Lithium(Li)metal is regarded as a promising anode candidate for high-energy-density rechargeable batteries.Nevertheless,Li metal is highly reactive against electrolytes,leading to rapid decay of active Li metal reserv...Lithium(Li)metal is regarded as a promising anode candidate for high-energy-density rechargeable batteries.Nevertheless,Li metal is highly reactive against electrolytes,leading to rapid decay of active Li metal reservoir.Here,alloying Li metal with low-content magnesium(Mg)is proposed to mitigate the reaction kinetics between Li metal anodes and electrolytes.Mg atoms enter the lattice of Li atoms,forming solid solution due to the low amount(5 wt%)of Mg.Mg atoms mainly concentrate near the surface of Mg-alloyed Li metal anodes.The reactivity of Mg-alloyed Li metal is mitigated kinetically,which results from the electron transfer from Li to Mg atoms due to the electronegativity difference.Based on quantitative experimental analysis,the consumption rate of active Li and electrolytes is decreased by using Mgalloyed Li metal anodes,which increases the cycle life of Li metal batteries under demanding conditions.Further,a pouch cell(1.25 Ah)with Mg-alloyed Li metal anodes delivers an energy density of 340 Wh kg^(-1)and a cycle life of 100 cycles.This work inspires the strategy of modifying Li metal anodes to kinetically mitigate the side reactions with electrolytes.展开更多
Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,i...Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial application.Herein,we report a liquid metal-coated lithium metal(LM@Li)anode strategy to improve the contact between lithium metal and a Li6PS5Cl inorganic electrolyte.The LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2mA cm^(-2) and a significantly higher critical current density of 9.8 mAcm^(-2) at 25°C.In addition,a full battery assembled with a high-capacity composite LiNbO3@-LiNi_(0.7)Co_(0.2)Mn_(0.1)O_(2)(LNO@NCM721)cathode shows stable cycling performance.Experimental and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.展开更多
The dendrite growth that results from the slow electrode process kinetics prevents the lithium(Li) metal anode from being used in practical applications. Here, full-chain enhanced ion transport for stabilizing Li meta...The dendrite growth that results from the slow electrode process kinetics prevents the lithium(Li) metal anode from being used in practical applications. Here, full-chain enhanced ion transport for stabilizing Li metal anodes is proposed. Experimental and theoretical studies confirm that full-chain enhanced ion transport(electrocrystallization, mass transport in the electrolyte and diffusion in solid electrolyte interphase) under magnetoelectrochemistry contributes to a homogeneous, dense, and dendrite-free morphology. Specifically, the enhanced electrocrystallization behavior promotes the Li nucleation;the enhanced mass transport in the electrolyte alleviates the ion concentration gradient at the electrode surface, which helps to inhibit dendrite growth;and the enhanced diffusion in the solid electrolyte interphase further homogenizes the Li deposition behavior, obtaining regular and uniform Li particles.Consequently, the Li metal anode has exceptional cycling stability in both symmetric and full cells,and the pouch cell performs long cycles(170 cycles) in practice evaluation. This work advances fundamental knowledge of the magneto-dendrite effect and offers a new perspective on stabilizing metal anodes.展开更多
Solid-state lithium-metal batteries,with their high theoretical energy density and safety,are highly promising as a next-generation battery contender.Among the alternatives proposed as solid-state electrolyte,lithium-...Solid-state lithium-metal batteries,with their high theoretical energy density and safety,are highly promising as a next-generation battery contender.Among the alternatives proposed as solid-state electrolyte,lithium-rich anti-perovskite(Li RAP)materials have drawn the most interest because of high theoretical Li^(+)conductivity,low cost and easy processing.Although solid-state electrolytes are believed to have the potential to physically inhibit the lithium dendrite growth,lithium-metal batteries still suffer from the lithium dendrite growth and thereafter the short circuiting.The voids in practical Li RAP pellets are considered as the root cause.Herein,we show that reducing the voids can effectively suppress the lithium dendrite growth.The voids in the pellet resulted in an irregular Li^(+)flux distribution and a poor interfacial contact with lithium metal anode;and hence the ununiform lithium dendrites.Consequently,the lithium-metal symmetric cell with void-reduced Li_(2)OHCl-HT pellet was able to display excellent cycling performance(750 h at 0.4 m A cm^(-2))and stability at high current density(0.8 m A cm^(-2)for 120 h).This study provides not only experimental evidence for the impact of the voids in Li RAP pellets on the lithium dendrite growth,but also a rational pellet fabrication approach to suppress the lithium dendrite growth.展开更多
Lithium(Li)metal anodes have attracted extensive attention due to their ultrahigh theoretical capacity and low potential.However,the uneven deposition of Li near the unstable electrode/electrolyte interfaces leads to ...Lithium(Li)metal anodes have attracted extensive attention due to their ultrahigh theoretical capacity and low potential.However,the uneven deposition of Li near the unstable electrode/electrolyte interfaces leads to the growth of Li dendrites and the degradation of active electrodes.Herein,we directly fluorinate alkyne-containing conjugated microporous polymers(ACMPs)microspheres with fluorine gas(F_(2))to introduce a novel fluorinated interlayer as an interfacial stabilizer in lithium metal batteries.Using density functional theory methods,it is found that as-prepared fluorinated ACMP(FACMP)has abundant partially ionic C–F bonds.The C–F bonds with electrochemical lability yield remarkable lithiophilicity during cycling.The in situ reactions between the active C–F bonds and Li ions enable transfer of lithium fluoride microcrystals to the solid electrolyte interphase(SEI)layers,guaranteeing effective ionic distribution and smooth Li deposition.Consequently,Li metal electrodes with the fluorinated interlayers demonstrate excellent cycling performances in both half-batteries and full cells with a lithium bis(trifluoromethanesulfonyl)imide electrolyte as well as a nonfluorinated lithium bis(oxalate)borate electrolyte system.This strategy is highly significant in customizable SEI layers to stabilize electrode interfaces and ensure high utilization of Li metal anodes,especially in a nonfluorinated electrolyte.展开更多
Ultrathin and air-stable Li metal anodes hold great promise toward high-energy and high-safety Li metal batteries(LMBs).However,the application of LMBs is technically impeded by existing Li metal anodes with large thi...Ultrathin and air-stable Li metal anodes hold great promise toward high-energy and high-safety Li metal batteries(LMBs).However,the application of LMBs is technically impeded by existing Li metal anodes with large thickness,high reactivity,and poor performance.Here,we developed a novel and scalable approach for the construction of a 10-μm-thick flexible and air-stable Li metal anode by conformally encapsulating Li within a multifunctional VN film.Specifically,the highly lithiophilic VN layer guides a uniform deposition of Li,while abundant and multilevel pores arising from assembly of ultrathin nanosheets enable a spatially confined immersion of metallic Li,thus ensuring an ultrathin and sandwiched Li anode.More impressively,the strong hydrophobicity of VN surface can effectively improve the stability of anode to humid air,whereas the highly conductive framework greatly boosts charge transfer dynamics and enhances Li utilization and high-rate capability.Benefiting from such fascinating features,the constructed Li-VN anode exhibits ultrastable cycling stability in both ether(2500 h)and carbonate(900 h)electrolytes,respectively.Moreover,even exposed to ambient air for 12 h,the anode still can retain~78%capacity,demonstrating excellent air-defendable capability.This work affords a promising strategy for fabricating high-performance,high-safety,and low-cost LMBs.展开更多
Lithium metal anode(LMA) is a promising candidate for achieving next-generation high-energy-density batteries due to its ultrahigh theoretical capacity and most negative electrochemical potential. However, the practic...Lithium metal anode(LMA) is a promising candidate for achieving next-generation high-energy-density batteries due to its ultrahigh theoretical capacity and most negative electrochemical potential. However, the practical application of lithium metal battery(LMB) is largely retarded by the instable interfaces, uncontrolled dendrites, and rapid capacity deterioration. Herein, we present a comprehensive overview towards the working principles and inherent challenges of LMAs. Firstly, we diligently summarize the intrinsic mechanism of Li stripping and plating process. The recent advances in atomic and mesoscale simulations which are crucial in guiding mechanism study and material design are also summarized. Furthermore, the advanced engineering strategies which have been proved effective in protecting LMAs are systematically reviewed, including electrolyte optimization, artificial interface, composite/alloy anodes and so on. Finally, we highlight the current limitations and promising research directions of LMAs. This review sheds new lights on deeply understanding the intrinsic mechanism of LMAs, and calls for more endeavors to realize practical Li metal batteries.展开更多
Lithium metal anode of lithium batteries,including lithium-ion batteries,has been considered the anode for next-generation batteries with desired high energy densities due to its high theoretical specific capacity(386...Lithium metal anode of lithium batteries,including lithium-ion batteries,has been considered the anode for next-generation batteries with desired high energy densities due to its high theoretical specific capacity(3860 mA h g^(-1))and low standards electrode potential(-3.04 V vs.SHE).However,the highly reactive nature of metallic lithium and its direct contact with the electrolyte could lead to severe chemical reactions,leading to the continuous consumption of the electrolyte and a reduction in the cycle life and Coulombic efficiency.In addition,the solid electrolyte interface formed during battery cycling is mainly inorganic,which is too fragile to withstand the extreme volume change during the plating and stripping of lithium.The uneven flux of lithium ions could lead to excessive lithium deposition at local points,resulting in needle-like lithium dendrites,which could pierce the separator and cause short circuits,battery failure,and safety issues.In the last five years,tremendous efforts have been dedicated to addressing these issues,and the most successful improvements have been related to lithiophilicity optimizations.Thus,this paper comprehensively reviewed the lithiophilicity regulation in lithium metal anode modifications and highlighted the vital effect of lithiophilicity.The remaining challenges faced by the lithiophilicity optimization for lithium metal anodes are discussed with the proposed research directions for overcoming the technical challenges in this subject.展开更多
The practical application of Li metal anodes(LMAs)is limited by uncontrolled dendrite growth and side reactions.Herein,we propose a new friction-induced strategy to produce high-performance thin Li anode(Li@CFO).By vi...The practical application of Li metal anodes(LMAs)is limited by uncontrolled dendrite growth and side reactions.Herein,we propose a new friction-induced strategy to produce high-performance thin Li anode(Li@CFO).By virtue of the in situ friction reaction between fluoropolymer grease and Li strips during rolling,a robust organic/inorganic hybrid interlayer(lithiophilic LiF/LiC_(6)framework hybridized-CF_(2)-O-CF_(2)-chains)was formed atop Li metal.The derived interface contributes to reversible Li plating/stripping behaviors by mitigating side reactions and decreasing the solvation degree at the interface.The Li@CFO||Li@CFO symmetrical cell exhibits a remarkable lifespan for 5,600 h(1.0 mA cm^(-2)and 1.0 mAh cm^(-2))and 1,350 cycles even at a harsh condition(18.0 mA cm^(-2)and 3.0 mAh cm^(-2)).When paired with high-loading LiFePO4 cathodes,the full cell lasts over 450 cycles at 1C with a high-capacity retention of 99.9%.This work provides a new friction-induced strategy for producing high-performance thin LMAs.展开更多
Lithium metal batteries are emerging as a strong candidate in the future energy storage market due to its extremely high energy density.However,the uncontrollable lithium dendrites and volume change of lithium metal a...Lithium metal batteries are emerging as a strong candidate in the future energy storage market due to its extremely high energy density.However,the uncontrollable lithium dendrites and volume change of lithium metal anodes severely hinder its application.In this work,the porous Cu skeleton modified with Cu_(6)Sn_(5)layer is prepared via dealloying brass foil following a facile electroless process.The porous Cu skeleton with large specific surface area and high electronic conductivity effectively reduces the local current density.The Cu_(6)Sn_(5)can react with lithium during the discharge process to form lithiophilic Li_(7)Sn_(2)in situ to promote Li-ions transport and reduce the nucleation energy barrier of lithium to guide the uniform lithium deposition.Therefore,more than 300 cycles at 1 mA cm^(−2)are achieved in the half-cell with an average Coulombic efficiency of 97.5%.The symmetric cell shows a superior cycle life of more than 1000 h at 1 mA cm^(−2)with a small average hysteresis voltage of 16 mV.When coupled with LiFePO_(4)cathode,the full cell also maintains excellent cycling and rate performance.展开更多
Lithium metal has been considered one of the most promising anodes for next-generation rechargeable batteries,but its practical application is largely hindered by the uncontrollable dendrite growth and infinite volume...Lithium metal has been considered one of the most promising anodes for next-generation rechargeable batteries,but its practical application is largely hindered by the uncontrollable dendrite growth and infinite volume change.Here,inspired by superior catalytic effects of single-atom catalysts,carbon-supported single atomic Co with asymmetric N,O-coordination(Co-N/O)is developed for Li metal battery.Experimental results and theoretical calculations indicate that single atomic Co atoms with asymmetric N,O-coordination present enhanced binding ability toward Li in comparison with N-coordinated atomic Co site and isolated O site,enabling uniform Li plating/stripping.Moreover,the asymmetric N,O-coordination around Co atoms induces co-activation effects,lowering the energy barriers toward Li^(+)to Li^(0)conversion and largely promoting the deposition kinetics.When used as a Li deposition host,the Co-N/O achieves a high average coulombic efficiency of 98.6%at a current density of 1 mA cm^(-2)and a capacity of 2 mAh cm^(-2),long cycling life of 2000 h in symmetrical cells,and excellent rate performance(voltage hysteresis of 23 mV at 8 mA cm^(-2)).This work provides a comprehensive understanding of single atomic metals with asymmetric heteroatom coordination in the design of Li metal anode.展开更多
Lithium(Li) metal has emerged as the most promising anode for rechargeable Li batteries owing to its high theoretical specific capacities, low negative electrochemical potential, and superior electrical conductivity. ...Lithium(Li) metal has emerged as the most promising anode for rechargeable Li batteries owing to its high theoretical specific capacities, low negative electrochemical potential, and superior electrical conductivity. Replacing the conventional graphite anodes with Li metal anodes(LMAs) provides great potential to exceed the theoretical limitations of current commercial Li-ion batteries, leading to nextgeneration high-energy–density rechargeable Li metal batteries(LMBs). However, further development of LMAs is hindered by several inherent issues, such as dangerous dendrite growth, infinite volume change, low Coulombic efficiency, and interfacial side reactions. MXenes, a family of two-dimensional(2 D) transition metal carbides and/or nitrides, have recently attracted much attention to address these issues due to their 2D structure, lithiophilic surface terminations, excellent electrical and ionic conductivity, and superior mechanical properties. Herein, an overview of recent advances in the roles of MXenes for stabilizing LMAs is presented. In particular, strategies of utilizing MXenes as the Li hosts, artificial protection layers, electrolyte additives, and for separator modifications to develop stable and dendrite-free LMAs are discussed. Moreover, a perspective on the current challenges and potential outlooks on MXenes for advanced LMAs is provided.展开更多
Lithium metal anode is one of the most important anode materials for next-generation high-specificenergy secondary batteries.Structured lithium metal anodes have received extensive attention in the development of prac...Lithium metal anode is one of the most important anode materials for next-generation high-specificenergy secondary batteries.Structured lithium metal anodes have received extensive attention in the development of practical lithium metal batteries.Methods of driving lithium metal to deposit inside the pores of structured lithium metal anodes have always been one of the most concerned issues,especially for highly conductive frameworks.An electrochemical phase field theory with galvanostatic lithium plating process is employed in this work,the mechanism that illustrates the preference of lithium metal to deposit at the top of the framework structure has been revealed,and through the simulation analysis of various regulating strategies,the strategies that can efficiently drive lithium to deposit inside structured pores are summarized.This work presents the theoretical calculation and analysis methods that can be used for the rational design of lithium metal batteries.展开更多
Lithium (Li) metal is a promising anode for the next generation high-energy–density batteries. However, the growth of Li dendrites, low coulombic efficiency and dramatic volume change limit its development. Here, we ...Lithium (Li) metal is a promising anode for the next generation high-energy–density batteries. However, the growth of Li dendrites, low coulombic efficiency and dramatic volume change limit its development. Here, we report a new synthetic poly-dioxolane (PDOL) approach to constructing an artificial 'elastic' SEI to stabilize the Li/electrolyte interface and the Li deposition/dissolution behavior in a variety of electrolytes. By coating PDOL with optimized molecular weights and synthetic routes on Li metal anode, the 'elastic' SEI layer could be maintained on top of the Li metal anode to accommodate the Li deposition/dissolution. No dendrite formation was observed during the cycling process, and the interfacial side reactions were reduced significantly. Consequently, we successfully achieved 330 cycles with a CE of 98.4% in ether electrolytes and 90 cycles with a CE of 94.3% in carbonate electrolytes. Simultaneously, the Li-metal batteries with LiFePO_(4) as cathodes also exhibited improved cycling performance. This strategy could promote the development of dendrite-free metal anodes toward high-performance Li-metal batteries.展开更多
Lithium(Li)metal batteries have long been deemed as the representative high-energy-density energy storage systems due to the ultrahigh theoretical capacity and lowest electrochemical potential of Li metal anode.Unfort...Lithium(Li)metal batteries have long been deemed as the representative high-energy-density energy storage systems due to the ultrahigh theoretical capacity and lowest electrochemical potential of Li metal anode.Unfortunately,the intractable dendritic Li deposition during cycling greatly restrains the large-scale applications of Li metal anodes.Recent advances have been explored to address this issue,among which a specific class of electrolyte additives for electroplating is deeply impressive,as they are economic and pragmatic.Different from the conventional additives that construct solid electrolyte interphase(SEI)layer on anodes,they make dendrite-free Li metal anodes feasible through altering Li plating behavior.In this research news article,the interlinked principles between industrial electroplating and Li deposition are firstly illustrated.The featured effects of electroplating additives on regulating Li plating morphology are also summarized and mainly divided into three categories:co-deposition with Li cation,coordination with Li cation,and leveling effect of Li films.Furthermore,the mechanism exploration or derivative use of electroplating additive for dendrite suppression and potential research directions are proposed,with emphasizing that industrial electroplating might enable Li metal anode to scalable battery techniques and spread to metal battery systems beyond Li.展开更多
Lithium metal,as the most ideal anode material for high energy density batteries,has been researched for several decades.However,the dendrite formation and large volume change during repetitive lithium plating/strippi...Lithium metal,as the most ideal anode material for high energy density batteries,has been researched for several decades.However,the dendrite formation and large volume change during repetitive lithium plating/stripping lead to a serious safety issue and impede the practical application of lithium metal anode.Herein,a nanoporous Ni foam current collector with high surface area and surface flaws is constructed via a facile oxidation-reduction method.The inherent macropore structure of Ni foam can partly accommodate the volume variation during Li plating/stripping.The well-distributed nanopores on the skeleton of Ni foam can effectively reduce the local current density,regulate the uniform lithium nucleation and deposition with homogenous distribution of Li^(+) flux.Moreover,the surface flaws induce the formation of ring Li structures at initial nucleation/deposition processes and concave Li metal spontaneously formed based on the ring Li structures during cycling,which can direct the even Li plating/stripping.Therefore,highly stable Coulombic efficiency is achieved at 1 mA cm^(-2) for 200 cycles.The symmetrical cell,based on the nanoporous Ni foam current collector,presents long lifespans of 1200 and 700 h respectively at different current densities of 0.5 and 1 mA cm^(-2) without short circuit.In addition,the LiFePO4 full cell,with the Li metal anode based on the nanoporous Ni foam current collector,shows excellent cycling performance at 1 C for 300 cycles and rate performance.展开更多
Electrode process kinetics is a key part that determines the morphology of metal electrodeposition.However,the liquid-phase mass transfer process and its effect on lithium(Li)metal electrodeposition are still poorly u...Electrode process kinetics is a key part that determines the morphology of metal electrodeposition.However,the liquid-phase mass transfer process and its effect on lithium(Li)metal electrodeposition are still poorly understood.Herein,the effect of mass transfer on the electrodeposition behavior of Li metal is explored.Experiments and COMSOL Multiphysics simulations reveal that the enhanced mass transfer,which is induced by ultrasonic wave,can homogenize the ion flow on the surface of electrode to obtain uniform Li nucleation.Meanwhile,the rapid mass transfer of Li^(+)provides sufficient cations around the germinated Li to avoid preferential growth of Li in a specific direction.Based on the simultaneous regulation of nucleation and growth behavior,a smooth and compact Li deposits can be achieved,which exhibit a small polarization voltage during repeated Li plating/striping and a considerably enhanced cyclability.This work enriches the fundamental understanding of Li electrodeposition without dendrite structure and affords fresh guidance to develop dendrite-free metal anodes for metal-based batteries.展开更多
Lithium metal batteries are strongly considered as one of the most promising candidates for nextgeneration high-performance battery systems.However,the uncontrollable growth of lithium dendrites and the highly reactiv...Lithium metal batteries are strongly considered as one of the most promising candidates for nextgeneration high-performance battery systems.However,the uncontrollable growth of lithium dendrites and the highly reactive lithium metal result in the severe safety risks and the short lifespan for highenergy-density rechargeable batteries.Here,we demonstrate a hydrophobic and ionically conductive ethylene-vinyl acetate(EVA)copolymer layer can not only endow lithium metal anodes with an air-stable and anti-water surface,but also efficiently suppress the lithium-dendrites growth during the electrochemical cycling process.Therefore,the introduction of the EVA copolymer as a bifunctional protection layer simultaneously improves the anti-water/air performance and electrochemical cycling stability of lithium metal anode.展开更多
With the increasing demand for high energy-density batteries for portable electronics and large-scale energy storage systems,the lithium metal anode(LMA)has received tremendous attention because of its high theoretica...With the increasing demand for high energy-density batteries for portable electronics and large-scale energy storage systems,the lithium metal anode(LMA)has received tremendous attention because of its high theoretical capacity and low redox potential.However,the commercial application of LMAs is impeded by the uncontrolled growth of lithium dendrites.Such dendrite growth may result in internal short circuits,detrimental side reactions,and the formation of dead lithium.Therefore,the growth of lithium metal must be controlled.This article summarizes our recent efforts in inhibiting such dendrite growth,decreasing the detrimental side reactions,and elongating the LMA lifespan by optimizing the electrolyte structure and by designing appropriate current collectors.After identifying that the unstable solid electrolyte inter-face(SEI)film is responsible for the potential dropping in carbonate electrolytes,we developed LiPF_(6)-LiNO_(3) dual-salt electrolyte and lithium bis(fluorosulfonyl)imide(LiFSI)-carbonate electrolyte to stabilize the SEI film of LMAs.In addition,we achieved controlled lithium depos-ition by designing the structure and material of the current collectors,including selective lithium deposition in porous current collectors,lithio-philic metal guided lithium deposition,and iron carbide induced underpotential lithium deposition in nano-cavities.The limitations of the cur-rent strategies and prospects for future research are also presented.展开更多
Lithium metal anode is the most potential anode material for the next generation high-energy rechargeable batteries owing to its highest specific capacity and lowest redox potential.Unfortunately,the uneven deposition...Lithium metal anode is the most potential anode material for the next generation high-energy rechargeable batteries owing to its highest specific capacity and lowest redox potential.Unfortunately,the uneven deposition of Li during plating/stripping and the formation of uncontrolled Li dendrites,which might cause poor battery performance and serious safety problems,are demonstrating to be a huge challenge for its practical application.Here,we show that a flexible and free-standing film hybriding with polypyrrole(PPy) nanotubes and reduced graphene oxide(rGO) can significantly regulate the Li nucleation and deposition,and further prohibit the formation of Li dendrites,owing to the large specific surface area,rich of nitrogen functional groups and porous structures.Finally,the high Coulombic efficiency and stable Li plating/stripping cycling performance with 98% for 230 cycles at 0.5 mA cm^(-2) and more than 900 hours stable lifespan are achieved.No Li dendrites form even at a Li deposition capacity as high as4.0 mA h cm^(-2).Besides,the designed PPy/rGO hybrid anode scaffold can also drive a superior battery performance in the lithium-metal full cell applications.展开更多
基金supported by the National Key Research and Development Program(2021YFB2400300)National Natural Science Foundation of China(22379013 and 22209010)the Beijing Institute of Technology“Xiaomi Young Scholars”program。
文摘Lithium(Li)metal is regarded as a promising anode candidate for high-energy-density rechargeable batteries.Nevertheless,Li metal is highly reactive against electrolytes,leading to rapid decay of active Li metal reservoir.Here,alloying Li metal with low-content magnesium(Mg)is proposed to mitigate the reaction kinetics between Li metal anodes and electrolytes.Mg atoms enter the lattice of Li atoms,forming solid solution due to the low amount(5 wt%)of Mg.Mg atoms mainly concentrate near the surface of Mg-alloyed Li metal anodes.The reactivity of Mg-alloyed Li metal is mitigated kinetically,which results from the electron transfer from Li to Mg atoms due to the electronegativity difference.Based on quantitative experimental analysis,the consumption rate of active Li and electrolytes is decreased by using Mgalloyed Li metal anodes,which increases the cycle life of Li metal batteries under demanding conditions.Further,a pouch cell(1.25 Ah)with Mg-alloyed Li metal anodes delivers an energy density of 340 Wh kg^(-1)and a cycle life of 100 cycles.This work inspires the strategy of modifying Li metal anodes to kinetically mitigate the side reactions with electrolytes.
基金financially supported by the Shenzhen Science and Technology Program (Grant No.KQTD20200820113045083,ZDSYS20190902093220279,and JCYJ20220818102403007)the National Natural Science Foundation of China (52201257)the Shenzhen Research Fund for Returned Scholars (DD11409017).
文摘Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial application.Herein,we report a liquid metal-coated lithium metal(LM@Li)anode strategy to improve the contact between lithium metal and a Li6PS5Cl inorganic electrolyte.The LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2mA cm^(-2) and a significantly higher critical current density of 9.8 mAcm^(-2) at 25°C.In addition,a full battery assembled with a high-capacity composite LiNbO3@-LiNi_(0.7)Co_(0.2)Mn_(0.1)O_(2)(LNO@NCM721)cathode shows stable cycling performance.Experimental and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.
基金supported by the National Natural Science Foundation of China (51974256 and 52034011)the Outstanding Young Scholars of Shaanxi (2019JC-12)+1 种基金the Natural Science Basic Research Plan in Shaanxi Province (2019JLZ-01 and 2019JLM-29)the Fundamental Research Funds of Universities in Inner Mongolia Autonomous Region (21300-5223735)。
文摘The dendrite growth that results from the slow electrode process kinetics prevents the lithium(Li) metal anode from being used in practical applications. Here, full-chain enhanced ion transport for stabilizing Li metal anodes is proposed. Experimental and theoretical studies confirm that full-chain enhanced ion transport(electrocrystallization, mass transport in the electrolyte and diffusion in solid electrolyte interphase) under magnetoelectrochemistry contributes to a homogeneous, dense, and dendrite-free morphology. Specifically, the enhanced electrocrystallization behavior promotes the Li nucleation;the enhanced mass transport in the electrolyte alleviates the ion concentration gradient at the electrode surface, which helps to inhibit dendrite growth;and the enhanced diffusion in the solid electrolyte interphase further homogenizes the Li deposition behavior, obtaining regular and uniform Li particles.Consequently, the Li metal anode has exceptional cycling stability in both symmetric and full cells,and the pouch cell performs long cycles(170 cycles) in practice evaluation. This work advances fundamental knowledge of the magneto-dendrite effect and offers a new perspective on stabilizing metal anodes.
基金financially supported by the National Natural Science Foundation of China(22105095)the Shenzhen Key Laboratory of Solid State Batteries(ZDSYS20180208184346531)+9 种基金the Shenzhen Science and Technology Program(KQTD20200820113047086)the Key Program of the National Natural Science Foundation of China(51732005)the Guangdong Basic and Applied Basic Research Foundation(2020A1515111129)the Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(2018B030322001)the Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices(2019B121205001)the Guangdong Basic and Applied Basic Research Foundation(2021A1515012403)the Basic Research Project of Science and Technology Innovation Commission of Shenzhen(JSGG20191129111001820)the Key Laboratory of Energy Conversion and Storage Technologies(Southern University of Science and Technology)the Ministry of Educationand Laboratory of Electrochemical Energy Storage Technologies,Academy for Advanced Interdisciplinary Studies(SUSTech)。
文摘Solid-state lithium-metal batteries,with their high theoretical energy density and safety,are highly promising as a next-generation battery contender.Among the alternatives proposed as solid-state electrolyte,lithium-rich anti-perovskite(Li RAP)materials have drawn the most interest because of high theoretical Li^(+)conductivity,low cost and easy processing.Although solid-state electrolytes are believed to have the potential to physically inhibit the lithium dendrite growth,lithium-metal batteries still suffer from the lithium dendrite growth and thereafter the short circuiting.The voids in practical Li RAP pellets are considered as the root cause.Herein,we show that reducing the voids can effectively suppress the lithium dendrite growth.The voids in the pellet resulted in an irregular Li^(+)flux distribution and a poor interfacial contact with lithium metal anode;and hence the ununiform lithium dendrites.Consequently,the lithium-metal symmetric cell with void-reduced Li_(2)OHCl-HT pellet was able to display excellent cycling performance(750 h at 0.4 m A cm^(-2))and stability at high current density(0.8 m A cm^(-2)for 120 h).This study provides not only experimental evidence for the impact of the voids in Li RAP pellets on the lithium dendrite growth,but also a rational pellet fabrication approach to suppress the lithium dendrite growth.
基金Science Foundation for Distinguished Young Scholars in Tianjin,Grant/Award Number:19JCJQJC61700National Natural Science Foundation of China,Grant/Award Numbers:51773147,51973151,52130303National Key R&D Program of China,Grant/Award Number:2022YFB3805702。
文摘Lithium(Li)metal anodes have attracted extensive attention due to their ultrahigh theoretical capacity and low potential.However,the uneven deposition of Li near the unstable electrode/electrolyte interfaces leads to the growth of Li dendrites and the degradation of active electrodes.Herein,we directly fluorinate alkyne-containing conjugated microporous polymers(ACMPs)microspheres with fluorine gas(F_(2))to introduce a novel fluorinated interlayer as an interfacial stabilizer in lithium metal batteries.Using density functional theory methods,it is found that as-prepared fluorinated ACMP(FACMP)has abundant partially ionic C–F bonds.The C–F bonds with electrochemical lability yield remarkable lithiophilicity during cycling.The in situ reactions between the active C–F bonds and Li ions enable transfer of lithium fluoride microcrystals to the solid electrolyte interphase(SEI)layers,guaranteeing effective ionic distribution and smooth Li deposition.Consequently,Li metal electrodes with the fluorinated interlayers demonstrate excellent cycling performances in both half-batteries and full cells with a lithium bis(trifluoromethanesulfonyl)imide electrolyte as well as a nonfluorinated lithium bis(oxalate)borate electrolyte system.This strategy is highly significant in customizable SEI layers to stabilize electrode interfaces and ensure high utilization of Li metal anodes,especially in a nonfluorinated electrolyte.
基金financialy supported by National Natural Science Foundation of China(52002297,51974208,and 21875080)Wuhan Yellow Crane Talents ProgramNumerical calculation is supported by High-Performance Computing Center of Wuhan University of Science and Technology)
文摘Ultrathin and air-stable Li metal anodes hold great promise toward high-energy and high-safety Li metal batteries(LMBs).However,the application of LMBs is technically impeded by existing Li metal anodes with large thickness,high reactivity,and poor performance.Here,we developed a novel and scalable approach for the construction of a 10-μm-thick flexible and air-stable Li metal anode by conformally encapsulating Li within a multifunctional VN film.Specifically,the highly lithiophilic VN layer guides a uniform deposition of Li,while abundant and multilevel pores arising from assembly of ultrathin nanosheets enable a spatially confined immersion of metallic Li,thus ensuring an ultrathin and sandwiched Li anode.More impressively,the strong hydrophobicity of VN surface can effectively improve the stability of anode to humid air,whereas the highly conductive framework greatly boosts charge transfer dynamics and enhances Li utilization and high-rate capability.Benefiting from such fascinating features,the constructed Li-VN anode exhibits ultrastable cycling stability in both ether(2500 h)and carbonate(900 h)electrolytes,respectively.Moreover,even exposed to ambient air for 12 h,the anode still can retain~78%capacity,demonstrating excellent air-defendable capability.This work affords a promising strategy for fabricating high-performance,high-safety,and low-cost LMBs.
基金supported by National Key Research and Development Program (2021YFB2400300)Beijing Natural Science Foundation (JQ20004)+1 种基金the National Natural Science Foundation of China (22109011, U1801257)Scientific and Technological Key Project of Shanxi Province (20191102003)。
文摘Lithium metal anode(LMA) is a promising candidate for achieving next-generation high-energy-density batteries due to its ultrahigh theoretical capacity and most negative electrochemical potential. However, the practical application of lithium metal battery(LMB) is largely retarded by the instable interfaces, uncontrolled dendrites, and rapid capacity deterioration. Herein, we present a comprehensive overview towards the working principles and inherent challenges of LMAs. Firstly, we diligently summarize the intrinsic mechanism of Li stripping and plating process. The recent advances in atomic and mesoscale simulations which are crucial in guiding mechanism study and material design are also summarized. Furthermore, the advanced engineering strategies which have been proved effective in protecting LMAs are systematically reviewed, including electrolyte optimization, artificial interface, composite/alloy anodes and so on. Finally, we highlight the current limitations and promising research directions of LMAs. This review sheds new lights on deeply understanding the intrinsic mechanism of LMAs, and calls for more endeavors to realize practical Li metal batteries.
基金supported by the National Natural Science Foundation of China(52072217,22179071)the Joint Funds of the National Natural Science Foundation of China(U20A20249)the Major Technological Innovation Project of Hubei Science and Technology Department(2019AAA164)。
文摘Lithium metal anode of lithium batteries,including lithium-ion batteries,has been considered the anode for next-generation batteries with desired high energy densities due to its high theoretical specific capacity(3860 mA h g^(-1))and low standards electrode potential(-3.04 V vs.SHE).However,the highly reactive nature of metallic lithium and its direct contact with the electrolyte could lead to severe chemical reactions,leading to the continuous consumption of the electrolyte and a reduction in the cycle life and Coulombic efficiency.In addition,the solid electrolyte interface formed during battery cycling is mainly inorganic,which is too fragile to withstand the extreme volume change during the plating and stripping of lithium.The uneven flux of lithium ions could lead to excessive lithium deposition at local points,resulting in needle-like lithium dendrites,which could pierce the separator and cause short circuits,battery failure,and safety issues.In the last five years,tremendous efforts have been dedicated to addressing these issues,and the most successful improvements have been related to lithiophilicity optimizations.Thus,this paper comprehensively reviewed the lithiophilicity regulation in lithium metal anode modifications and highlighted the vital effect of lithiophilicity.The remaining challenges faced by the lithiophilicity optimization for lithium metal anodes are discussed with the proposed research directions for overcoming the technical challenges in this subject.
基金This work was supported by the National Natural Science Foundation of China(U1904216 and U22A20141)the Natural Science Foundation of Changsha City(kq2208258).
文摘The practical application of Li metal anodes(LMAs)is limited by uncontrolled dendrite growth and side reactions.Herein,we propose a new friction-induced strategy to produce high-performance thin Li anode(Li@CFO).By virtue of the in situ friction reaction between fluoropolymer grease and Li strips during rolling,a robust organic/inorganic hybrid interlayer(lithiophilic LiF/LiC_(6)framework hybridized-CF_(2)-O-CF_(2)-chains)was formed atop Li metal.The derived interface contributes to reversible Li plating/stripping behaviors by mitigating side reactions and decreasing the solvation degree at the interface.The Li@CFO||Li@CFO symmetrical cell exhibits a remarkable lifespan for 5,600 h(1.0 mA cm^(-2)and 1.0 mAh cm^(-2))and 1,350 cycles even at a harsh condition(18.0 mA cm^(-2)and 3.0 mAh cm^(-2)).When paired with high-loading LiFePO4 cathodes,the full cell lasts over 450 cycles at 1C with a high-capacity retention of 99.9%.This work provides a new friction-induced strategy for producing high-performance thin LMAs.
基金supported by the National Natural Science Foundation of China(52072173)the Jiangsu Province Outstanding Youth Fund(BK20200016)the International Cooperation of Jiangsu Province(SBZ2022000084)
文摘Lithium metal batteries are emerging as a strong candidate in the future energy storage market due to its extremely high energy density.However,the uncontrollable lithium dendrites and volume change of lithium metal anodes severely hinder its application.In this work,the porous Cu skeleton modified with Cu_(6)Sn_(5)layer is prepared via dealloying brass foil following a facile electroless process.The porous Cu skeleton with large specific surface area and high electronic conductivity effectively reduces the local current density.The Cu_(6)Sn_(5)can react with lithium during the discharge process to form lithiophilic Li_(7)Sn_(2)in situ to promote Li-ions transport and reduce the nucleation energy barrier of lithium to guide the uniform lithium deposition.Therefore,more than 300 cycles at 1 mA cm^(−2)are achieved in the half-cell with an average Coulombic efficiency of 97.5%.The symmetric cell shows a superior cycle life of more than 1000 h at 1 mA cm^(−2)with a small average hysteresis voltage of 16 mV.When coupled with LiFePO_(4)cathode,the full cell also maintains excellent cycling and rate performance.
基金supported by the Ministry of Education,Singapore,under its MOE tier2 grant MOE2019-T2-1-181.
文摘Lithium metal has been considered one of the most promising anodes for next-generation rechargeable batteries,but its practical application is largely hindered by the uncontrollable dendrite growth and infinite volume change.Here,inspired by superior catalytic effects of single-atom catalysts,carbon-supported single atomic Co with asymmetric N,O-coordination(Co-N/O)is developed for Li metal battery.Experimental results and theoretical calculations indicate that single atomic Co atoms with asymmetric N,O-coordination present enhanced binding ability toward Li in comparison with N-coordinated atomic Co site and isolated O site,enabling uniform Li plating/stripping.Moreover,the asymmetric N,O-coordination around Co atoms induces co-activation effects,lowering the energy barriers toward Li^(+)to Li^(0)conversion and largely promoting the deposition kinetics.When used as a Li deposition host,the Co-N/O achieves a high average coulombic efficiency of 98.6%at a current density of 1 mA cm^(-2)and a capacity of 2 mAh cm^(-2),long cycling life of 2000 h in symmetrical cells,and excellent rate performance(voltage hysteresis of 23 mV at 8 mA cm^(-2)).This work provides a comprehensive understanding of single atomic metals with asymmetric heteroatom coordination in the design of Li metal anode.
基金supported by the NJIT Start-Up FundsFaculty Seed Grant。
文摘Lithium(Li) metal has emerged as the most promising anode for rechargeable Li batteries owing to its high theoretical specific capacities, low negative electrochemical potential, and superior electrical conductivity. Replacing the conventional graphite anodes with Li metal anodes(LMAs) provides great potential to exceed the theoretical limitations of current commercial Li-ion batteries, leading to nextgeneration high-energy–density rechargeable Li metal batteries(LMBs). However, further development of LMAs is hindered by several inherent issues, such as dangerous dendrite growth, infinite volume change, low Coulombic efficiency, and interfacial side reactions. MXenes, a family of two-dimensional(2 D) transition metal carbides and/or nitrides, have recently attracted much attention to address these issues due to their 2D structure, lithiophilic surface terminations, excellent electrical and ionic conductivity, and superior mechanical properties. Herein, an overview of recent advances in the roles of MXenes for stabilizing LMAs is presented. In particular, strategies of utilizing MXenes as the Li hosts, artificial protection layers, electrolyte additives, and for separator modifications to develop stable and dendrite-free LMAs are discussed. Moreover, a perspective on the current challenges and potential outlooks on MXenes for advanced LMAs is provided.
基金supported by Beijing Natural Science Foundation(JQ20004)National Key Research and Development Program(2021YFB2400300)+1 种基金National Natural Scientific Foundation of China(22109011)the China Postdoctoral Science Foundation(BX20200047,2021M690380)。
文摘Lithium metal anode is one of the most important anode materials for next-generation high-specificenergy secondary batteries.Structured lithium metal anodes have received extensive attention in the development of practical lithium metal batteries.Methods of driving lithium metal to deposit inside the pores of structured lithium metal anodes have always been one of the most concerned issues,especially for highly conductive frameworks.An electrochemical phase field theory with galvanostatic lithium plating process is employed in this work,the mechanism that illustrates the preference of lithium metal to deposit at the top of the framework structure has been revealed,and through the simulation analysis of various regulating strategies,the strategies that can efficiently drive lithium to deposit inside structured pores are summarized.This work presents the theoretical calculation and analysis methods that can be used for the rational design of lithium metal batteries.
基金This research was supported financially by the Major Program of the National Natural Science Foundation of China(21890731).
文摘Lithium (Li) metal is a promising anode for the next generation high-energy–density batteries. However, the growth of Li dendrites, low coulombic efficiency and dramatic volume change limit its development. Here, we report a new synthetic poly-dioxolane (PDOL) approach to constructing an artificial 'elastic' SEI to stabilize the Li/electrolyte interface and the Li deposition/dissolution behavior in a variety of electrolytes. By coating PDOL with optimized molecular weights and synthetic routes on Li metal anode, the 'elastic' SEI layer could be maintained on top of the Li metal anode to accommodate the Li deposition/dissolution. No dendrite formation was observed during the cycling process, and the interfacial side reactions were reduced significantly. Consequently, we successfully achieved 330 cycles with a CE of 98.4% in ether electrolytes and 90 cycles with a CE of 94.3% in carbonate electrolytes. Simultaneously, the Li-metal batteries with LiFePO_(4) as cathodes also exhibited improved cycling performance. This strategy could promote the development of dendrite-free metal anodes toward high-performance Li-metal batteries.
基金support from National Nature Science Foundation of China(Grant No.51872157)Shenzhen Technical Plan Project(Grant Nos.JCYJ20170412170911187 and JCYJ20170817161753629)+1 种基金Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(Grant No.2017BT01N111)Guangdong Technical Plan Project(Grant No.2017B090907005)
文摘Lithium(Li)metal batteries have long been deemed as the representative high-energy-density energy storage systems due to the ultrahigh theoretical capacity and lowest electrochemical potential of Li metal anode.Unfortunately,the intractable dendritic Li deposition during cycling greatly restrains the large-scale applications of Li metal anodes.Recent advances have been explored to address this issue,among which a specific class of electrolyte additives for electroplating is deeply impressive,as they are economic and pragmatic.Different from the conventional additives that construct solid electrolyte interphase(SEI)layer on anodes,they make dendrite-free Li metal anodes feasible through altering Li plating behavior.In this research news article,the interlinked principles between industrial electroplating and Li deposition are firstly illustrated.The featured effects of electroplating additives on regulating Li plating morphology are also summarized and mainly divided into three categories:co-deposition with Li cation,coordination with Li cation,and leveling effect of Li films.Furthermore,the mechanism exploration or derivative use of electroplating additive for dendrite suppression and potential research directions are proposed,with emphasizing that industrial electroplating might enable Li metal anode to scalable battery techniques and spread to metal battery systems beyond Li.
基金the National Natural Science Foundation of China(No.51761135123)the National Key Research&Development Program(2016YFB0303903,2016YFE0201600)。
文摘Lithium metal,as the most ideal anode material for high energy density batteries,has been researched for several decades.However,the dendrite formation and large volume change during repetitive lithium plating/stripping lead to a serious safety issue and impede the practical application of lithium metal anode.Herein,a nanoporous Ni foam current collector with high surface area and surface flaws is constructed via a facile oxidation-reduction method.The inherent macropore structure of Ni foam can partly accommodate the volume variation during Li plating/stripping.The well-distributed nanopores on the skeleton of Ni foam can effectively reduce the local current density,regulate the uniform lithium nucleation and deposition with homogenous distribution of Li^(+) flux.Moreover,the surface flaws induce the formation of ring Li structures at initial nucleation/deposition processes and concave Li metal spontaneously formed based on the ring Li structures during cycling,which can direct the even Li plating/stripping.Therefore,highly stable Coulombic efficiency is achieved at 1 mA cm^(-2) for 200 cycles.The symmetrical cell,based on the nanoporous Ni foam current collector,presents long lifespans of 1200 and 700 h respectively at different current densities of 0.5 and 1 mA cm^(-2) without short circuit.In addition,the LiFePO4 full cell,with the Li metal anode based on the nanoporous Ni foam current collector,shows excellent cycling performance at 1 C for 300 cycles and rate performance.
基金the financial support provided by the National Natural Science Foundation of China(51974256)the Outstanding Young Scholars of Shaanxi(2019JC-12)+2 种基金the Natural Science Basic Research Plan in Shaanxi Province of China(2019JLZ-01 and 2019JLM-29)the Fundamental Research Funds for the Central Universities(19GH020302 and 3102019JC005)the Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University(CX202005)。
文摘Electrode process kinetics is a key part that determines the morphology of metal electrodeposition.However,the liquid-phase mass transfer process and its effect on lithium(Li)metal electrodeposition are still poorly understood.Herein,the effect of mass transfer on the electrodeposition behavior of Li metal is explored.Experiments and COMSOL Multiphysics simulations reveal that the enhanced mass transfer,which is induced by ultrasonic wave,can homogenize the ion flow on the surface of electrode to obtain uniform Li nucleation.Meanwhile,the rapid mass transfer of Li^(+)provides sufficient cations around the germinated Li to avoid preferential growth of Li in a specific direction.Based on the simultaneous regulation of nucleation and growth behavior,a smooth and compact Li deposits can be achieved,which exhibit a small polarization voltage during repeated Li plating/striping and a considerably enhanced cyclability.This work enriches the fundamental understanding of Li electrodeposition without dendrite structure and affords fresh guidance to develop dendrite-free metal anodes for metal-based batteries.
基金supported by the National Key Research and Development Program(2016YFA0202500)National Natural Science Foundation of China(21776019,21808124,51972121)+1 种基金Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program(2017TQ04C419)Beijing Natural Science Foundation(L182021)。
文摘Lithium metal batteries are strongly considered as one of the most promising candidates for nextgeneration high-performance battery systems.However,the uncontrollable growth of lithium dendrites and the highly reactive lithium metal result in the severe safety risks and the short lifespan for highenergy-density rechargeable batteries.Here,we demonstrate a hydrophobic and ionically conductive ethylene-vinyl acetate(EVA)copolymer layer can not only endow lithium metal anodes with an air-stable and anti-water surface,but also efficiently suppress the lithium-dendrites growth during the electrochemical cycling process.Therefore,the introduction of the EVA copolymer as a bifunctional protection layer simultaneously improves the anti-water/air performance and electrochemical cycling stability of lithium metal anode.
基金financially supported by the National Natural Science Foundation of China(No.21773301)。
文摘With the increasing demand for high energy-density batteries for portable electronics and large-scale energy storage systems,the lithium metal anode(LMA)has received tremendous attention because of its high theoretical capacity and low redox potential.However,the commercial application of LMAs is impeded by the uncontrolled growth of lithium dendrites.Such dendrite growth may result in internal short circuits,detrimental side reactions,and the formation of dead lithium.Therefore,the growth of lithium metal must be controlled.This article summarizes our recent efforts in inhibiting such dendrite growth,decreasing the detrimental side reactions,and elongating the LMA lifespan by optimizing the electrolyte structure and by designing appropriate current collectors.After identifying that the unstable solid electrolyte inter-face(SEI)film is responsible for the potential dropping in carbonate electrolytes,we developed LiPF_(6)-LiNO_(3) dual-salt electrolyte and lithium bis(fluorosulfonyl)imide(LiFSI)-carbonate electrolyte to stabilize the SEI film of LMAs.In addition,we achieved controlled lithium depos-ition by designing the structure and material of the current collectors,including selective lithium deposition in porous current collectors,lithio-philic metal guided lithium deposition,and iron carbide induced underpotential lithium deposition in nano-cavities.The limitations of the cur-rent strategies and prospects for future research are also presented.
基金supported by the National Natural Science Foundation of China(Nos.21603019,201503025)Key Program for International Science and Technology Cooperation Projects of Ministry of Science and Technology of China(No.2016YFE0125900)program for the Hundred Talents Program of Chongqing University。
文摘Lithium metal anode is the most potential anode material for the next generation high-energy rechargeable batteries owing to its highest specific capacity and lowest redox potential.Unfortunately,the uneven deposition of Li during plating/stripping and the formation of uncontrolled Li dendrites,which might cause poor battery performance and serious safety problems,are demonstrating to be a huge challenge for its practical application.Here,we show that a flexible and free-standing film hybriding with polypyrrole(PPy) nanotubes and reduced graphene oxide(rGO) can significantly regulate the Li nucleation and deposition,and further prohibit the formation of Li dendrites,owing to the large specific surface area,rich of nitrogen functional groups and porous structures.Finally,the high Coulombic efficiency and stable Li plating/stripping cycling performance with 98% for 230 cycles at 0.5 mA cm^(-2) and more than 900 hours stable lifespan are achieved.No Li dendrites form even at a Li deposition capacity as high as4.0 mA h cm^(-2).Besides,the designed PPy/rGO hybrid anode scaffold can also drive a superior battery performance in the lithium-metal full cell applications.
