-sized Si O/C anode can achieve an ICE of nearly 100%. Interestingly, the best prelithium efficiency does not correspond to the lowest redox half-potential(E_(1/2)), and the prelithiation efficiency is determined by the specific influencing factors(E_(1/2), Li^(+) concentration, desolvation energy, and ion diffusion path). In addition, molecular dynamics simulations demonstrate that the ideal prelithiation efficiency can be achieved by choosing appropriate anion ligand and solvent to regulate the solvation structure of Li^(+). Furthermore, the positive effect of prelithiation on cycle performance has been verified by using an in-situ electrochemical dilatometry and solid electrolyte interphase film characterizations.
基金supported by the National Natural Science Foundation of China (51673017)the National Natural Science Foundation of China (21404005)+1 种基金the Fundamental Research Funds for the Central Universities (XK1802-2)the Natural Science Foundation of Jiangsu Province (BK20150273)。
文摘Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH) groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.
基金supported by the National Natural Science Foundation of China(No.12205252)the Basic Public Welfare Re-search Special Project of Zhejiang Province(No.LZY22B040001)+4 种基金the Quzhou Science and Technology Plan Project(No.2022K39)Science and Technology Project of Quzhou Research Institute,Zhejiang University(Nos.IZQ2021KJ2032,IZQ2022KJ3014,and IZQ2022KJ3002)Independent scientific Research Project of Quzhou Research Institute,Zhejiang University(No.IZQ2021RCZX007)New“115 talents”Project ofQuzhou,National Nature Science Foundation of China(No.52172244)Fundamental Research Funds for the Central University(No.226202200053).
文摘The inferior conductivity and drastic volume expansion of silicon still remain the bottleneck in achieving high energy density Lithium-ion Batteries(LIBs).The design of the three-dimensional structure of electrodes by compositing silicon and carbon materials has been employed to tackle the above challenges,however,the exorbitant costs and the uncertainty of the conductive structure persist,leaving ample room for improvement.Herein,silicon nanoparticles were innovatively composited with eco-friendly biochar sourced from cotton to fabricate a 3D globally consecutive conductive network.The network serves a dual purpose:enhancing overall electrode conductivity and serving as a scaffold to maintain electrode integrity.The conductivity of the network was further augmented by introducing P-doping at the optimum doping temperature of 350℃.Unlike the local conductive sites formed by the mere mixing of silicon and conductive agents,the consecutive network can affirm the improvement of the conductivity at a macro level.Moreover,first-principle calculations further validated that the rapid diffusion of Li^(+)is attributed to the tailored electronic microstructure and charge rearrangement of the fiber.The prepared consecutive conductive Si@P-doped carbonized cotton fiber anode outperforms the inconsecutive Si@Graphite anode in both cycling performance(capacity retention of 1777.15 mAh g^(-1) vs.682.56 mAh g^(-1) after 150 cycles at 0.3 C)and rate performance(1244.24 mAh g^(-1) vs.370.28 mAh g^(-1) at 2.0 C).The findings of this study may open up new avenues for the development of globally interconnected conductive networks in Si-based anodes,thereby enabling the fabrication of high-performance LIBs.
基金supported by the Science and Technology Plan of Fujian Provincial,China(2022G02020 and 2022H6002)the Collaborative Innovation Platform Project for Advanced Electrochemical Energy Storage Technology,Fuxiaquan National Independent Innovation Demonstration Zone,China(3502ZCQXT2022001)+1 种基金the Significant Science and Technology Project of Xiamen(the Future Industrial Area),China(3502Z20231058)the Scientific Research Startup Funding for Special Professor of Minjiang Scholars。
文摘Silicon(Si)-based anodes have emerged as promising candidates for the next-generation lithium-ion batteries(LIBs)due to their high theoretical capacity(4200 mAh g^(-1)).However,their further application is hindered by critical challenges,including severe volume expansion(~300%),formation of unstable solid electrolyte interphase(SEI),and inherently low conductivity.While extensive research has sought to alleviate the substantial internal stress caused by volume expansion through the rational design of Si-based anode structures,the underlying mechanisms that govern these improvements remain insufficiently understood,leaving significant gaps in mechanical and interface electrical failure.To build a comprehensive understanding relationship between structural design and performance enhancement of Si-based anodes,this review first analyzes the characteristics of various Sibased anode structures and their associated internal stresses.Subsequently,it summarizes effective strategies to optimize the performance of Si-based anodes,including doping design,novel electrolyte design,and fu nctional binder design.Additionally,we assess emerging technologies with high commercial potential for structural design and interfacial modification,such as porous carbon carriers,chemical vapor deposition(CVD),spray granulation,and pre-lithiation.Finally,this work provides perspectives on the structural design of Si-based anodes.Overall,this review systematically summarizes modification strategies for Si-based anodes through structural regulation and interface engineering,thereby providing a foundation for advanced structural and interfacial design.
文摘With the rapid advancement of technology and the growing demand for renewable energy,lithium-ion batteries have become the cornerstone of modern energy storage,particularly in electric vehicles.However,traditional graphite anodes limit further improvements in energy density and charging speed.Silicon,with its ultrahigh theoretical capacity,low cost,and environmental compatibility,has emerged as a promising alternative anode material.Nevertheless,its practical application is hindered by severe volume expansion during lithiation,unstable Solid-Electrolyte Interphase(SEI)formation,and low electrical conductivity.This study reviews and analyzes three mainstream strategies developed to address these challenges:(1)the design of silicon–carbon composite anodes to improve conductivity and structural stability;(2)the application of nano-engineered silicon architectures(0D to 3D)to buffer mechanical stress and enhance cycling performance;and(3)electrolyte modification to form more flexible and robust SEI layers.Through comparative analysis of multiple research teams,this paper summarizes how composite engineering,structural optimization,and electrolyte innovation collectively enhance silicon anode performance in terms of capacity retention,rate capability,and long-term stability.The findings indicate that hybrid approaches—combining chemical compositing,nanostructural design,and interfacial engineering—represent the most promising direction for achieving practical,scalable silicon-based anodes.With continued progress in low-cost synthesis and interface stabilization,silicon is expected to play a crucial role in next-generation high-energy lithium-ion batteries,meeting the growing global demand for efficient and sustainable energy storage.
基金support from the Australian Research Council Discovery Program(DP220103416,DP240102177)Australian Research Council Future Fellowships(FT200100730,FT210100804).
文摘Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth and side reactions.Existing Zn interfacial modification strategies based on single-component or homogeneous structure are insufficient to address these issues comprehensively.Herein,we rationally designed an organic-inorganic hybrid interfacial layer with rigid-to-soft graded structure for dendrite-free and stable Zn anodes.A liquid plasma-assisted oxidation technology is developed to rapidly construct a porous ZnO inner framework in situ.This ZnO layer offers high interfacial energy,mechanical robustness,and an open structure that facilitates ion transport while firmly anchoring a subsequently coated soft polymer layer.The resulting architecture presents a structurally graded and functionally complementary interface,enabling effective dendrite suppression,continuous Zn ion transport,and enhanced corrosion resistance.As a result,a long cycling stability of more than 6000 h can be achieved at 1 mA cm^(-2)for 1 mAh cm^(-2)in symmetric cells.When used as anodes for zinc-iodine full battery,the hybrid interlayer can effectively prevent the Zn anodes from the corrosion by polyiodine,enabling stable cycling and negligible capacity decay(~0.02‰per cycle)for over 10,000 cycles at 2.0 A g^(-1).This work demonstrates a promising interfacial design strategy and introduces a novel liquid plasma-assisted oxidation route for fabricating high-performance Zn anodes towards next-generation aqueous batteries.
基金supported by the Yunnan Province Basic Research General Program,China(No.202201BE070001-002)the Major Science and Technology Projects in Yunnan Province,China(No.202402AF 080005).
文摘The rapid expansion of the photovoltaic industry has generated heavily oxidized waste silicon(wSi),which hinders efficient recycling owing to its small particle size and uncontrolled surface oxidation.This study introduces a molten salt electrochemical strategy for converting photovoltaic wSi into NiSi_(2)-silicon nanorods(NiSi_(2)-SiNRs)as high-performance anode materials for lithium-ion batteries.A stable oxidized passivation layer is formed on the wSi surface via controlled oxidation,and further in situ generated highly active NiSi_(2) droplets.The molten salt electric field modulates the surface energy of silicon,while particle integration drives localized directional growth,enabling the self-assembly of NiSi_(2)-SiNRs composites.These NiSi_(2)-SiNRs anodes exhibit rapid ion transport and effective strain buffering.The high aspect ratio of SiNRs and the presence of retained NiSi_(2) facilitate both longitudinal and transverse Li^(+) diffusion.Owing to their robust structural design,the NiSi_(2)-SiNRs anode achieves an excellent initial Coulombic efficiency of 91.61%and retains 72.99%of its capacity after 800 cycles at 2 A·g^(−1).This study establishes a model system for investigating silicide/silicon interfaces in molten salt electrochemical synthesis and provides an effective strategy for upcycling photovoltaic wSi into high-performance lithium-ion battery anodes.
基金supported by Multi-Year Research Grants from the University of Macao(MYRG-GRG2023-00010-IAPME,MYRG-GRG2024-00038-IAPME,MYRG2022-00026-IAPME)the Science and Technology Development Fund(FDCT)from Macao SAR(0023/2023/AFJ,0050/2023/RIB2,006/2022/ALC,0087/2024/AFJ,0111/2022/A2).
文摘Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.
基金financially supported by the National Natural Science Foundation of China(No.52074360)the Natural Science Foundation for Distinguished Young Scholars of Hunan Province(No.2020JJ2047)+1 种基金the Program of Huxiang Young Talents(No.2019RS2002)the Innovation-Driven Project of Central South University(No.2020CX027).
文摘Silicon(Si)is widely considered to be the most attractive candidate anode material for use in next-generation high-energy-density lithium(Li)-ion batteries(LIBs)because it has a high theoretical gravimetric Li storage capacity,relatively low lithiation voltage,and abundant resources.Consequently,massive efforts have been exerted to improve its electrochemical performance.While some progress in this field has been achieved,a number of severe challenges,such as the element’s large volume change during cycling,low intrinsic electronic conductivity,and poor rate capacity,have yet to be solved.Methods to solve these problems have been attempted via the development of nanosized Si materials.Unfortunately,reviews summarizing the work on Si-based alloys are scarce.Herein,the recent progress related to Si-based alloy anode materials is reviewed.The problems associated with Si anodes and the corresponding strategies used to address these problems are first described.Then,the available Si-based alloys are divided into Si/Li-active and inactive systems,and the characteristics of these systems are discussed.Other special systems are also introduced.Finally,perspectives and future outlooks are provided to enable the wider application of Si-alloy anodes to commercial LIBs.
基金the financial support of this work by the National Natural Science Foundation of China (No.21773078)the Fundamental Research Funds for the Central Universities of China (Nos.2662015PY163 and 2662017JC025).
文摘Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challenged by its low conductivity and drastic volume variation during the Li uptake/release process. Tremendous efforts have been made on shrinking the particle size of Si into nanoscale so that the volume variation could be accommodated. However, the bare nano-Si material would still pulverize upon (de)lithiation. Moreover, it shows an excessive surface area to invite unlimited growth of solid electrolyte interface that hinders the transportation of charge carriers, and an increased interparticle resistance. As a result, the Si nanoparticles gradually lose their electrical contact during the cycling process, which accounts for poor thermodynamic stability and sluggish kinetics of the anode reaction versus Li. To address these problems and improve the Li storage performance of nano-Si anode, proper structural design should be applied on the Si anode. In this perspective, we will briefly review some strategies for improving the electrochemistry versus Li of nano-Si materials and their derivatives, and show opinions on the optimal design of nanostructured Si anode for advanced LIBs.
基金Beijing National Laboratory for Molecular Sciences,Grant/Award Number:2019BMS20022National Natural Science Foundation of China,Grant/Award Number:22005314+3 种基金Strategic Priority Research Program of the Chinese Academy of Sciences,Grant/Award Number:XDA21070300The China Postdoctoral Science Foundation,Grant/Award Number:2019M660805The National Key R&D Program of China,Grant/Award Number:2019YFA0705600The Special Financial Grant from the China Postdoctoral Science Foundation,Grant/Award Number:2020T130658。
文摘Conventional lithium-ion batteries(LIBs)with graphite anodes are approaching their theoretical limitations in energy density.Replacing the conventional graphite anodes with high-capacity Si-based anodes represents one of the most promising strategies to greatly boost the energy density of LIBs.However,the inherent huge volume expansion of Si-based materials after lithiation and the resulting series of intractable problems,such as unstable solid electrolyte interphase layer,cracking of electrode,and especially the rapid capacity degradation of cells,severely restrict the practical application of Sibased anodes.Over the past decade,numerous reports have demonstrated that polymer binders play a critical role in alleviating the volume expansion and maintaining the integrity and stable cycling of Si-based anodes.In this review,the state-of-the-art designing of polymer binders for Si-based anodes have been systematically summarized based on their structures,including the linear,branched,crosslinked,and conjugated conductive polymer binders.Especially,the comprehensive designing of multifunctional polymer binders,by a combination of multiple structures,interactions,crosslinking chemistries,ionic or electronic conductivities,soft and hard segments,and so forth,would be promising to promote the practical application of Si-based anodes.Finally,a perspective on the rational design of practical polymer binders for the large-scale application of Si-based anodes is presented.
基金supported by the National Natural Science Foundation of China(Grants Nos.52072323,52122211 and 21875155)the State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources(Grant No.LAPS22005)+3 种基金the Frontier Exploration Projects of Longmen Laboratory(Grant No.LMQYTSKT008)the Shenzhen Technical Plan Project(No.JCYJ20220818101003008)the support of High-Tech Industrialization Project of Tan Kah Kee Innovation Laboratory(Grant No.RD2021010101)the“Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen University.L.Zhang and Q.Zhang acknowledge the support of the Nanqiang Young Top-notch Talent Fellowship at Xiamen University.
文摘Silicon(Si)-based solid-state batteries(Si-SSBs)are attracting tremendous attention because of their high energy density and unprecedented safety,making them become promising candidates for next-generation energy storage systems.Nevertheless,the commercialization of Si-SSBs is significantly impeded by enormous challenges including large volume variation,severe interfacial problems,elusive fundamental mechanisms,and unsatisfied electrochemical performance.Besides,some unknown electrochemical processes in Si-based anode,solid-state electrolytes(SSEs),and Si-based anode/SSE interfaces are still needed to be explored,while an in-depth understanding of solid–solid interfacial chemistry is insufficient in Si-SSBs.This review aims to summarize the current scientific and technological advances and insights into tackling challenges to promote the deployment of Si-SSBs.First,the differences between various conventional liquid electrolyte-dominated Si-based lithium-ion batteries(LIBs)with Si-SSBs are discussed.Subsequently,the interfacial mechanical contact model,chemical reaction properties,and charge transfer kinetics(mechanical–chemical kinetics)between Si-based anode and three different SSEs(inorganic(oxides)SSEs,organic–inorganic composite SSEs,and inorganic(sulfides)SSEs)are systemically reviewed,respectively.Moreover,the progress for promising inorganic(sulfides)SSE-based Si-SSBs on the aspects of electrode constitution,three-dimensional structured electrodes,and external stack pressure is highlighted,respectively.Finally,future research directions and prospects in the development of Si-SSBs are proposed.
基金financially supported by the Research Project Supported by Shanxi Scholarship Council of China(No.2022-049)the Natural Science Foundation of Shanxi Province,China(No.20210302123167)。
文摘Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilization,are crucially important for the development of a more sustainable world.In this study,we employed a straightforward direct carbonization method within the temperature range of 700-1000℃to convert the worthless solid waste CTR into economically valuable carbon materials as anodes for potassium-ion batteries(PIBs).The effect of carbonization temperature on the microstructure and the potassium ions storage properties of CTR-derived carbons(CTRCs)were systematically explored by structural and morphological characterization,alongside electrochemical performances assessment.Based on the co-regulation between the turbine layers,crystal structure,pore structure,functional groups,and electrical conductivity of CTR-derived carbon carbonized at 900℃(CTRC-900H),the electrode material with high reversible capacity of 265.6m Ah·g^(-1)at 50 m A·g^(-1),a desirable cycling stability with 93.8%capacity retention even after 100 cycles,and the remarkable rate performance for PIBs were obtained.Furthermore,cyclic voltammetry(CV)at different scan rates and galvanostatic intermittent titration technique(GITT)have been employed to explore the potassium ions storage mechanism and electrochemical kinetics of CTRCs.Results indicate that the electrode behavior is predominantly governed by surface-induced capacitive processes,particularly under high current densities,with the potassium storage mechanism characterized by an“adsorption-weak intercalation”mechanism.This work highlights the potential of CTR-based carbon as a promising electrode material category suitable for high-performance PIBs electrodes,while also provides valuable insights into the new avenues for the high value-added utilization of CTR.
文摘In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid solution atoms in theα-Mg matrix without its second-phase generation,and at the same time facilitates grain refinement,dendritic segregation and Mg17Sr2-phases precipitation.During discharge operation,Sr modifies the film composition via its compounds and promoted the redeposition of In at the substrate/film interface;their co-deposition behavior on the anodic reaction surface enhances anode reaction kinetics,suppresses the negative difference effect(NDE)and mitigates the“chunk effect”(CE),which is contributed to uniform dissolution and low self-corrosion hydrogen evolution rate(HER).Therefore,Mg-Sr-xIn alloy anodes show excellent discharge performance,e.g.,0.5Sr-1.0In shows an average discharge voltage of 1.4234 V and a specific energy density of 1990.71 Wh kg^(-1)at 10 mA cm^(-2).Furthermore,the decisive factor(CE and self-discharge HE)for anodic efficiency are quantitively analyzed,the self-discharge is the main factor of cell efficiency loss.Surprisingly,all Mg-Sr-xIn anodes show anodic efficiency greater than 60%at high current density(≥10 mA cm^(-2)),making them excellent candidate anodes for Mg-Air cells at high-power output.
基金financially supported by the Natural Science Foundation of China(Nos.22208214,22005190,and 21938005)the Science&Technology Commission of Shanghai Municipality(Nos.20QB1405700,and 19DZ1205500)Zhejiang Key Research and Development Program(No.2020C01128)
文摘Sodium-ion batteries(SIBs) are promising electrochemical energy storage systems as lithium-ion batteries by virtue of their similar chemical properties and natural abundance and availability.However,the ionic radius of Na^(+)is larger than that of Li^(+),leading to challenges in its insertion/extraction at anode side.As a class of anode materials,phosphorus allotropes(PAs,red,and black) and metal phosphides(MPs) have shown great prospects because of high theoretical gravimetric/volumetric capacity,high carrier mobility,and suitable redox potential.In this review,recent developments in the studies of PAs and MPs with particular emphasis on understanding sodium storage mechanisms,developing novel synthesis strategies,and performance validations have been manifested valuable solutions to address these challenges.We begin with the introduction and classification of the macroscopic sodiation mechanisms of PAs and MPs,and the various fabrication strategies of PAs and MPs are comprehensively summarized in second section.The third section thoroughly reviews the progresses on PAs and MPs-based advanced materials for their application in SIBs.Finally,we also discuss the significant challenges and outline a roadmap for future research directions.
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support from the National Natural Science Foundation of China(No.U2333210)the Sichuan Science and Technology Program,China(No.21SYSX0011)。
文摘Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.
基金financially supported by the Science and Technology Development Project of Henan Province,China(No.242102241042)the Joint Fund of Henan Province Science and Technology R&D Program(No.225200810093)+1 种基金the Startup Research of Henan Academy of Sciences(No.231817001)the Key Innovation Projects for Postgraduates of Henan Academy of Sciences(No.24331712)。
文摘Aqueous zinc-ion batteries are regarded as promising electrochemical energy-storage systems for various applications because of their high safety,low costs,and high capacities.However,dendrite formation and side reactions during zinc plating or stripping greatly reduce the capacity and cycle life of a battery and subsequently limit its practical application.To address these issues,we modified the surface of a zinc anode with a functional bilayer composed of zincophilic Cu and flexible polymer layers.The zincophilic Cu interfacial layer was prepared through CuSO_(4)solution pretreatment to serve as a nucleation site to facilitate uniform Zn deposition.Meanwhile,the polymer layer was coated onto the Cu interface layer to serve as a protective layer that would prevent side reactions between zinc and electrolytes.Benefiting from the synergistic effect of the zincophilic Cu and protective polymer layers,the symmetric battery exhibits an impressive cycle life,lasting over 2900 h at a current density of 1 m A·cm^(-2)with a capacity of 1 m A·h·cm^(-2).Moreover,a full battery paired with a vanadium oxide cathode achieves a remarkable capacity retention of 72%even after 500 cycles.
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 Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.RS-2024-00453815)Korea Institute of Energy Technology Evaluation and Planning(KETEP)grant funded by the Korea government(MOTIE)(20228510070100)。
文摘Recently,potassium-ion batteries(PIBs)have received significant attention in the energy storage field owing to their high-power output,fast charging capability,natural abundance,and environmental sustainability.Herein,we comprehensively review recent advancements in the design and development of carbon-based anode materials for PIBs anodes,covering graphite,hard carbon,alloy and conversion materials with carbon,and carbon host for K metal deposition.Chemical strategies such as structural engineering,heteroatom-doping,and surface modifications are highlighted to improve electrochemical performances as well as to resolve technical challenges,such as electrode instability,low initial Coulombic efficiency,and electrolyte compatibility.Furthermore,we discuss the fundamental understanding of potassium-ion storage mechanisms of carbon-based materials and their correlation with electrochemical performance.Finally,we present the current challenges and future research directions for the practical implementation of carbon-based anodes to enhance their potential as next-generation energy storage materials for PIBs.This review aims to provide our own insights into innovative design strategies for advanced PIB's anode through the chemical and engineering strategies.
