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
Practical application of lithium-sulfur(Li-S)batteries is hindered by the migration of lithium polysulfides(LiPSs),sluggish conversion kinetics,and anode instability.In these regards,with a novel strategy focusing on ...Practical application of lithium-sulfur(Li-S)batteries is hindered by the migration of lithium polysulfides(LiPSs),sluggish conversion kinetics,and anode instability.In these regards,with a novel strategy focusing on the selective elevation of d-orbitals,Mn/Fe dual-atom catalysts(MnFe DACs)embedded in Ndoped carbon frameworks are designed.Theoretical calculations reveal that energy levels of d_(z2),d_(zx),and d_(yz)orbitals participating in d-p hybridization are elevated closer to the Fermi level at both Mn and Fe sites,thereby reducing orbital occupancy in antibonding states.Consequently,these electronic features via the selective d-orbital elevation enable enhanced adsorption strength toward intermediate LiPSs and accelerate redox reaction during cell operation.Also,the MnFe DAC improves anode stability by regulating Li-ion flux with its lithiophilic active sites.Specifically,the cell equipped with MnFe DAC-modified separator maintains a capacity of 758.4 mAh g^(-1)after 400 cycles at 0.5 C.Notably,the cell demonstrates a high initial capacity of 822.7 mAh g^(-1)with only 0.047%decay rate over 1000 cycles at 1 C.Even under high sulfur-loading(5.0 mg cm^(-2))and low electrolyte-to-sulfur(E/S)ratio(6μL mg^(-1)),a high initial areal capacity of 4.94 m Ah cm^(-2)with 92.5%retention after 50 cycles at 0.1 C is achieved.This study provides guidelines on selective modulation of d-orbitals in DACs for high-performance Li-S batteries.展开更多
Arising from the increasing demand for electric vehicles(EVs),Ni-rich LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM,x+y+z=1,x≥0.8)cathode with greatly increased energy density are being researched and commercialized for lithium-ion ...Arising from the increasing demand for electric vehicles(EVs),Ni-rich LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM,x+y+z=1,x≥0.8)cathode with greatly increased energy density are being researched and commercialized for lithium-ion batteries(LIBs).However,parasitic crack formation during the discharge–charge cycling process remains as a major degradation mechanism.Cracking leads to increase in the specific surface area,loss of electrical contact between the primary particles,and facilitates liquid electrolyte infiltration into the cathode active material,accelerating capacity fading and decrease in lifetime.In contrast,Ni-rich NCM when used as a single crystal exhibits superior cycling performances due to its rigid mechanical property that resists cracking during long charge–discharge process even under harsh conditions.In this paper,we present comparative investigation between single crystal Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(SC)and polycrystalline Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(PC).The relatively improved cycling performances of SC are attributed to smaller anisotropic volume change,higher reversibility of phase transition,and resistance to crack formation.The superior properties of SC are demonstrated by in situ characterization and battery tests.Consequently,it is inferred from the results obtained that optimization of preparation conditions can be regarded as a key approach to obtain well crystallized and superior electrochemical performances.展开更多
Amidst the ever-growing interest in high-mass-loading Li battery electrodes,a persistent challenge has been the insufficient continuity of their ion/electron conduction pathways.Here,we propose cellulose elementary fi...Amidst the ever-growing interest in high-mass-loading Li battery electrodes,a persistent challenge has been the insufficient continuity of their ion/electron conduction pathways.Here,we propose cellulose elementary fibrils(CEFs)as a class of deagglomerated binder for high-mass-loading electrodes.Derived from natural wood,CEF represents the most fundamental unit of cellulose with nanoscale diameter.The preparation of the CEFs involves the modulation of intermolecular hydrogen bonding by the treatment with a proton acceptor and a hydrotropic agent.This elementary deagglomeration of the cellulose fibers increases surface area and anionic charge density,thus promoting uniform dispersion with carbon conductive additives and suppressing interfacial side reactions at electrodes.Consequently,a homogeneous redox reaction is achieved throughout the electrodes.The resulting CEF-based cathode(overlithiated layered oxide(OLO)is chosen as a benchmark electrode active material)exhibits a high areal-mass-loading(50 mg cm^(-2),equivalent to an areal capacity of 12.5 mAh cm^(-2))and a high specific energy density(445.4 Wh kg–1)of a cell,which far exceeds those of previously reported OLO cathodes.This study highlights the viability of the deagglomerated binder in enabling sustainable high-mass-loading electrodes that are difficult to achieve with conventional synthetic polymer binders.展开更多
We have entered the age of renewable energy revolution.Hence,energy-dense all-solid-state lithium metal batteries are now being actively researched as one of the most promising energy storage systems.However,they have...We have entered the age of renewable energy revolution.Hence,energy-dense all-solid-state lithium metal batteries are now being actively researched as one of the most promising energy storage systems.However,they have not yet been a silver bullet due to the dendrite formation and interfacial issue.Here,we introduce the hybrid polymer electrolyte via a novel solvent-free strategy as well as utilize a polymerization and gelation effect of cyanoethyl polyvinyl alcohol to achieve superior electrochemical performance.The hybrid polymer electrolyte,using cyanoethyl polyvinyl alcohol,demonstrates a stable artificial solid electrolyte interface layer,which suppresses the continuous decomposition of Li salts.Importantly,we also present the lithium-graphite composite anode to reach the super-highenergy-density anode materials.Taken together,these advancements represent a significant stride toward addressing the challenges associated with all-solid-state lithium metal batteries.展开更多
All-solid-state batteries(ASSBs)with sulfide-type solid electrolytes(SEs)are gaining significant attention due to their potential for the enhanced safety and energy density.In the slurry-coating process for ASSBs,nitr...All-solid-state batteries(ASSBs)with sulfide-type solid electrolytes(SEs)are gaining significant attention due to their potential for the enhanced safety and energy density.In the slurry-coating process for ASSBs,nitrile rubber(NBR)is primarily used as a binder due to its moderate solubility in non-polar solvents,which exhibites minimal chemical reactivity with sulfide SEs.However,the NBR binder,composed of butadiene and acrylonitrile units with differing polarities,exhibits different chemical compatibility depending on the subtle differences in polarity of solvents.Herein,we systematically demonstrate how the chemical compatibility of solvents with the NBR binder influences the performance of ASSBs.Anisole is found to activate the acrylonitrile units,inducing an elongated polymer chain configuration in the binder solution,which gives an opportunity to strongly interact with the solid components of the electrode and the current collector.Consequently,selecting anisole as a solvent for the NBR binder enables the fabrication of a mechanically robust graphite-silicon anode,allowing ASSBs to operate at a lower stacking pressure of 16 MPa.This approach achieves an initial capacity of 480 mAh g^(-1),significantly higher than the 390 mAh g^(-1)achieved with the NBR/toluene binder that has less chemical compatibility.Furthermore,internal stress variations during battery operation are monitored,revealing that the enhanced mechanical properties,achieved through acrylonitrile activation,effectively mitigate internal stress in the graphite/silicon composite anode.展开更多
With electric vehicles(EVs)emerging as a primary mode of transportation,ensuring their reliable operation in harsh environments is crucial.However,lithium-ion batteries(LIBs)suffer from severe polarization at low temp...With electric vehicles(EVs)emerging as a primary mode of transportation,ensuring their reliable operation in harsh environments is crucial.However,lithium-ion batteries(LIBs)suffer from severe polarization at low temperatures,limiting their operation in cold climates.In addition,difficulties in discovering new battery materials have highlighted a growing demand for innovative electrode designs that achieve high performance,even at low temperatu res.To address this issue,we prepared a thin,resistive,and patterned carbon interlayer on the anode current collector.This carbon-patterned layer(CPL)serves as a self-heating layer to efficiently elevate the entire cell temperature,thus improving the rate capability and cyclability at low temperatures while maintaining the performance at room temperature.Furthermore,we validated the versatile applicability of CPLs to large-format LIB cells through experimental studies and electrochemo-thermal multiphysics modeling and simulations,with the results confirming 11%capacity enhancement in 21,700 cylindrical cells at a 0.5C-rate and-24℃.We expect this electrode design to offer reliable power delivery in harsh climates,thereby potentially expanding the applications of LIBs.展开更多
The robust respective formations of a solid electrolyte interphase(SEI)and pillar at the surfaces of hard carbon and O3-type positive electrodes are the consequences of integrating Li PF_6 salt into a sodium-ion batte...The robust respective formations of a solid electrolyte interphase(SEI)and pillar at the surfaces of hard carbon and O3-type positive electrodes are the consequences of integrating Li PF_6 salt into a sodium-ion battery electrolyte that considerably strengthens both interfaces of positive and negative electrodes.The improvement of cycle performances due to the formation of highly passivating SEI on the hard carbon electrode is induced by the alternated solvation structure following the addition of Li salt,which inhibits sodium-ion and electron leakage from further electrolyte decomposition.The SEI with incorporated Li is less soluble than Na-based SEI,and the passivation ability of the initially formed SEI can thus be well preserved.Conversely,the gas evolution caused by oxygen release is reduced considerably by the marginal surface intercalation of Li ions at the surface of the O3-positive electrode.Additionally,the Li F layer that forms on the O3 surface diminishes additional deterioration of the electrolyte after formation.Compared with the fluoroethylene carbonate additive that is typically applied,a simultaneously strengthened interface yields major improvements in capacity retention.展开更多
Lithium metal anodes are promising for next-generation high-energy batteries,but their practical application is limited by safety issues arising from uncontrolled Li metal growth.To address these challenges,we report ...Lithium metal anodes are promising for next-generation high-energy batteries,but their practical application is limited by safety issues arising from uncontrolled Li metal growth.To address these challenges,we report a scalable approach to fabricate flexible,free-standing 3D carbon textiles derived from low-cost cellulose textiles,uniformly decorated with cobalt particles(Co@c-Textile).The work function difference between cobalt particles and carbon induces a redistribution of surface charge,enabling the synergistic combination of cobalt and defective carbon to enhance lithiophilicity and promote uniform Li growth through accelerate surface diffusion.Detailed analyses further reveal that lithium preferentially plates not directly on the cobalt particles,but on the adjacent carbon regions,eventually encapsulating the cobalt and growing uniformly across the carbon surface.As a result,the Co@c-Textile@Li anode exhibits prolonged and stable cycling over 700 h in symmetric cells,along with improved Li+transport kinetics.Furthermore,in full-cells with Li Fe PO_(4)(LFP)cathodes,it delivers over 90%capacity retention at both1C and 4C,and also demonstrates excellent stability under high-voltage conditions with Ni-rich cathodes.These findings clarify the role of transition metal/carbon composites in directing uniform Li plating and provide a viable strategy for designing advanced carbon-hosted Li metal anodes.展开更多
To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as wel...To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.展开更多
The electrolyte additive,lithium nitrate(LiNO_(3)),is widely recognized for suppressing dendritic lithium growth in anode-free lithium metal batteries,yet its stabilizing effect is transient,and the mechanistic origin...The electrolyte additive,lithium nitrate(LiNO_(3)),is widely recognized for suppressing dendritic lithium growth in anode-free lithium metal batteries,yet its stabilizing effect is transient,and the mechanistic origin of this limitation has remained unresolved.Here,we uncover the origin of this behavior through a comprehensive analysis driven by artifact/damage-free direct cryogenic transmission electron microscopy,which enabled one of the most chemically specific and morphologically intuitive visualizations to date of intact solid-electrolyte interphases(SEIs)and lithium growth.Contrary to conventional interpretations centered on nitrogen-rich or single-component SEIs,we reveal that LiNO_(3) rapidly generates lithium hydroxide(LiOH)and lithium oxide(Li_(2)O)rich interphases,whose complementary functions—ionic transport through LiOH and mechanical robustness from Li_(2)O—synergistically suppress whisker nucleation and favor compact,particle-like growth.Over the extended plating,however,depletion of these species in combination with crystallographically favored orientations drives the particle-towhisker transition,explaining why the effectiveness of LiNO_(3) is inherently limited.This direct mechanistic visualization resolves a long-standing ambiguity regarding the transient efficacy of LiNO_(3) and reframes its function from a nitrogen-driven mechanism to a synergistic dual oxygen-interphase framework.Beyond mechanistic clarification,these findings establish that continuous regeneration of LiOH and Li_(2)O is essential for stable lithium deposition,offering a design principle for the development of durable electrolytes in high-performance anode-free lithium metal batteries.展开更多
In this review,we discuss the electrochemical properties of Prussian blue(PB)for Na^(+)storage by combining structural engineering and electrolyte modifications.We integrated experimental data and density functional t...In this review,we discuss the electrochemical properties of Prussian blue(PB)for Na^(+)storage by combining structural engineering and electrolyte modifications.We integrated experimental data and density functional theory(DFT)in sodium-ion battery(SIB)research to refine the atomic arrangements and crystal lattices and introduce substitutions and dopants.These changes affect the lattice stability,intercalation,electronic and ionic conductivities,and electrochemical performance.We unraveled the intricate structure-electrochemical behavior relationship by combining experimental data with computational models,including first-principles calculations.This holistic approach identified techniques for optimizing PB and Prussian blue analog(PBA)structu ral properties for SIBs.We also discuss the tuning of electrolytes by systematically adjusting their composition,concentration,and additives using a combination of molecular dynamics(MD)simulations and DFT computations.Our review offers a comprehensive assessment of strategies for enhancing the electrochemical properties of PB and PBAs through structural engineering and electrolyte modifications,combining experimental insights with advanced computational simulations,and paving the way for next-generation energy storage systems.展开更多
Ni-rich layered oxides in lithium-ion batteries have problems with gas generation and electrochemical performance reduction due to residual lithium's reaction on the surface with the electrolyte.To address this is...Ni-rich layered oxides in lithium-ion batteries have problems with gas generation and electrochemical performance reduction due to residual lithium's reaction on the surface with the electrolyte.To address this issue,in this study,the Acid solvent evaporation(AsE)method has been proposed as a potential method to remove residual lithium while promoting the formation of a new LiNO_(3)-derived coating layer on the cathode surface.The reduction of residual lithium using the ASE method and the construction of a LiNO_(3)-derived coating layer suppresses gas evolution caused by the side effects of the electrolyte,improves electrochemical performance,and improves thermal stability by facilitating the smooth movement of lithium ions.Furthermore,the structural stability and resistance change due to the LiNO_(3)-derived coating layer effects is guaranteed through cycling and DCIR of the pouch cell.As a result,compared to Pristine,the capacity retention of coin cells increased by 8%after 100 cycles,and pouch cells increased by 25%after 160 cycles.In addition,after cycling the pouch cell,CO_(2) gas has significantly reduced by about 30%compared to Pristine using gas chromatography.The ASE method effectively forms a robust LiNO_(3)-derived coating layer on the cathode active material,which helps minimize electrolyte reactivity,suppress ,CO_(2) emissions,enhance surface structure stability,improve thermal stability,and improveoverallbatteryperformance.展开更多
Lithium-sulfur batteries(LSBs)have garnered attention from both academia and industry because they can achieve high energy densities(>400 Wh kg^(–1)),which are difficult to achieve in commercially available lithiu...Lithium-sulfur batteries(LSBs)have garnered attention from both academia and industry because they can achieve high energy densities(>400 Wh kg^(–1)),which are difficult to achieve in commercially available lithium-ion batteries.As a preparation step for practically utilizing LSBs,there is a problem,wherein battery cycle life rapidly reduces as the loading level of the sulfur cathode increases and the electrode area expands.In this study,a separator coated with boehmite on both sides of polyethylene(hereinafter denoted as boehmite separator)is incorporated into a high-loading Li-S pouch battery to suppress sudden capacity drops and achieve a longer cycle life.We explore a phenomenon by which inequality is generated in regions where an electrochemical reaction occurs in the sulfur cathode during the discharging and charging of a high-capacity Li-S pouch battery.The boehmite separator inhibits the accumulation of sulfur-related species on the surface of the sulfur cathode to induce an even reaction across the entire cathode and suppresses the degradation of the Li metal anode,allowing the pouch battery with an areal capacity of 8 mAh cm^(–2) to operate stably for 300 cycles.These results demonstrate the importance of customizing separators for the practical use of LSBs.展开更多
All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the unde...All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the undesirable side reactions of sulfide-based solid electrolytes(SEs),resulting in poor electrochemical properties with increased interfacial resistance.Here,we propose a wet chemical method rationally designed to achieve a conformal coating of lithium-indium chloride(Li_(3)InCl_(6))onto vapor-grown carbon fibers(VGCFs)as conductive agents.First,with the advantage of the Li_(3)InCl_(6) protective layer,use of VGCF@Li_(3)InCl_(6) leads to enhanced interfacial stability and improved electrochemical properties,including stable cycle performance.These results indicate that the Li_(3)InCl_(6) protective layer suppresses the unwanted reaction between Li_(6)PS_(5)Cl(LPSCl)and VGCF.Second,VGCF@Li_(3)InCl_(6) effectively promotes polytetrafluoroethylene(PTFE)fibrillization,leading to a homogeneous electrode microstructure.The uniform distribution of the cathode active material(CAM)in the electrode results in reduced charge-transfer resistance(R_(ct))and enhanced Li-ion kinetics.As a result,a full cell with the LiNi_(x)Mn_(y)Co_(z)O_(2)(NCM)/VGCF@Li_(3)InCl_(6) electrode shows an areal capacity of 7.7mAhcm^(−2) at 0.05 C and long-term cycle stability of 77.9%over 400 cycles at 0.2 C.This study offers a strategy for utilizing stable carbon-based conductive agents in sulfide-based ASSBs to enhance their electrochemical performance.展开更多
Energy harvesting storage hybrid devices have garnered considerable attention as self-rechargeable power sources for wireless and ubiquitous electronics.Triboelectric nanogenerators(TENGs),a common type of energy harv...Energy harvesting storage hybrid devices have garnered considerable attention as self-rechargeable power sources for wireless and ubiquitous electronics.Triboelectric nanogenerators(TENGs),a common type of energy harvester,generate alternating current-based,irregular short pulses,posing a challenge for storing the generated electrical energy in energy storage systems that typically operate with direct current(DC)-based low-frequency response.In this study,we propose a new strategy that leverages high-frequency response to develop efficient chargeable TENG-supercapacitor(SC)hybrid devices.A highfrequency SC was fabricated using hollow-structured MXene electrode materials,resulting in a twofold increase in the charging efficiency of the hybrid device compared to a control SC made with conventional carbon electrode materials.For a systematic understanding,the electrochemical interplay between the TENGs and SCs was investigated as a function of the frequency characteristics of SCs(f_(SC))and the output pulse duration of TENGs(Δt_(TENG)).Increasing the fSC·Δt_(TENG) enhanced the charging efficiency of the TENG-SC hybrid devices.This study highlights the importance of frequency response design in developing efficient chargeable TENG-SC hybrid devices.展开更多
All-solid-state batteries(ASSBs)are a promising next-generation energy storage solution due to their high energy density and enhanced safety.To achieve this,specialized electrode designs are required to efficiently en...All-solid-state batteries(ASSBs)are a promising next-generation energy storage solution due to their high energy density and enhanced safety.To achieve this,specialized electrode designs are required to efficiently enhance interparticle lithium-ion transport between solid components.In particular,for active materials with high specific capacity,such as silicon,their volume expansion and shrinkage must be carefully controlled to maintain mechanical interface stability,which is crucial for effective lithium-ion transport in ASSBs.Herein,we propose a mechanical stress-tolerant all-solid-state graphite/silicon electrode design to ensure stable lithium-ion diffusion at the interface through morphology control of active material particles.Plate-type graphite with a high surface-area-to-volume ratio is used to maximize the dispersion of silicon within the electrode.The carefully designed electrode can accommodate the volume changes of silicon,ensuring stable capacity retention over cycles.Additionally,spherical graphite is shown to contribute to improved rate performance by providing an efficient lithium-ion diffusion pathway within the electrode.Therefore,the synergistic effect of our electrode structure offers balanced electrochemical performance,providing practical insights into the mechano-electrochemical interactions essential for designing highperformance all-solid-state electrodes.展开更多
Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and of...Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and often conflicting requirements of the bulk electrolyte and the electrode-electrolyte interphase.Here,we present a weakly coordinating cationic polymer electrolyte(WCPE)specifically designed to regulate the Li^(+)coordination structure,thereby enabling fast-charging SSLMBs.The WCPE comprises an imidazolium-based polycationic matrix combined with a succinonitrile(SN)-based highconcentration electrolyte.Unlike conventional neutral polymer matrices,the polycationic matrix in the WCPE competes with Li^(+)for interactions with SN,weakening the original coordination between SN and Li^(+).This modulation of SN-Li^(+)interaction improves both Li^(+)conductivity of the WCPE(σ_(Li^(+))=1.29mS cm^(-1))and redox kinetics at the electrode-electrolyte interphase.Consequently,SSLMB cells(comprising LiFePO_(4)cathodes and Li-metal anodes)with the WCPE achieve fast-charging capability(reaching over 80%state of charge within 10 min),outperforming those of previously reported polymer electrolytebased SSLMBs.展开更多
The global transition to sustainable energy systems requires breakthroughs in electrochemical storage technologies that are not only safe but also resource efficient.Solid-state batteries(SSBs),which use superionic so...The global transition to sustainable energy systems requires breakthroughs in electrochemical storage technologies that are not only safe but also resource efficient.Solid-state batteries(SSBs),which use superionic solid electrolytes(SEs)instead of flammable liquid electrolytes,are at the forefront of this transformation.In general,SEs promise increased safety,access to high-voltage cathode and metal anode chemistries,and new avenues for circular design and recyclability.However,to reach their full potential,intertwined challenges related to ion transport,(electro)chemical stability,manufacturing,processing,and cost must be overcome.This 2026 roadmap on next-generation SEs for battery applications outlines new directions that will contribute to research in the field of SSBs over the next decade.It provides an overview of the current state of the art in sulfide-and halide-based SEs for Li and Na systems,examines post-Li/Na chemistries(K,Mg,and others),and highlights advances in hydroborate,fully reduced(irreducible),and compositionally complex(high-entropy)electrolytes,as well as glass-ceramic electrolytes.Beyond material innovation,the paper emphasizes the critical role of redox activity in SEs,scalable processing,high-throughput synthesis,and machine learning,as well as operando analytics and nuclear magnetic resonance spectroscopy to accelerate discoveries and gain a better understanding of structure–property relationships.Finally,the growing importance of recycling and circular design for ensuring sustainability is highlighted.By combining insights from chemistry,materials science,data(computational)science,and manufacturing,this article assumes that future SEs will progressively evolve from passive components to active design elements in high-energy-density electrochemical systems.The integration of multidisciplinary innovations will be crucial to realizing the potential of SSBs in practical technologies that power a decarbonized world.展开更多
Layered-type transition metal(TM)oxides are considered as one of the most promising cathodes for K-ion batteries because of the large theoretical gravimetric capacity by low molar mass.However,they suffer from severe ...Layered-type transition metal(TM)oxides are considered as one of the most promising cathodes for K-ion batteries because of the large theoretical gravimetric capacity by low molar mass.However,they suffer from severe structural change by de/intercalation and diffusion of K^(+)ions with large ionic size,which results in not only much lower reversible capacity than the theoretical capacity but also poor power capability.Thus,it is important to enhance the structural stability of the layered-type TM oxides for outstanding electrochemical behaviors under the K-ion battery system.Herein,it is investigated that the substitution of the appropriate Ti^(4+)contents enables a highly enlarged reversible capacity of P3-type KxCrO_(2) using combined studies of first-principles calculation and various experiments.Whereas the pristine P3-type KxCrO_(2) just exhibits the reversible capacity of∼120 mAh g^(−1) in the voltage range of 1.5-4.0 V(vs.K^(+)/K),the∼0.61 mol K^(+)corresponding to∼150 mAh g^(−1) can be reversible de/intercalated at the structure of P3-type K0.71[Cr_(0.75)Ti_(0.25)]O_(2) under the same conditions.Furthermore,even at the high current density of 788 mA g^(−1),the specific capacity of P3-type K0.71[Cr_(0.75)Ti_(0.25)]O_(2) is∼120 mAh g^(−1),which is∼81 times larger than that of the pristine P3-type KxCrO_(2).It is believed that this research can provide an effective strategy to improve the electrochemical performances of the cathode materials suffered by severe structural change that occurred during charge/discharge under not only K-ion battery system but also other rechargeable battery systems.展开更多
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.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(RS-2024-00355916)by the NRF grant funded by the Korea government(MSIT)(RS-2021-NR060090)by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea Government(MOTIE)(RS-2024-00419413,HRD Program for Industrial Innovation)。
文摘Practical application of lithium-sulfur(Li-S)batteries is hindered by the migration of lithium polysulfides(LiPSs),sluggish conversion kinetics,and anode instability.In these regards,with a novel strategy focusing on the selective elevation of d-orbitals,Mn/Fe dual-atom catalysts(MnFe DACs)embedded in Ndoped carbon frameworks are designed.Theoretical calculations reveal that energy levels of d_(z2),d_(zx),and d_(yz)orbitals participating in d-p hybridization are elevated closer to the Fermi level at both Mn and Fe sites,thereby reducing orbital occupancy in antibonding states.Consequently,these electronic features via the selective d-orbital elevation enable enhanced adsorption strength toward intermediate LiPSs and accelerate redox reaction during cell operation.Also,the MnFe DAC improves anode stability by regulating Li-ion flux with its lithiophilic active sites.Specifically,the cell equipped with MnFe DAC-modified separator maintains a capacity of 758.4 mAh g^(-1)after 400 cycles at 0.5 C.Notably,the cell demonstrates a high initial capacity of 822.7 mAh g^(-1)with only 0.047%decay rate over 1000 cycles at 1 C.Even under high sulfur-loading(5.0 mg cm^(-2))and low electrolyte-to-sulfur(E/S)ratio(6μL mg^(-1)),a high initial areal capacity of 4.94 m Ah cm^(-2)with 92.5%retention after 50 cycles at 0.1 C is achieved.This study provides guidelines on selective modulation of d-orbitals in DACs for high-performance Li-S batteries.
基金supported by the Technology Innovation Program(RS-2023-00256202Development of MLCB design and manufacturing process technology for board mounting)funded By the Ministry of Trade,Industry&Energy(MOTIE,Korea)+2 种基金supported by the Technology Innovation Program(or Industrial Strategic Technology Development Program-Public-private joint investment semiconductor R&D program(K-CHIPS)to foster high-quality human resources)(RS-2023-00237003,High selectivity etching technology using cryoetch)funded By the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by 2022 Research Grant from Kangwon National University(No.202203080001)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(RS-2023-00280367).
文摘Arising from the increasing demand for electric vehicles(EVs),Ni-rich LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM,x+y+z=1,x≥0.8)cathode with greatly increased energy density are being researched and commercialized for lithium-ion batteries(LIBs).However,parasitic crack formation during the discharge–charge cycling process remains as a major degradation mechanism.Cracking leads to increase in the specific surface area,loss of electrical contact between the primary particles,and facilitates liquid electrolyte infiltration into the cathode active material,accelerating capacity fading and decrease in lifetime.In contrast,Ni-rich NCM when used as a single crystal exhibits superior cycling performances due to its rigid mechanical property that resists cracking during long charge–discharge process even under harsh conditions.In this paper,we present comparative investigation between single crystal Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(SC)and polycrystalline Ni-rich LiNi_(0.92)Co_(0.04)Mn_(0.04)O_(2)(PC).The relatively improved cycling performances of SC are attributed to smaller anisotropic volume change,higher reversibility of phase transition,and resistance to crack formation.The superior properties of SC are demonstrated by in situ characterization and battery tests.Consequently,it is inferred from the results obtained that optimization of preparation conditions can be regarded as a key approach to obtain well crystallized and superior electrochemical performances.
基金supported by the Institute of Civil Military Technology Cooperation funded by the Defense Acquisition Program Administration and Ministry of Trade,Industry and Energy of Korean government under grant No 23-CM-AI-08.
文摘Amidst the ever-growing interest in high-mass-loading Li battery electrodes,a persistent challenge has been the insufficient continuity of their ion/electron conduction pathways.Here,we propose cellulose elementary fibrils(CEFs)as a class of deagglomerated binder for high-mass-loading electrodes.Derived from natural wood,CEF represents the most fundamental unit of cellulose with nanoscale diameter.The preparation of the CEFs involves the modulation of intermolecular hydrogen bonding by the treatment with a proton acceptor and a hydrotropic agent.This elementary deagglomeration of the cellulose fibers increases surface area and anionic charge density,thus promoting uniform dispersion with carbon conductive additives and suppressing interfacial side reactions at electrodes.Consequently,a homogeneous redox reaction is achieved throughout the electrodes.The resulting CEF-based cathode(overlithiated layered oxide(OLO)is chosen as a benchmark electrode active material)exhibits a high areal-mass-loading(50 mg cm^(-2),equivalent to an areal capacity of 12.5 mAh cm^(-2))and a high specific energy density(445.4 Wh kg–1)of a cell,which far exceeds those of previously reported OLO cathodes.This study highlights the viability of the deagglomerated binder in enabling sustainable high-mass-loading electrodes that are difficult to achieve with conventional synthetic polymer binders.
基金supported by the Technology Innovation Program(RS-2023-00256202,Development of MLCB design and manufacturing process technology for board mounting)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘We have entered the age of renewable energy revolution.Hence,energy-dense all-solid-state lithium metal batteries are now being actively researched as one of the most promising energy storage systems.However,they have not yet been a silver bullet due to the dendrite formation and interfacial issue.Here,we introduce the hybrid polymer electrolyte via a novel solvent-free strategy as well as utilize a polymerization and gelation effect of cyanoethyl polyvinyl alcohol to achieve superior electrochemical performance.The hybrid polymer electrolyte,using cyanoethyl polyvinyl alcohol,demonstrates a stable artificial solid electrolyte interface layer,which suppresses the continuous decomposition of Li salts.Importantly,we also present the lithium-graphite composite anode to reach the super-highenergy-density anode materials.Taken together,these advancements represent a significant stride toward addressing the challenges associated with all-solid-state lithium metal batteries.
基金supported by the Technology Innovation Program(00404166,Development of thin-film coating current collector and aqueous binder to enhance the adhesion and conductivity properties on the silicon-rich anode)funded By the Ministry of Trade,Industry&Energy(MOTIE,Korea),the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.2710024139)the Institute of Civil Military Technology Cooperation funded by the Defense Acquisition Program Administration and Ministry of Trade,Industry and Energy of Korean government under grant No.22-CM-FC-20。
文摘All-solid-state batteries(ASSBs)with sulfide-type solid electrolytes(SEs)are gaining significant attention due to their potential for the enhanced safety and energy density.In the slurry-coating process for ASSBs,nitrile rubber(NBR)is primarily used as a binder due to its moderate solubility in non-polar solvents,which exhibites minimal chemical reactivity with sulfide SEs.However,the NBR binder,composed of butadiene and acrylonitrile units with differing polarities,exhibits different chemical compatibility depending on the subtle differences in polarity of solvents.Herein,we systematically demonstrate how the chemical compatibility of solvents with the NBR binder influences the performance of ASSBs.Anisole is found to activate the acrylonitrile units,inducing an elongated polymer chain configuration in the binder solution,which gives an opportunity to strongly interact with the solid components of the electrode and the current collector.Consequently,selecting anisole as a solvent for the NBR binder enables the fabrication of a mechanically robust graphite-silicon anode,allowing ASSBs to operate at a lower stacking pressure of 16 MPa.This approach achieves an initial capacity of 480 mAh g^(-1),significantly higher than the 390 mAh g^(-1)achieved with the NBR/toluene binder that has less chemical compatibility.Furthermore,internal stress variations during battery operation are monitored,revealing that the enhanced mechanical properties,achieved through acrylonitrile activation,effectively mitigate internal stress in the graphite/silicon composite anode.
基金financially supported by the Institute of Civil Military Technology Cooperation funded by the Defense Acquisition Program Administration and Ministry of Trade,Industry and Energy of Korean government under grant No.22-CM-FC-20the support from the DGIST Supercomputing and Bigdata Center。
文摘With electric vehicles(EVs)emerging as a primary mode of transportation,ensuring their reliable operation in harsh environments is crucial.However,lithium-ion batteries(LIBs)suffer from severe polarization at low temperatures,limiting their operation in cold climates.In addition,difficulties in discovering new battery materials have highlighted a growing demand for innovative electrode designs that achieve high performance,even at low temperatu res.To address this issue,we prepared a thin,resistive,and patterned carbon interlayer on the anode current collector.This carbon-patterned layer(CPL)serves as a self-heating layer to efficiently elevate the entire cell temperature,thus improving the rate capability and cyclability at low temperatures while maintaining the performance at room temperature.Furthermore,we validated the versatile applicability of CPLs to large-format LIB cells through experimental studies and electrochemo-thermal multiphysics modeling and simulations,with the results confirming 11%capacity enhancement in 21,700 cylindrical cells at a 0.5C-rate and-24℃.We expect this electrode design to offer reliable power delivery in harsh climates,thereby potentially expanding the applications of LIBs.
基金supported by Ministry of TradeIndustry&Energy/Korea Evaluation Institute of Industrial Technology(MOTIE/KEIT)(No.RS-2024-00406080)an Institute of Information&Communications Technology Planning&Evaluation(IITP)grant funded by the Korean government(MSIT)(RS-2023-00221723)。
文摘The robust respective formations of a solid electrolyte interphase(SEI)and pillar at the surfaces of hard carbon and O3-type positive electrodes are the consequences of integrating Li PF_6 salt into a sodium-ion battery electrolyte that considerably strengthens both interfaces of positive and negative electrodes.The improvement of cycle performances due to the formation of highly passivating SEI on the hard carbon electrode is induced by the alternated solvation structure following the addition of Li salt,which inhibits sodium-ion and electron leakage from further electrolyte decomposition.The SEI with incorporated Li is less soluble than Na-based SEI,and the passivation ability of the initially formed SEI can thus be well preserved.Conversely,the gas evolution caused by oxygen release is reduced considerably by the marginal surface intercalation of Li ions at the surface of the O3-positive electrode.Additionally,the Li F layer that forms on the O3 surface diminishes additional deterioration of the electrolyte after formation.Compared with the fluoroethylene carbonate additive that is typically applied,a simultaneously strengthened interface yields major improvements in capacity retention.
基金supported by’regional innovation mega project’program through the Korea Innovation Foundation funded by Ministry of Science and ICT(2710033465)the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(RS-2025-25441256)。
文摘Lithium metal anodes are promising for next-generation high-energy batteries,but their practical application is limited by safety issues arising from uncontrolled Li metal growth.To address these challenges,we report a scalable approach to fabricate flexible,free-standing 3D carbon textiles derived from low-cost cellulose textiles,uniformly decorated with cobalt particles(Co@c-Textile).The work function difference between cobalt particles and carbon induces a redistribution of surface charge,enabling the synergistic combination of cobalt and defective carbon to enhance lithiophilicity and promote uniform Li growth through accelerate surface diffusion.Detailed analyses further reveal that lithium preferentially plates not directly on the cobalt particles,but on the adjacent carbon regions,eventually encapsulating the cobalt and growing uniformly across the carbon surface.As a result,the Co@c-Textile@Li anode exhibits prolonged and stable cycling over 700 h in symmetric cells,along with improved Li+transport kinetics.Furthermore,in full-cells with Li Fe PO_(4)(LFP)cathodes,it delivers over 90%capacity retention at both1C and 4C,and also demonstrates excellent stability under high-voltage conditions with Ni-rich cathodes.These findings clarify the role of transition metal/carbon composites in directing uniform Li plating and provide a viable strategy for designing advanced carbon-hosted Li metal anodes.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.NRF-2021M3H4A1A02048529)the Ministry of Trade,Industry and Energy(MOTIE)of the Korean government under grant No.RS-2022-00155854support from the DGIST Supercomputing and Big Data Center.
文摘To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS-2024-00406724(50%)RS-2023-00222411,RS-2025-24533073)+2 种基金the Korea Basic Science Institute(National research Facilities and Equipment Center)grant funded by the Korea government(MOE)(RS-2024-00436346)the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea government(MOTIE)(RS-2024-00417730,HRD Program for Industrial Innovation)the research fund of Hanyang University(HY-202100000003295)。
文摘The electrolyte additive,lithium nitrate(LiNO_(3)),is widely recognized for suppressing dendritic lithium growth in anode-free lithium metal batteries,yet its stabilizing effect is transient,and the mechanistic origin of this limitation has remained unresolved.Here,we uncover the origin of this behavior through a comprehensive analysis driven by artifact/damage-free direct cryogenic transmission electron microscopy,which enabled one of the most chemically specific and morphologically intuitive visualizations to date of intact solid-electrolyte interphases(SEIs)and lithium growth.Contrary to conventional interpretations centered on nitrogen-rich or single-component SEIs,we reveal that LiNO_(3) rapidly generates lithium hydroxide(LiOH)and lithium oxide(Li_(2)O)rich interphases,whose complementary functions—ionic transport through LiOH and mechanical robustness from Li_(2)O—synergistically suppress whisker nucleation and favor compact,particle-like growth.Over the extended plating,however,depletion of these species in combination with crystallographically favored orientations drives the particle-towhisker transition,explaining why the effectiveness of LiNO_(3) is inherently limited.This direct mechanistic visualization resolves a long-standing ambiguity regarding the transient efficacy of LiNO_(3) and reframes its function from a nitrogen-driven mechanism to a synergistic dual oxygen-interphase framework.Beyond mechanistic clarification,these findings establish that continuous regeneration of LiOH and Li_(2)O is essential for stable lithium deposition,offering a design principle for the development of durable electrolytes in high-performance anode-free lithium metal batteries.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(NRF-2022R1C1C1011058)。
文摘In this review,we discuss the electrochemical properties of Prussian blue(PB)for Na^(+)storage by combining structural engineering and electrolyte modifications.We integrated experimental data and density functional theory(DFT)in sodium-ion battery(SIB)research to refine the atomic arrangements and crystal lattices and introduce substitutions and dopants.These changes affect the lattice stability,intercalation,electronic and ionic conductivities,and electrochemical performance.We unraveled the intricate structure-electrochemical behavior relationship by combining experimental data with computational models,including first-principles calculations.This holistic approach identified techniques for optimizing PB and Prussian blue analog(PBA)structu ral properties for SIBs.We also discuss the tuning of electrolytes by systematically adjusting their composition,concentration,and additives using a combination of molecular dynamics(MD)simulations and DFT computations.Our review offers a comprehensive assessment of strategies for enhancing the electrochemical properties of PB and PBAs through structural engineering and electrolyte modifications,combining experimental insights with advanced computational simulations,and paving the way for next-generation energy storage systems.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIP)(2021R1F1A1055946)SolarEdge Technologies Korea(GCU-202203070002)。
文摘Ni-rich layered oxides in lithium-ion batteries have problems with gas generation and electrochemical performance reduction due to residual lithium's reaction on the surface with the electrolyte.To address this issue,in this study,the Acid solvent evaporation(AsE)method has been proposed as a potential method to remove residual lithium while promoting the formation of a new LiNO_(3)-derived coating layer on the cathode surface.The reduction of residual lithium using the ASE method and the construction of a LiNO_(3)-derived coating layer suppresses gas evolution caused by the side effects of the electrolyte,improves electrochemical performance,and improves thermal stability by facilitating the smooth movement of lithium ions.Furthermore,the structural stability and resistance change due to the LiNO_(3)-derived coating layer effects is guaranteed through cycling and DCIR of the pouch cell.As a result,compared to Pristine,the capacity retention of coin cells increased by 8%after 100 cycles,and pouch cells increased by 25%after 160 cycles.In addition,after cycling the pouch cell,CO_(2) gas has significantly reduced by about 30%compared to Pristine using gas chromatography.The ASE method effectively forms a robust LiNO_(3)-derived coating layer on the cathode active material,which helps minimize electrolyte reactivity,suppress ,CO_(2) emissions,enhance surface structure stability,improve thermal stability,and improveoverallbatteryperformance.
基金This work was supported by a Human ResourcesDevelopment program(No.20214000000320)as part ofa Korea Institute of Energy'Technology Evaluation andPlanning(KETEP)grant,funded by the Ministry of Trade,Industry,and Energy of the Korean government.
文摘Lithium-sulfur batteries(LSBs)have garnered attention from both academia and industry because they can achieve high energy densities(>400 Wh kg^(–1)),which are difficult to achieve in commercially available lithium-ion batteries.As a preparation step for practically utilizing LSBs,there is a problem,wherein battery cycle life rapidly reduces as the loading level of the sulfur cathode increases and the electrode area expands.In this study,a separator coated with boehmite on both sides of polyethylene(hereinafter denoted as boehmite separator)is incorporated into a high-loading Li-S pouch battery to suppress sudden capacity drops and achieve a longer cycle life.We explore a phenomenon by which inequality is generated in regions where an electrochemical reaction occurs in the sulfur cathode during the discharging and charging of a high-capacity Li-S pouch battery.The boehmite separator inhibits the accumulation of sulfur-related species on the surface of the sulfur cathode to induce an even reaction across the entire cathode and suppresses the degradation of the Li metal anode,allowing the pouch battery with an areal capacity of 8 mAh cm^(–2) to operate stably for 300 cycles.These results demonstrate the importance of customizing separators for the practical use of LSBs.
基金supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(RS-2024-00417730,HRD Program for Industrial Innovation)supported by the Technology Innovation Program(or Industrial Strategic Technology Development Program-Materials&Components Technology Development Program)(20024261),Development of thick film electrodes and cell manufacturing technology for a high-performance lithium iron phosphate battery with energy density of over 200 Wh/kg was funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the undesirable side reactions of sulfide-based solid electrolytes(SEs),resulting in poor electrochemical properties with increased interfacial resistance.Here,we propose a wet chemical method rationally designed to achieve a conformal coating of lithium-indium chloride(Li_(3)InCl_(6))onto vapor-grown carbon fibers(VGCFs)as conductive agents.First,with the advantage of the Li_(3)InCl_(6) protective layer,use of VGCF@Li_(3)InCl_(6) leads to enhanced interfacial stability and improved electrochemical properties,including stable cycle performance.These results indicate that the Li_(3)InCl_(6) protective layer suppresses the unwanted reaction between Li_(6)PS_(5)Cl(LPSCl)and VGCF.Second,VGCF@Li_(3)InCl_(6) effectively promotes polytetrafluoroethylene(PTFE)fibrillization,leading to a homogeneous electrode microstructure.The uniform distribution of the cathode active material(CAM)in the electrode results in reduced charge-transfer resistance(R_(ct))and enhanced Li-ion kinetics.As a result,a full cell with the LiNi_(x)Mn_(y)Co_(z)O_(2)(NCM)/VGCF@Li_(3)InCl_(6) electrode shows an areal capacity of 7.7mAhcm^(−2) at 0.05 C and long-term cycle stability of 77.9%over 400 cycles at 0.2 C.This study offers a strategy for utilizing stable carbon-based conductive agents in sulfide-based ASSBs to enhance their electrochemical performance.
基金supported by the Basic Science Research Program(RS-2024-00344021 and RS-2023-00261543)through the National Research Foundation of Korea(NRF)grant by the Korean Government(MSIT)the National Research Council of Science&Technology(NST)grant by the Korea Government(MSIT)(GTL24011-000)Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea Government(MOTIE)(RS-2024-00420590,HRD Program for Industrial Innovation).
文摘Energy harvesting storage hybrid devices have garnered considerable attention as self-rechargeable power sources for wireless and ubiquitous electronics.Triboelectric nanogenerators(TENGs),a common type of energy harvester,generate alternating current-based,irregular short pulses,posing a challenge for storing the generated electrical energy in energy storage systems that typically operate with direct current(DC)-based low-frequency response.In this study,we propose a new strategy that leverages high-frequency response to develop efficient chargeable TENG-supercapacitor(SC)hybrid devices.A highfrequency SC was fabricated using hollow-structured MXene electrode materials,resulting in a twofold increase in the charging efficiency of the hybrid device compared to a control SC made with conventional carbon electrode materials.For a systematic understanding,the electrochemical interplay between the TENGs and SCs was investigated as a function of the frequency characteristics of SCs(f_(SC))and the output pulse duration of TENGs(Δt_(TENG)).Increasing the fSC·Δt_(TENG) enhanced the charging efficiency of the TENG-SC hybrid devices.This study highlights the importance of frequency response design in developing efficient chargeable TENG-SC hybrid devices.
基金supported by the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.GTL24011-000)the National Research Foundation of Korea(NRF2022M3J1A1085396)the Technology Innovation Program(RS-2024-00445442)through the Korea Planning&Evaluation Institute of Industrial Technology(KEIT)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘All-solid-state batteries(ASSBs)are a promising next-generation energy storage solution due to their high energy density and enhanced safety.To achieve this,specialized electrode designs are required to efficiently enhance interparticle lithium-ion transport between solid components.In particular,for active materials with high specific capacity,such as silicon,their volume expansion and shrinkage must be carefully controlled to maintain mechanical interface stability,which is crucial for effective lithium-ion transport in ASSBs.Herein,we propose a mechanical stress-tolerant all-solid-state graphite/silicon electrode design to ensure stable lithium-ion diffusion at the interface through morphology control of active material particles.Plate-type graphite with a high surface-area-to-volume ratio is used to maximize the dispersion of silicon within the electrode.The carefully designed electrode can accommodate the volume changes of silicon,ensuring stable capacity retention over cycles.Additionally,spherical graphite is shown to contribute to improved rate performance by providing an efficient lithium-ion diffusion pathway within the electrode.Therefore,the synergistic effect of our electrode structure offers balanced electrochemical performance,providing practical insights into the mechano-electrochemical interactions essential for designing highperformance all-solid-state electrodes.
基金supported by the Basic Science Research Program(RS-2024-00344021,RS-2023-00261543,and RS-202300257666)through the National Research Foundation of Korea(NRF),the National Research Council of Science(000)Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea Government(MOTIE)(RS-2024-00420590,HRD Program for Industrial Innovation)The computational resources were provided by KITSI(KSC-2024-CRE-0143)。
文摘Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and often conflicting requirements of the bulk electrolyte and the electrode-electrolyte interphase.Here,we present a weakly coordinating cationic polymer electrolyte(WCPE)specifically designed to regulate the Li^(+)coordination structure,thereby enabling fast-charging SSLMBs.The WCPE comprises an imidazolium-based polycationic matrix combined with a succinonitrile(SN)-based highconcentration electrolyte.Unlike conventional neutral polymer matrices,the polycationic matrix in the WCPE competes with Li^(+)for interactions with SN,weakening the original coordination between SN and Li^(+).This modulation of SN-Li^(+)interaction improves both Li^(+)conductivity of the WCPE(σ_(Li^(+))=1.29mS cm^(-1))and redox kinetics at the electrode-electrolyte interphase.Consequently,SSLMB cells(comprising LiFePO_(4)cathodes and Li-metal anodes)with the WCPE achieve fast-charging capability(reaching over 80%state of charge within 10 min),outperforming those of previously reported polymer electrolytebased SSLMBs.
基金Financial support from the Deutsche Forschungsgemeinschaft(DFG)is highly appreciated(former Research Unit 1277(molife)).
文摘The global transition to sustainable energy systems requires breakthroughs in electrochemical storage technologies that are not only safe but also resource efficient.Solid-state batteries(SSBs),which use superionic solid electrolytes(SEs)instead of flammable liquid electrolytes,are at the forefront of this transformation.In general,SEs promise increased safety,access to high-voltage cathode and metal anode chemistries,and new avenues for circular design and recyclability.However,to reach their full potential,intertwined challenges related to ion transport,(electro)chemical stability,manufacturing,processing,and cost must be overcome.This 2026 roadmap on next-generation SEs for battery applications outlines new directions that will contribute to research in the field of SSBs over the next decade.It provides an overview of the current state of the art in sulfide-and halide-based SEs for Li and Na systems,examines post-Li/Na chemistries(K,Mg,and others),and highlights advances in hydroborate,fully reduced(irreducible),and compositionally complex(high-entropy)electrolytes,as well as glass-ceramic electrolytes.Beyond material innovation,the paper emphasizes the critical role of redox activity in SEs,scalable processing,high-throughput synthesis,and machine learning,as well as operando analytics and nuclear magnetic resonance spectroscopy to accelerate discoveries and gain a better understanding of structure–property relationships.Finally,the growing importance of recycling and circular design for ensuring sustainability is highlighted.By combining insights from chemistry,materials science,data(computational)science,and manufacturing,this article assumes that future SEs will progressively evolve from passive components to active design elements in high-energy-density electrochemical systems.The integration of multidisciplinary innovations will be crucial to realizing the potential of SSBs in practical technologies that power a decarbonized world.
基金Korea Institute of Materials Science,Grant/Award Number:PNK9370National Research Foundation of Korea,Grant/Award Numbers:NRF-2021R1A2C1014280,NRF-2022R1C1C1011058,NRF-2022M3H446401037201Korea Institute of Science and Technology,Grant/Award Number:2E32581-23-092。
文摘Layered-type transition metal(TM)oxides are considered as one of the most promising cathodes for K-ion batteries because of the large theoretical gravimetric capacity by low molar mass.However,they suffer from severe structural change by de/intercalation and diffusion of K^(+)ions with large ionic size,which results in not only much lower reversible capacity than the theoretical capacity but also poor power capability.Thus,it is important to enhance the structural stability of the layered-type TM oxides for outstanding electrochemical behaviors under the K-ion battery system.Herein,it is investigated that the substitution of the appropriate Ti^(4+)contents enables a highly enlarged reversible capacity of P3-type KxCrO_(2) using combined studies of first-principles calculation and various experiments.Whereas the pristine P3-type KxCrO_(2) just exhibits the reversible capacity of∼120 mAh g^(−1) in the voltage range of 1.5-4.0 V(vs.K^(+)/K),the∼0.61 mol K^(+)corresponding to∼150 mAh g^(−1) can be reversible de/intercalated at the structure of P3-type K0.71[Cr_(0.75)Ti_(0.25)]O_(2) under the same conditions.Furthermore,even at the high current density of 788 mA g^(−1),the specific capacity of P3-type K0.71[Cr_(0.75)Ti_(0.25)]O_(2) is∼120 mAh g^(−1),which is∼81 times larger than that of the pristine P3-type KxCrO_(2).It is believed that this research can provide an effective strategy to improve the electrochemical performances of the cathode materials suffered by severe structural change that occurred during charge/discharge under not only K-ion battery system but also other rechargeable battery systems.
