Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ions.Currently,organic electrode materials ...Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ions.Currently,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials(>1 V).Organic electrodes with low redox potential that can be used as anode are rare.Herein,a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na_(4)TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic stability.Its three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per cycle.Moreover,the Na_(4)TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm^(-2).By pairing with a thick Na_(3)V_(2)(PO_(4))_(3)cathode (20.6 mg cm^(-2)),the as-fabricated full cell exhibited high operating voltage (2.8 V),excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na_(4)TDC anode material for SIBs.展开更多
With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its ...With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its exceptionally high capacity for LIBs.However,the significant volumetric changes of SiO_(x)during cycling and its initial Coulombic efficiency(ICE)complicate its use,whether alone or in combination with graphite materials.In this study,a three-dimensional conductive binder network with high electronic conductivity and robust elasticity for graphite/SiO_(x)blended anodes was proposed by chemically anchoring carbon nanotubes and carboxymethyl cellulose binders using tannic acid as a chemical cross-linker.In addition,a dehydrogenation-based prelithiation strategy employing lithium hydride was utilized to enhance the ICE of SiO_(x).The combination of these two strategies increased the CE of SiO_(x)from 74%to87%and effectively mitigated its volume expansion in the graphite/SiO_(x)blended electrode,resulting in an efficient electron-conductive binder network.This led to a remarkable capacity retention of 94%after30 cycles,even under challenging conditions,with a high capacity of 550 mA h g^(-1)and a current density of 4 mA cm^(-2).Furthermore,to validate the feasibility of utilizing prelithiated SiO_(x)anode materials and the conductive binder network in LIBs,a full cell incorporating these materials and a single-crystalline Ni-rich cathode was used.This cell demonstrated a~27.3%increase in discharge capacity of the first cycle(~185.7 mA h g^(-1))and exhibited a cycling stability of 300 cycles.Thus,this study reports a simple,feasible,and insightful method for designing high-performance LIB electrodes.展开更多
The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batterie...The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batteries,especially in terms of energy density and reliability.Nevertheless,few SLMBs can deliver the required cycling performance and long-term stability for practical use,primarily due to suboptimal interface properties.Given the diverse solidification pathways leading to different interface characteristics,it is crucial to pinpoint the source of interface deterioration and develop appropriate remedies.This review focuses on Li|SSE interface issues between lithium metal anode and SSE,discussing recent advancements in the understanding of(electro)chemistry,the impact of defects,and interface evolutions that vary among different SSE species.The state-ofthe-art strategies concerning modified SEI,artificial interlayer,surface architecture,and composite structure are summarized and delved into the internal relationships between interface characteristics and performance enhancements.The current challenges and opportunities in characterizing and modifying the Li|SSE interface are suggested as potential directions for achieving practical SLMBs.展开更多
H_(2)O-induced side reactions and dendrite growth occurring at the Zn anode-electrolyte interface(AEI)limit the electrochemical performances of aqueous zinc ion batteries.Herein,methionine(Met)is introduced as an elec...H_(2)O-induced side reactions and dendrite growth occurring at the Zn anode-electrolyte interface(AEI)limit the electrochemical performances of aqueous zinc ion batteries.Herein,methionine(Met)is introduced as an electrolyte additive to solve the above issues by three aspects:Firstly,Met is anchored on Zn anode by amino/methylthio groups to form a H_(2)O-poor AEI,thus increasing the overpotential of hydrogen evolution reaction(HER);secondly,Met serves as a pH buffer to neutralize the HER generated OH-,thereby preventing the formation of by-products(e.g.Zn_(4)SO_(4)(OH)_(6)·xH_(2)O);thirdly,Zn^(2+) could be captured by carboxyl group of the anchored Met through electrostatic interaction,which promotes the dense and flat Zn deposition.Consequently,the Zn||Zn symmetric cell obtains a long cycle life of 3200 h at 1.0 mA cm^(-2),1.0 mAh cm^(-2),and 1400 h at 5.0 mA cm^(-2),5.0 mAh cm^(-2).Moreover,Zn||VO_(2) full cell exhibits a capacity retention of 91.0%after operating for 7000 cycles at 5.0 A g^(-1).This study offers a novel strategy for modulating the interface microenvironment of AEI via integrating the molecular adsorption,pH buffer,and Zn^(2+) capture strategies to design advanced industrial-oriented batteries.展开更多
Sodium metal has been widely studied in the field of batteries due to its high theoretical specific capacity(~1,166 m Ah/g),low redox potential(-2.71 V compared to standard hydrogen electrode),and lowcost advantages.H...Sodium metal has been widely studied in the field of batteries due to its high theoretical specific capacity(~1,166 m Ah/g),low redox potential(-2.71 V compared to standard hydrogen electrode),and lowcost advantages.However,problems such as unstable solid electrolyte interface(SEI),uncontrolled dendrite growth,and side reactions between solid-liquid interfaces have hindered the practical application of sodium metal anodes(SMAs).Currently,lots of strategies have been developed to achieve stabilized sodium metal anodes.Among these strategies,modified metal current collectors(MCCs)stand out due to their unique role in accommodating volumetric fluctuations with superior structure,lowering the energy barrier for sodium nucleation,and providing guided uniform sodium deposition.In this review,we first introduced three common metal-based current collectors applied to SMAs.Then,we summarized strategies to improve sodium deposition behavior by optimally engineering the surface of MCCs,including surface loading,surface structural design,and surface engineering for functional modification.We have followed the latest research progress and summarized surface optimization cases on different MCCs and their applications in battery systems.展开更多
Metal foils have emerged as one of the promising materials for anode-free batteries due to their high energy density and scalability in production.The unclear lithium plating/stripping kinetics of metal foil current c...Metal foils have emerged as one of the promising materials for anode-free batteries due to their high energy density and scalability in production.The unclear lithium plating/stripping kinetics of metal foil current collectors in anode-free batteries was addressed by using the non-destructive distribution of relaxation times(DRT)analysis to systematically investigate the lithium transport behavior of 14 metal foils and its correlation with electrochemical performance.By integrating energy-dispersive spectro scopy(EDS),cyclic voltammetry(CV),and galvanostatic testing,the exceptional properties of indium(In),tin(Sn),and silver(Ag)were revealed:the Li-In alloying reaction exhibits high reversibility,Li-Sn alloys demonstrate outstanding cycling stability,and the Li-Ag solid-solution mechanism provides an ideal lithium deposition interface on the silver substrate.The DRT separates the polarization internal resistance of lithium ions passing through the SEI layer(R_(sei),τ2)and the polarization internal resistance of lithium ions undergoing charge transfer reaction at the electrolyte/electrode interface(R_(ct),τ3)by decoupling the electrochemical impedance spectroscopy(EIS).For the first time,the correlation betweenτ2,τ3,and the cycle life/Coulombic efficiency of alloy/solid-solution metals was established,while non-alloy metals are not suitable for this method due to differences in lithium deposition mechanisms.This study not only illuminates the structure-property relationship governing the lithium kinetics of metal foil electrodes but also provides a novel non-destructive analytical strategy and theoretical guidance for the rational design of stable anodes in high-energy-density batteries,facilitating the efficient screening and optimization of anode-free battery.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
The dominated contradiction in optimizing the performance of magnesium-air battery anode lies in the difficulty of achieving a good balance between activation and passivation during discharge process.To further reconci...The dominated contradiction in optimizing the performance of magnesium-air battery anode lies in the difficulty of achieving a good balance between activation and passivation during discharge process.To further reconcile this contradiction,two Mg-0.1Sc-0.1Y-0.1Ag anodes with different residual strain distribution through extrusion with/without annealing are fabricated.The results indicate that annealing can significantly lessen the“pseudo-anode”regions,thereby changing the dissolution mode of the matrix and achieving an effective dissolution during discharge.Additionally,p-type semiconductor characteristic of discharge productfilm could suppress the self-corrosion reaction without reducing the polarization of anode.The magnesium-air battery utilizing annealed Mg-0.1Sc-0.1Y-0.1Ag as anode achieves a synergistic improvement in specific capacity(1388.89 mA h g^(-1))and energy density(1960.42 mW h g^(-1)).This anode modification method accelerates the advancement of high efficiency and long lifespan magnesium-air batteries,offering renewable and cost-effective energy solutions for electronics and emergency equipment.展开更多
The poor reversibility and stability of Zn anodes greatly restrict the practical application of aqueous Zn-ion batteries(AZIBs),resulting from the uncontrollable dendrite growth and H_(2)O-induced side reactions durin...The poor reversibility and stability of Zn anodes greatly restrict the practical application of aqueous Zn-ion batteries(AZIBs),resulting from the uncontrollable dendrite growth and H_(2)O-induced side reactions during cycling.Electrolyte additive modification is considered one of the most effective and simplest methods for solving the aforementioned problems.Herein,the pyridine derivatives(PD)including 2,4-dihydroxypyridine(2,4-DHP),2,3-dihydroxypyridine(2,3-DHP),and 2-hydroxypyrdine(2-DHP),were em-ployed as novel electrolyte additives in ZnSO_(4)electrolyte.Both density functional theory calculation and experimental findings demonstrated that the incorporation of PD additives into the electrolyte effectively modulates the solvation structure of hydrated Zn ions,thereby suppressing side reactions in AZIBs.Ad-ditionally,the adsorption of PD molecules on the zinc anode surface contributed to uniform Zn deposi-tion and dendrite growth inhibition.Consequently,a 2,4-DHP-modified Zn/Zn symmetrical cell achieved an extremely long cyclic stability up to 5650 h at 1 mA cm^(-2).Furthermore,the Zn/NH_(4)V_(4)O_(10)full cell with 2,4-DHP-containing electrolyte exhibited an outstanding initial capacity of 204 mAh g^(-1),with a no-table capacity retention of 79%after 1000 cycles at 5 A g^(-1).Hence,this study expands the selection of electrolyte additives for AZIBs,and the working mechanism of PD additives provides new insights for electrolyte modification enabling highly reversible zinc anode.展开更多
Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hamp...Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hampered by the instability of both the anode-electrolyte interface and the cathode-electrolyte interface.The use of sodium gluconate(SG),an organic sodium salt with multiple hydroxyl groups,as an electrolyte additive is suggested.Experimental and theoretical analyses demonstrate that Na^(+)from SG can intercalate and deintercalate within the associated V_(2)O_(5) cathode during in situ electrochemical processes.This action supports the layered structure of V_(2)O_(5),prevents structural collapse and phase transitions,and enhances Zn^(2+)diffusion kinetics.Additionally,the gluconate anion disrupts the original Zn^(2+)solvation structure,mitigates water-induced side reactions,and suppresses Zn dendrite growth.The synchronous regulation of both the V_(2)O_(5) cathode and Zn anode by the SG additive leads to considerable performance improvements.Zn‖Zn symmetric batteries demonstrate a cycle life exceeding 2800 h at 0.5 mA cm^(-2)and 1 mAh cm^(-2).In Zn‖V_(2)O_(5) full batteries,a high specific capacity of 288.92 mAh g^(-1)and capacity retention of 82.29%are maintained over 1000 cycles at a current density of 2 A g^(-1).This multifunctional additive strategy offers a new pathway for the practical application of AZIBs.展开更多
Silicon is believed to be a critical anode material for approaching the roadmap of lithium-ion batteries due to its high specific capacity. But this aim has been hindered by the quick capacity fading of its electrodes...Silicon is believed to be a critical anode material for approaching the roadmap of lithium-ion batteries due to its high specific capacity. But this aim has been hindered by the quick capacity fading of its electrodes during repeated charge–discharge cycles. In this work, a “soft-hard”double-layer coating has been proposed and carried out on ball-milled silicon particles. It is composed of inside conductive pathway and outside elastic coating, which is achieved by decomposing a conductive graphite layer on the silicon surface and further coating it with a polymer layer.The incorporation of the second elastic coating on the inside carbon coating enables silicon particles strongly interacted with binders, thereby making the electrodes displaying an obviously improved cycling stability. As-obtained double-coated silicon anodes deliver a reversible capacity of 2280 m Ah g^(-1)at the voltage of 0.05–2 V, and maintains over 1763 mAh g^(-1)after 50 cycles. The double-layer coating does not crack after the repeated cycling, critical for the robust performance of the electrodes. In addition, as-obtained silicon particles are mixed with commercial graphite to make actual anodes for lithium-ion batteries. A capacity of 714 mAh g^(-1)has been achieved based on the total mass of the electrodes containing 10 wt.% double-coated silicon particles. Compared with traditional carbon coating or polymeric coating, the double-coating electrodes display a much better performance. Therefore, the double-coating strategy can give inspiration for better design and synthesis of silicon anodes, as well as other battery materials.展开更多
Graphite-silicon species(Gr-Si)hybrid anodes have merged as potential candidates for high-energy lithium-ion batteries(LIBs),yet long been plagued by rapid capacity fading due to their unstable mechano-electrochemistr...Graphite-silicon species(Gr-Si)hybrid anodes have merged as potential candidates for high-energy lithium-ion batteries(LIBs),yet long been plagued by rapid capacity fading due to their unstable mechano-electrochemistry.The dominant approach to enhance electrochemical stability of the Gr-Si hybrid anodes typically involves the optimization of the electrode material structures and the employment of low active Si species content in electrode(<10 wt%in most instances).However,the electrode structure design,a factor of equal importance in determining the electrochemical performance of Gr-Si hybrid anodes,has received scant attention.In this study,three Gr-Si hybrid anodes with the identical material composition but distinct electrode structures are designed to investigate the mechanoelectrochemistry of the electrodes.It is revealed that the substantial volume change of Si species particles in Gr-Si hybrid anodes led to the local lattice stress of Gr at their contact interface during the charge/discharge processes,thereby increasing thermodynamic and kinetic barrier of Li-ion migration.Furthermore,the huge disparity in volume change of Si species and Gr particles trigger the separate agglomeration of these two materials,resulting in a considerable electrode volume change and increased electrochemical resistance.An advanced Gr/Si hybrid anode with upper Gr and lower Si species layer structure design addresses the above challenges using photovoltaic waste silicon sources under high Si species content(17 wt%)and areal capacity(2.0 mA h cm^(-2))in Ah-level full pouch cells with a low negative/positive(N/P)ratio of 1.09.The cell shows stable cycling for 100 cycles at 0.3 C with an impressively low capacity decay rate of 0.0546%per cycle,outperforming most reported Gr-Si hybrid anodes.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
Manganese-based chalcogenides have significant potential as anodes for sodium-ion batteries(SIBs) due to their high theoretical specific capacity, abundant natural reserves, and environmental friendliness. However, th...Manganese-based chalcogenides have significant potential as anodes for sodium-ion batteries(SIBs) due to their high theoretical specific capacity, abundant natural reserves, and environmental friendliness. However, their application is hindered by poor cycling stability, resulting from severe volume changes during cycling and slow reaction kinetics due to their complex crystal structure. Here, an efficient and straightforward strategy was employed to in-situ encapsulate single-phase porous nanocubic MnS_(0.5)Se_(0.5) into carbon nanofibers using electrospinning and the hard template method, thus forming a necklace-like porous MnS_(0.5)Se_(0.5)-carbon nanofiber composite(MnS_(0.5)Se_(0.5)@N-CNF). The introduction of Se significantly impacts both the composition and microstructure of MnS_(0.5)Se_(0.5), including lattice distortion that generates additional defects, optimization of chemical bonds, and a nano-spatially confined design. In situ/ex-situ characterization and density functional theory calculations verified that this MnS_(0.5)Se_(0.5)@N-CNF allevi- ates the volume expansion and facilitates the transfer of Na+/electron. As expected, MnS_(0.5)Se_(0.5)@N-CNF anode demonstrates excellent sodium storage performance, characterized by high initial Coulombic efficiency(90.8%), high-rate capability(370.5 m Ahg^(-1) at 10 Ag^(-1)) and long durability(over 5000 cycles at 5 Ag^(-1)). The MnS_(0.5)Se_(0.5)@N-CNF//NVP@C full cell, assembled with MnS_(0.5)Se_(0.5)@N-CNF as anode and Na_(3)V_(2)(PO_4)_(3)@C as cathode, exhibits a high energy density of 254 Wh kg^(-1) can be provided. This work presents a novel strategy to optimize the design of anode materials through structural engineering and Se substitution, while also elucidating the underlying reaction mechanisms.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
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
As an emerging electrochemical energy storage technology,potassium-ion batteries(PIBs),which are considered a“beyond Li-ion”battery system,have attracted tremendous attention due to their potential for providing a h...As an emerging electrochemical energy storage technology,potassium-ion batteries(PIBs),which are considered a“beyond Li-ion”battery system,have attracted tremendous attention due to their potential for providing a high energy density,and having abundant resource,and a low cost.However,their commercialization is hindered by the lack of practical anode materials.Among various reported anodes,conventional carbon materials,including graphite,soft carbon,and hard carbon,have emerged as promising candidates because of their abundance,low cost,high conductivity,and tunable structures.However,these materials have problems such as a low initial Coulombic efficiency,significant volume expansion,and unsatisfactory cyclability and rate performance.Various strategies to solve these have been explored,including optimizing the interlayer spacing,structural design,surface coating,constructing a multifunctional framework,and forming composites.This review provides a comprehensive overview of the recent progress in conventional carbon anodes,highlighting structural design strategies,mechanisms for improving the electrochemical performance,and underscores the critical role of these materials in promoting the practical application of PIBs.展开更多
Direct ethanol fuel cells(DEFCs)are a promising alternative to conventional energy sources,offering high energy density,environmental sustainability,and operational safety.Compared to methanol fuel cells,DEFCs exhibit...Direct ethanol fuel cells(DEFCs)are a promising alternative to conventional energy sources,offering high energy density,environmental sustainability,and operational safety.Compared to methanol fuel cells,DEFCs exhibit lower toxicity and a more mature preparation process.Unlike hydrogen fuel cells,DEFCs provide superior storage and transport feasibility,as well as cost-effectiveness,significantly enhancing their commercial viability.However,the stable C-C bond in ethanol creates a high activation energy barrier,often resulting in incomplete electrooxidation.Current commercial platinum(Pt)-and palladium(Pd)-based catalysts demonstrate low C-C bond cleavage efficiency(<7.5%),severely limiting DEFC energy output and power density.Furthermore,high catalyst costs and insufficient activity impede large-scale commercialization.Recent advances in DEFC anode catalyst design have focused on optimizing material composition and elucidating catalytic mechanisms.This review systematically examines developments in ethanol electrooxidation catalysts over the past five years,highlighting strategies to improve C1 pathway selectivity and C-C bond activation.Key approaches,such as alloying,nanostructure engineering,and interfacial synergy effects,are discussed alongside their mechanistic implications.Finally,we outline current challenges and future prospects for DEFC commercialization.展开更多
The advantages of sodium-ion batteries(SIBs)for large-scale energy storage are well known.Among possible anode materials,hard carbon(HC)stands out as the most viable commercial option because of its superior performan...The advantages of sodium-ion batteries(SIBs)for large-scale energy storage are well known.Among possible anode materials,hard carbon(HC)stands out as the most viable commercial option because of its superior performance.However,there is still disagreement regarding the sodium storage mechanism in the low-voltage plateau region of HC anodes,and the structure-performance relationship between its complex multiscale micro/nanostructure and electrochemical behavior remains unclear.This paper summarizes current research progress and the major problems in understanding HC’s microstructure and sodium storage mechanism,and the relationship between them.Findings about a universal sodium storage mechanism in HC,including predictions about micropore-capacity relationships,and the opportunities and challenges for using HC anodes in commercial SIBs are presented.展开更多
基金National Key Research and Development Program of China (2022YFB2402200)National Natural Science Foundation of China (22225201,22379028)+2 种基金Fundamental Research Funds for the Central Universities (20720220010)Shanghai Pilot Program for Basic Research–Fudan University 21TQ1400100 (21TQ009)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (23520750400)。
文摘Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C,H,O,and sodium ions.Currently,organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials(>1 V).Organic electrodes with low redox potential that can be used as anode are rare.Herein,a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate,Na_(4)TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic stability.Its three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations,showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022%per cycle.Moreover,the Na_(4)TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm^(-2).By pairing with a thick Na_(3)V_(2)(PO_(4))_(3)cathode (20.6 mg cm^(-2)),the as-fabricated full cell exhibited high operating voltage (2.8 V),excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles,well highlighting the Na_(4)TDC anode material for SIBs.
基金supported by the National Research Foundation(NRF)of Korea grant funded by the Korean government(MSIT)(No.NRF-2021 M3 H4A1A02045962).
文摘With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its exceptionally high capacity for LIBs.However,the significant volumetric changes of SiO_(x)during cycling and its initial Coulombic efficiency(ICE)complicate its use,whether alone or in combination with graphite materials.In this study,a three-dimensional conductive binder network with high electronic conductivity and robust elasticity for graphite/SiO_(x)blended anodes was proposed by chemically anchoring carbon nanotubes and carboxymethyl cellulose binders using tannic acid as a chemical cross-linker.In addition,a dehydrogenation-based prelithiation strategy employing lithium hydride was utilized to enhance the ICE of SiO_(x).The combination of these two strategies increased the CE of SiO_(x)from 74%to87%and effectively mitigated its volume expansion in the graphite/SiO_(x)blended electrode,resulting in an efficient electron-conductive binder network.This led to a remarkable capacity retention of 94%after30 cycles,even under challenging conditions,with a high capacity of 550 mA h g^(-1)and a current density of 4 mA cm^(-2).Furthermore,to validate the feasibility of utilizing prelithiated SiO_(x)anode materials and the conductive binder network in LIBs,a full cell incorporating these materials and a single-crystalline Ni-rich cathode was used.This cell demonstrated a~27.3%increase in discharge capacity of the first cycle(~185.7 mA h g^(-1))and exhibited a cycling stability of 300 cycles.Thus,this study reports a simple,feasible,and insightful method for designing high-performance LIB electrodes.
基金Financial support from National Key R&D Program(2022YFB2404600)Natural Science Foundation of China(Key Project of 52131306)+1 种基金Project on Carbon Emission Peak and Neutrality of Jiangsu Province(BE2022031-4)the Big Data Computing Center of Southeast University are greatly appreciated.
文摘The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batteries,especially in terms of energy density and reliability.Nevertheless,few SLMBs can deliver the required cycling performance and long-term stability for practical use,primarily due to suboptimal interface properties.Given the diverse solidification pathways leading to different interface characteristics,it is crucial to pinpoint the source of interface deterioration and develop appropriate remedies.This review focuses on Li|SSE interface issues between lithium metal anode and SSE,discussing recent advancements in the understanding of(electro)chemistry,the impact of defects,and interface evolutions that vary among different SSE species.The state-ofthe-art strategies concerning modified SEI,artificial interlayer,surface architecture,and composite structure are summarized and delved into the internal relationships between interface characteristics and performance enhancements.The current challenges and opportunities in characterizing and modifying the Li|SSE interface are suggested as potential directions for achieving practical SLMBs.
基金supported by the National Natural Science Foundation of China(22479031,22162004)the Natural Science Foundation of Guangxi(2022JJD120011).
文摘H_(2)O-induced side reactions and dendrite growth occurring at the Zn anode-electrolyte interface(AEI)limit the electrochemical performances of aqueous zinc ion batteries.Herein,methionine(Met)is introduced as an electrolyte additive to solve the above issues by three aspects:Firstly,Met is anchored on Zn anode by amino/methylthio groups to form a H_(2)O-poor AEI,thus increasing the overpotential of hydrogen evolution reaction(HER);secondly,Met serves as a pH buffer to neutralize the HER generated OH-,thereby preventing the formation of by-products(e.g.Zn_(4)SO_(4)(OH)_(6)·xH_(2)O);thirdly,Zn^(2+) could be captured by carboxyl group of the anchored Met through electrostatic interaction,which promotes the dense and flat Zn deposition.Consequently,the Zn||Zn symmetric cell obtains a long cycle life of 3200 h at 1.0 mA cm^(-2),1.0 mAh cm^(-2),and 1400 h at 5.0 mA cm^(-2),5.0 mAh cm^(-2).Moreover,Zn||VO_(2) full cell exhibits a capacity retention of 91.0%after operating for 7000 cycles at 5.0 A g^(-1).This study offers a novel strategy for modulating the interface microenvironment of AEI via integrating the molecular adsorption,pH buffer,and Zn^(2+) capture strategies to design advanced industrial-oriented batteries.
基金supported by the National Natural Science Foundation of China(Nos.52102291,52271011,and 51701142)supported by a grant from the Cangzhou Institute of Tiangong University(No.TGCYY-F-0201)。
文摘Sodium metal has been widely studied in the field of batteries due to its high theoretical specific capacity(~1,166 m Ah/g),low redox potential(-2.71 V compared to standard hydrogen electrode),and lowcost advantages.However,problems such as unstable solid electrolyte interface(SEI),uncontrolled dendrite growth,and side reactions between solid-liquid interfaces have hindered the practical application of sodium metal anodes(SMAs).Currently,lots of strategies have been developed to achieve stabilized sodium metal anodes.Among these strategies,modified metal current collectors(MCCs)stand out due to their unique role in accommodating volumetric fluctuations with superior structure,lowering the energy barrier for sodium nucleation,and providing guided uniform sodium deposition.In this review,we first introduced three common metal-based current collectors applied to SMAs.Then,we summarized strategies to improve sodium deposition behavior by optimally engineering the surface of MCCs,including surface loading,surface structural design,and surface engineering for functional modification.We have followed the latest research progress and summarized surface optimization cases on different MCCs and their applications in battery systems.
基金supported by the Quzhou Science and Technology Bureau Project(2023D023,2023D030,2023D002,and2024D028)the Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(LZY23B030002)+3 种基金the Shijiazhuang Shangtai Technology Co.,Ltd.Hebei Provincial Department of Science and Technology(24291101Z)the International Cooperation Projects of Sichuan Provincial Department of Science and Technology(2021YFH0126)the Sichuan Provincial Science and Technology Department's key research project(2023YFG0203)。
文摘Metal foils have emerged as one of the promising materials for anode-free batteries due to their high energy density and scalability in production.The unclear lithium plating/stripping kinetics of metal foil current collectors in anode-free batteries was addressed by using the non-destructive distribution of relaxation times(DRT)analysis to systematically investigate the lithium transport behavior of 14 metal foils and its correlation with electrochemical performance.By integrating energy-dispersive spectro scopy(EDS),cyclic voltammetry(CV),and galvanostatic testing,the exceptional properties of indium(In),tin(Sn),and silver(Ag)were revealed:the Li-In alloying reaction exhibits high reversibility,Li-Sn alloys demonstrate outstanding cycling stability,and the Li-Ag solid-solution mechanism provides an ideal lithium deposition interface on the silver substrate.The DRT separates the polarization internal resistance of lithium ions passing through the SEI layer(R_(sei),τ2)and the polarization internal resistance of lithium ions undergoing charge transfer reaction at the electrolyte/electrode interface(R_(ct),τ3)by decoupling the electrochemical impedance spectroscopy(EIS).For the first time,the correlation betweenτ2,τ3,and the cycle life/Coulombic efficiency of alloy/solid-solution metals was established,while non-alloy metals are not suitable for this method due to differences in lithium deposition mechanisms.This study not only illuminates the structure-property relationship governing the lithium kinetics of metal foil electrodes but also provides a novel non-destructive analytical strategy and theoretical guidance for the rational design of stable anodes in high-energy-density batteries,facilitating the efficient screening and optimization of anode-free battery.
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the National Natural Science:Foundation of China(52375370)the Open Project of Salt Lake Chemical Engineering Research Complex,Qinghai University(2023-DXSSKF-Z02)+2 种基金the Nat-ural Science Foundation of Shanxi(202103021224049)GDAS Projects of International cooperation platform of Sci-ence and Technology(2022GDASZH-2022010203-003)Guangdong province Science and Technology Plan Projects(2023B1212060045).
文摘The dominated contradiction in optimizing the performance of magnesium-air battery anode lies in the difficulty of achieving a good balance between activation and passivation during discharge process.To further reconcile this contradiction,two Mg-0.1Sc-0.1Y-0.1Ag anodes with different residual strain distribution through extrusion with/without annealing are fabricated.The results indicate that annealing can significantly lessen the“pseudo-anode”regions,thereby changing the dissolution mode of the matrix and achieving an effective dissolution during discharge.Additionally,p-type semiconductor characteristic of discharge productfilm could suppress the self-corrosion reaction without reducing the polarization of anode.The magnesium-air battery utilizing annealed Mg-0.1Sc-0.1Y-0.1Ag as anode achieves a synergistic improvement in specific capacity(1388.89 mA h g^(-1))and energy density(1960.42 mW h g^(-1)).This anode modification method accelerates the advancement of high efficiency and long lifespan magnesium-air batteries,offering renewable and cost-effective energy solutions for electronics and emergency equipment.
基金supported by the Key Science and Technol-ogy Program of Henan Province(No.232102241020)the Ph.D.Research Startup Foundation of Henan University of Science and Technology(No.400613480015)+1 种基金the Postdoctoral Research Startup Foundation of Henan University of Science and Technology(No.400613554001)the Natural Science Foundation of Henan Province(242300420021).
文摘The poor reversibility and stability of Zn anodes greatly restrict the practical application of aqueous Zn-ion batteries(AZIBs),resulting from the uncontrollable dendrite growth and H_(2)O-induced side reactions during cycling.Electrolyte additive modification is considered one of the most effective and simplest methods for solving the aforementioned problems.Herein,the pyridine derivatives(PD)including 2,4-dihydroxypyridine(2,4-DHP),2,3-dihydroxypyridine(2,3-DHP),and 2-hydroxypyrdine(2-DHP),were em-ployed as novel electrolyte additives in ZnSO_(4)electrolyte.Both density functional theory calculation and experimental findings demonstrated that the incorporation of PD additives into the electrolyte effectively modulates the solvation structure of hydrated Zn ions,thereby suppressing side reactions in AZIBs.Ad-ditionally,the adsorption of PD molecules on the zinc anode surface contributed to uniform Zn deposi-tion and dendrite growth inhibition.Consequently,a 2,4-DHP-modified Zn/Zn symmetrical cell achieved an extremely long cyclic stability up to 5650 h at 1 mA cm^(-2).Furthermore,the Zn/NH_(4)V_(4)O_(10)full cell with 2,4-DHP-containing electrolyte exhibited an outstanding initial capacity of 204 mAh g^(-1),with a no-table capacity retention of 79%after 1000 cycles at 5 A g^(-1).Hence,this study expands the selection of electrolyte additives for AZIBs,and the working mechanism of PD additives provides new insights for electrolyte modification enabling highly reversible zinc anode.
基金supported by the Battery Energy Storage Testing Center of Chongqing through their provision of testing support and technical assistance。
文摘Aqueous zinc-ion batteries(AZIBs)are gaining attention owing to their affordability,high safety,and high energy density,making them a promising solution for large-scale energy storage.However,their performance is hampered by the instability of both the anode-electrolyte interface and the cathode-electrolyte interface.The use of sodium gluconate(SG),an organic sodium salt with multiple hydroxyl groups,as an electrolyte additive is suggested.Experimental and theoretical analyses demonstrate that Na^(+)from SG can intercalate and deintercalate within the associated V_(2)O_(5) cathode during in situ electrochemical processes.This action supports the layered structure of V_(2)O_(5),prevents structural collapse and phase transitions,and enhances Zn^(2+)diffusion kinetics.Additionally,the gluconate anion disrupts the original Zn^(2+)solvation structure,mitigates water-induced side reactions,and suppresses Zn dendrite growth.The synchronous regulation of both the V_(2)O_(5) cathode and Zn anode by the SG additive leads to considerable performance improvements.Zn‖Zn symmetric batteries demonstrate a cycle life exceeding 2800 h at 0.5 mA cm^(-2)and 1 mAh cm^(-2).In Zn‖V_(2)O_(5) full batteries,a high specific capacity of 288.92 mAh g^(-1)and capacity retention of 82.29%are maintained over 1000 cycles at a current density of 2 A g^(-1).This multifunctional additive strategy offers a new pathway for the practical application of AZIBs.
基金supported by the National Natural Science Foundation of China (No. 22008256)。
文摘Silicon is believed to be a critical anode material for approaching the roadmap of lithium-ion batteries due to its high specific capacity. But this aim has been hindered by the quick capacity fading of its electrodes during repeated charge–discharge cycles. In this work, a “soft-hard”double-layer coating has been proposed and carried out on ball-milled silicon particles. It is composed of inside conductive pathway and outside elastic coating, which is achieved by decomposing a conductive graphite layer on the silicon surface and further coating it with a polymer layer.The incorporation of the second elastic coating on the inside carbon coating enables silicon particles strongly interacted with binders, thereby making the electrodes displaying an obviously improved cycling stability. As-obtained double-coated silicon anodes deliver a reversible capacity of 2280 m Ah g^(-1)at the voltage of 0.05–2 V, and maintains over 1763 mAh g^(-1)after 50 cycles. The double-layer coating does not crack after the repeated cycling, critical for the robust performance of the electrodes. In addition, as-obtained silicon particles are mixed with commercial graphite to make actual anodes for lithium-ion batteries. A capacity of 714 mAh g^(-1)has been achieved based on the total mass of the electrodes containing 10 wt.% double-coated silicon particles. Compared with traditional carbon coating or polymeric coating, the double-coating electrodes display a much better performance. Therefore, the double-coating strategy can give inspiration for better design and synthesis of silicon anodes, as well as other battery materials.
基金the financial support by the National Natural Science Foundation of China(52072137)the National Natural Science Foundation of China(22205068)the"CUG Scholar"Scientific Research Funds at China University of Geosciences(Wuhan)(2022118)。
文摘Graphite-silicon species(Gr-Si)hybrid anodes have merged as potential candidates for high-energy lithium-ion batteries(LIBs),yet long been plagued by rapid capacity fading due to their unstable mechano-electrochemistry.The dominant approach to enhance electrochemical stability of the Gr-Si hybrid anodes typically involves the optimization of the electrode material structures and the employment of low active Si species content in electrode(<10 wt%in most instances).However,the electrode structure design,a factor of equal importance in determining the electrochemical performance of Gr-Si hybrid anodes,has received scant attention.In this study,three Gr-Si hybrid anodes with the identical material composition but distinct electrode structures are designed to investigate the mechanoelectrochemistry of the electrodes.It is revealed that the substantial volume change of Si species particles in Gr-Si hybrid anodes led to the local lattice stress of Gr at their contact interface during the charge/discharge processes,thereby increasing thermodynamic and kinetic barrier of Li-ion migration.Furthermore,the huge disparity in volume change of Si species and Gr particles trigger the separate agglomeration of these two materials,resulting in a considerable electrode volume change and increased electrochemical resistance.An advanced Gr/Si hybrid anode with upper Gr and lower Si species layer structure design addresses the above challenges using photovoltaic waste silicon sources under high Si species content(17 wt%)and areal capacity(2.0 mA h cm^(-2))in Ah-level full pouch cells with a low negative/positive(N/P)ratio of 1.09.The cell shows stable cycling for 100 cycles at 0.3 C with an impressively low capacity decay rate of 0.0546%per cycle,outperforming most reported Gr-Si hybrid anodes.
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financially supported by the National Natural Science Foundation of China (No. 22225902, U22A20436, 22209185)National Key Research&Development Program of China (2022YFE0115900, 2023YFA1507101, 2021YFA1501500)+1 种基金the Self-deployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences (No. CXZX-2022-GH04, CXZX-2023-JQ08)Science and Technology Program of Fuzhou (2023-P-009)。
文摘Manganese-based chalcogenides have significant potential as anodes for sodium-ion batteries(SIBs) due to their high theoretical specific capacity, abundant natural reserves, and environmental friendliness. However, their application is hindered by poor cycling stability, resulting from severe volume changes during cycling and slow reaction kinetics due to their complex crystal structure. Here, an efficient and straightforward strategy was employed to in-situ encapsulate single-phase porous nanocubic MnS_(0.5)Se_(0.5) into carbon nanofibers using electrospinning and the hard template method, thus forming a necklace-like porous MnS_(0.5)Se_(0.5)-carbon nanofiber composite(MnS_(0.5)Se_(0.5)@N-CNF). The introduction of Se significantly impacts both the composition and microstructure of MnS_(0.5)Se_(0.5), including lattice distortion that generates additional defects, optimization of chemical bonds, and a nano-spatially confined design. In situ/ex-situ characterization and density functional theory calculations verified that this MnS_(0.5)Se_(0.5)@N-CNF allevi- ates the volume expansion and facilitates the transfer of Na+/electron. As expected, MnS_(0.5)Se_(0.5)@N-CNF anode demonstrates excellent sodium storage performance, characterized by high initial Coulombic efficiency(90.8%), high-rate capability(370.5 m Ahg^(-1) at 10 Ag^(-1)) and long durability(over 5000 cycles at 5 Ag^(-1)). The MnS_(0.5)Se_(0.5)@N-CNF//NVP@C full cell, assembled with MnS_(0.5)Se_(0.5)@N-CNF as anode and Na_(3)V_(2)(PO_4)_(3)@C as cathode, exhibits a high energy density of 254 Wh kg^(-1) can be provided. This work presents a novel strategy to optimize the design of anode materials through structural engineering and Se substitution, while also elucidating the underlying reaction mechanisms.
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.
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.
文摘As an emerging electrochemical energy storage technology,potassium-ion batteries(PIBs),which are considered a“beyond Li-ion”battery system,have attracted tremendous attention due to their potential for providing a high energy density,and having abundant resource,and a low cost.However,their commercialization is hindered by the lack of practical anode materials.Among various reported anodes,conventional carbon materials,including graphite,soft carbon,and hard carbon,have emerged as promising candidates because of their abundance,low cost,high conductivity,and tunable structures.However,these materials have problems such as a low initial Coulombic efficiency,significant volume expansion,and unsatisfactory cyclability and rate performance.Various strategies to solve these have been explored,including optimizing the interlayer spacing,structural design,surface coating,constructing a multifunctional framework,and forming composites.This review provides a comprehensive overview of the recent progress in conventional carbon anodes,highlighting structural design strategies,mechanisms for improving the electrochemical performance,and underscores the critical role of these materials in promoting the practical application of PIBs.
基金supported by the National Natural Science Foundation of China(22472023,22202037)the Jilin Province Science and Technology Development Program(20250102077JC)the Fundamental Research Funds for the Central Universities(2412024QD014,2412023QD019).
文摘Direct ethanol fuel cells(DEFCs)are a promising alternative to conventional energy sources,offering high energy density,environmental sustainability,and operational safety.Compared to methanol fuel cells,DEFCs exhibit lower toxicity and a more mature preparation process.Unlike hydrogen fuel cells,DEFCs provide superior storage and transport feasibility,as well as cost-effectiveness,significantly enhancing their commercial viability.However,the stable C-C bond in ethanol creates a high activation energy barrier,often resulting in incomplete electrooxidation.Current commercial platinum(Pt)-and palladium(Pd)-based catalysts demonstrate low C-C bond cleavage efficiency(<7.5%),severely limiting DEFC energy output and power density.Furthermore,high catalyst costs and insufficient activity impede large-scale commercialization.Recent advances in DEFC anode catalyst design have focused on optimizing material composition and elucidating catalytic mechanisms.This review systematically examines developments in ethanol electrooxidation catalysts over the past five years,highlighting strategies to improve C1 pathway selectivity and C-C bond activation.Key approaches,such as alloying,nanostructure engineering,and interfacial synergy effects,are discussed alongside their mechanistic implications.Finally,we outline current challenges and future prospects for DEFC commercialization.
文摘The advantages of sodium-ion batteries(SIBs)for large-scale energy storage are well known.Among possible anode materials,hard carbon(HC)stands out as the most viable commercial option because of its superior performance.However,there is still disagreement regarding the sodium storage mechanism in the low-voltage plateau region of HC anodes,and the structure-performance relationship between its complex multiscale micro/nanostructure and electrochemical behavior remains unclear.This paper summarizes current research progress and the major problems in understanding HC’s microstructure and sodium storage mechanism,and the relationship between them.Findings about a universal sodium storage mechanism in HC,including predictions about micropore-capacity relationships,and the opportunities and challenges for using HC anodes in commercial SIBs are presented.
