Lithium metal is one of the most promising anode materials for rechargeable battery with high energy density,but its practical use is still hindered by two main problems,namely,lithium dendrite growth and low Coulombi...Lithium metal is one of the most promising anode materials for rechargeable battery with high energy density,but its practical use is still hindered by two main problems,namely,lithium dendrite growth and low Coulombic efficiency.To address the issues,cesium nitrate(CsNO3)is selected as the additive to modify the electrolyte for lithium secondary battery.Here we report electrochemical performance of lithium secondary battery with different concentration of CsNO3 as electrolyte additive.The study result demonstrates that Coulombic efficiency of Li–Cu cells and the lifetime of symmetric lithium cells contained CsNO3 additive are improved greatly.Li–Cu cell with 0.05 mol/L CsNO3 and 0.15 mol/L LiNO3 as electrolyte additive presents the best electrochemical performance,having the highest Coulombic efficiency of around 97%and the lowest interfacial resistance.With increasing the concentration of CsNO3 as electrolyte additive,the electrochemical performance of cells becomes poor.Meanwhile,the morphology of lithium deposited films with CsNO3-modified electrolyte become smoother and more uniform compared with the basic electrolyte.展开更多
The uncontrolled dendrite growth of lithium metal anodes(LMAs)caused by unstable anode/electrolyte interface and uneven lithium deposition have impeded the practical applications of lithium metal batteries(LMBs).Const...The uncontrolled dendrite growth of lithium metal anodes(LMAs)caused by unstable anode/electrolyte interface and uneven lithium deposition have impeded the practical applications of lithium metal batteries(LMBs).Constructing a robust artificial solid electrolyte interphase(SEI)and regulating the lithium deposition behavior is an effective strategy to address these issues.Herein,a three-dimensional(3D)lithium anode with gradient Li_(3)N has been in-situ fabricated on carbon-based framework by thermal diffusion method(denoted as CC/Li/Li_(3)N).Density functional theory(DFT)calculations reveal that Li_(3)N can effectively promote the transport of Li^(+)due to the low energy barrier of Li^(+)diffusion.As expected,the Li_(3)N-rich conformal artificial SEI film can not only effectively stabilize the interface and avoid parasitic reactions,but also facilitate fast Li^(+)transport across the SEI layer.The anode matrix with uniformly distributed Li3N can enable homogenous deposition of Li,thus preventing Li dendrite propagation.Benefiting from these merits,the CC/Li/Li_(3)N anode achieves ultralong-term cycling for>1000 h at a current density of 2 m A cm^(-2)and dendrite-free Li deposition at an ultrahigh rate of 20 m A cm^(-2).Moreover,the full cells coupled with LiFePO4cathodes show extraordinary cycling stability for>300 cycles in liquidelectrolyte-based batteries and display a high-capacity retention of 96.7%after 100 cycles in solid-state cells,demonstrating the promising prospects for the practical applications of LMBs.展开更多
The effects of different coating layers on lithium metal anode formed by reacting with different controlled atmospheres（argon,CO_2–O_2（2：1）,N_2,and CO_2–O_2–N_2（2：1：3））have been investigated.The obtained X...The effects of different coating layers on lithium metal anode formed by reacting with different controlled atmospheres（argon,CO_2–O_2（2：1）,N_2,and CO_2–O_2–N_2（2：1：3））have been investigated.The obtained XRD,second ion mass spectroscopy（SIMS）,and scanning probe microscope（SPM）results demonstrate the formation of coating layers composed of Li_2CO_3,Li_3N,and the mixture of them on lithium tablets,respectively.The Li/Li symmetrical cell and Li/S cell are assembled to prove the advantages of the protected lithium tablet on electrochemical performance.The comparison of SEM and SIMS characterizations before/after cycles clarifies that an SEI-like composition formed on the lithium tablets could modulate the interfacial stabilization between the lithium foil and the ether electrolyte.展开更多
In the development of 3D conductive frameworks for lithium metal anode(LMA),two models have been proposed:top growth model and bottom-up growth model.However,Li tends to accumulate on the top of these 3D frameworks wi...In the development of 3D conductive frameworks for lithium metal anode(LMA),two models have been proposed:top growth model and bottom-up growth model.However,Li tends to accumulate on the top of these 3D frameworks with homogenous lithiophilicity(top growth)and Li dendrite still forms.To address this issue,some researchers have focused on developing 3D frameworks with gradient lithio-philicity,which realized bottom-up growth of Li.Nevertheless,partial Li nucleation sites on the top of these frameworks were missed.Inspired by the two models talked above,this work firstly proposed a novel intermittent lithiophilic model for lithium deposition.To demonstrate the feasibility of this model,a bimetallic metal-organic frameworks derived ZnMn_(2)O_(4)-MnO nanoparticles were grown on carbon cloth for LMA.It can cycle stably under ultra-high current and areal capacity(10 mA/cm^(2),10 mAh/cm^(2)).The in-situ optical microscopy(OM)was conducted to observe the Li deposition behavior,no dendrite was found during 80 h in ester-based electrolyte while the pure Li only cycled for 2h.What is more,it can also be well-coupled with LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and solid-state electrolyte,which further prove the advantages of the intermittent model for the development of LMAs with high safety and high energy density.展开更多
Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuin...Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuing higher energy density,of which application has been challenged due to the unstable interface caused by the non-uniform electrodeposition as well as high chemical activity.Operating at higher temperature can be recommended to uniform electrodeposition of Li metal.Nevertheless,the intrinsic side-reaction between Li metal anode and electrolyte is inevitably aggravated and thus fosters the failure of Li metal anode rapidly with uneven electrodeposition.Here,a kind of temperature-tolerated ionic liquid(1-methyl-3-ethylimidazole bis(fluorosulfo nyl)imide/lithium bis(trifluoromethylsulfo nyl)imide,EF/LT)based electrolyte that matrixed with poly(vinylidene fluoride-hexafluoropropylene) was designed to maintain the interfacial stabilization of Li metal due to the weak interfacial reaction and uniform electrodeposition at high temperature of 80℃.It is the matter that the 660-h cycle with lower polarization is achieved with EF/LT-based electrolyte at temperature of 80 ℃ and the full cell embraces outstanding cyclic performance,without capacity fading within 100 cycles.Delighting,a door for practical application of Li metal anode for higher energy density as the carbon neutrality progresses in the blooming human society has been opened gradually.展开更多
Lithium(Li)metal is the most promising electrode for next-gene ration rechargeable batteries.In order to push the commercialization of the lithium metal batteries,a kind of nitrogen(N)-doped composite graphene(NCG)ado...Lithium(Li)metal is the most promising electrode for next-gene ration rechargeable batteries.In order to push the commercialization of the lithium metal batteries,a kind of nitrogen(N)-doped composite graphene(NCG)adopted as the Li plating host was prepared to regulate Li metal nucleation and suppress dendrite growth.Furthermore,a new kind of sandwich-type composite lithium metal(STCL)electrode was developed to improve its application.The STCL electrode can be used as convenient as a piece of Li foil but no dendrite growth.In a symmetric battery,the STCL electrode cycled for more than 4500 h with the overpotential of less than 40 mV.And due to the creative design,the STCL promises the Li-S battery with a prolonged cycling lifespan.展开更多
Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the sol...Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.展开更多
Li metal is widely recognized as the desired anode for next-generation energy storage,Li metal batteries,due to its highest theoretical capacity and lowest potential.Nonetheless,it suffers from unstable electrochemica...Li metal is widely recognized as the desired anode for next-generation energy storage,Li metal batteries,due to its highest theoretical capacity and lowest potential.Nonetheless,it suffers from unstable electrochemical behaviors like dendrite growth and side reactions in practical application.Herein,we report a highly stable anode with collector,Li_(5)Mg@Cu,realized by the melting-rolling process.The Li_(5)Mg@Cu anode delivers ultrahigh cycle stability for 2000 and 1000 h at the current densities of 1 and 2 mA cm^(-2),respectively in symmetric cells.Meanwhile,the Li_(5)Mg@Cu|LFP cell exhibits a high-capacity retention of 91.8% for 1000 cycles and 78.8% for 2000 cycles at 1 C.Moreover,we investigate the suppression effects of Mg on the dendrite growth by studying the performance of Li_(x)Mg@Cu electrodes with different Mg contents(2.0-16.7 at%).The exchange current density,surface energy,Li^(+)diffusion coefficient,and chemical stability of Li_(x)Mg@Cu concretely reveal this improving suppression effect when Mg content becomes higher.In addition,a Mg-rich phase with“hollow brick”morphology forming in the high Mg content Li_(x)Mg@Cu guides the uniform deposition of Li.This study reveals the suppression effects of Mg on Li dendrites growth and offers a perspective for finding the optimal component of Li-Mg alloys.展开更多
The disorganized lithium dendrites and unstable solid electrolyte interphase(SEI)severely impede the practical application of lithium metal batteries(LMBs).Herein,the N-Zn-F coordinated triazine-based covalent organic...The disorganized lithium dendrites and unstable solid electrolyte interphase(SEI)severely impede the practical application of lithium metal batteries(LMBs).Herein,the N-Zn-F coordinated triazine-based covalent organic framework(TTA-COF-ZnF_(2))is fabricated for the first time as an artificial SEI layer on the surface of lithium metal anodes(LMAs)to handle these issues.Zn-N coordination in onedimensional(1D)ordered COF can increase lithiophilic sites,reduce the Li-nucleation barrier,and regulate the Li+local coordination environment by optimizing surface charge density around the Zn metal.The electron-rich state induced by strong electron-withdrawing F-groups constructs electronegative nanochannels,which trigger efficient Li+desolvation.These beneficial attributes boost Li^(+)transfer,and homogenize Li^(+)flux,leading to uniform Li deposition.Besides,the lithiophilic triazine ring polar groups in TTA-COF-ZnF_(2)further facilitate the Li^(+)migration.The latent working mechanism of adjusting Li deposition behaviors and stabilizing LMAs for TTA-COF-ZnF_(2)is illustrated by detailed in-situ/ex-situ characterizations and density functional theory(DFT)calculations.As expected,TTA-COF-ZnF_(2)-modified Li|Cu half cells deliver a higher Coulombic efficiency(CE)of 98.4% over 250 cycles and lower nucleation overpotential(11 mV)at 1 mA cm^(-2),while TTA-COF-ZnF_(2)@Li symmetric cells display a long lifespan over3785 h at 2 mA cm^(-2).The TTA-COF-ZnF_(2)@Li|S full cells exert ultra high capacity retention of 81%(837 mA h g^(-1))after 600 cycles at 1C.Besides,the TTA-COF-ZnF_(2)@Li|LFP full cells with a high loading of 7.1 mg cm^(-2)exert ultrahigh capacity retention of 89%(108 mAh g^(-1))after 700 cycles at 5C.This synergistic strategy in N-Zn-F coordinated triazine-based COF provides a new insight to regulate the uniform platins/stripping behaviors for developing ultra-stable and dendrite-free LMBs.展开更多
This study presents a novel Li metal host material with a unique hollow nano-spherical structure that incorporates Ag nano-seeds into a graphitic carbon nitride(g-C_(3)N_(4))shell layer,referred to as g-C_(3)N_(4)@Ag ...This study presents a novel Li metal host material with a unique hollow nano-spherical structure that incorporates Ag nano-seeds into a graphitic carbon nitride(g-C_(3)N_(4))shell layer,referred to as g-C_(3)N_(4)@Ag hollow spheres.The g-C_(3)N_(4)@Ag spheres provide a managed internal site for Li metal encapsulation and promote stable Li plating.The g-C_(3)N_(4) spheres are uniformly coated using polydopamine,which has an adhesive nature,to enhance lithium plating/stripping stability.The strategic presence of Ag nano-seeds eliminates the nucleation barrier,properly directing Li growth within the hollow spheres.This design facilitates highly reversible and consistent lithium deposition,offering a promising direction for the production of high-performance lithium metal anodes.These well-designed g-C_(3)N_(4)@Ag hollow spheres ensure stable Li plating/stripping kinetics over more than 500 cycles with a high coulombic efficiency of over 97%.Furthermore,a full cell made using LiNi_(0.90)Co_(0.07)Mn_(0.03)O_(2) and Li-g-C_(3)N_(4)@Ag host electrodes demonstrated highly competitive performance over 200 cycles,providing a guide for the implementation of this technology in advanced lithium metal batteries.展开更多
The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batterie...The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batteries,especially in terms of energy density and reliability.Nevertheless,few SLMBs can deliver the required cycling performance and long-term stability for practical use,primarily due to suboptimal interface properties.Given the diverse solidification pathways leading to different interface characteristics,it is crucial to pinpoint the source of interface deterioration and develop appropriate remedies.This review focuses on Li|SSE interface issues between lithium metal anode and SSE,discussing recent advancements in the understanding of(electro)chemistry,the impact of defects,and interface evolutions that vary among different SSE species.The state-ofthe-art strategies concerning modified SEI,artificial interlayer,surface architecture,and composite structure are summarized and delved into the internal relationships between interface characteristics and performance enhancements.The current challenges and opportunities in characterizing and modifying the Li|SSE interface are suggested as potential directions for achieving practical SLMBs.展开更多
Lithium metal has emerged as a highly promising anode material for enhancing the energy density of secondary batteries,attributed to its high theoretical specific capacity and low electrochemical potential.However,saf...Lithium metal has emerged as a highly promising anode material for enhancing the energy density of secondary batteries,attributed to its high theoretical specific capacity and low electrochemical potential.However,safety concerns related to lithium dendrite-induced short circuits and suboptimal electrochemical performance have impeded the commercial viability of lithium metal batteries.Current research efforts primarily focus on altering the solvated structure of Li+by modifying the current collector or introducing electrolyte additives to lower the nucleation barrier,expedite the desolvation process,and suppress the growth of lithium dendrites.Nevertheless,an integrated approach that combines the advantages of these two strategies remains elusive.In this study,we successfully employed metal-organic salt additives with lithophilic properties to accelerate the desolvation process,reduce the nucleation barrier of Li+,and modulate its solvated structure.This approach enhanced the inorganic compound content in the solid electrolyte interphase(SEI)on lithium foil surfaces,leading to stable Li+deposition and stripping.Specifically,Li||Cu cells demonstrated excellent cycle life and Coulombic efficiency(97.28%and 98.59%,respectively)at 0.5 m A/cm^(2)@0.5 m Ah/cm^(2)and 1 m A/cm^(2)@1 m Ah/cm^(2)for 410 and 240 cycles,respectively.Li||Li symmetrical cells showed no short circuit at 1 m A/cm^(2)@1 m Ah/cm^(2)for 1150 h,and Li||LFP full cells retained 68.9%of their capacity(104.6 m Ah/g)after 250 cycles at N/P(1.1:1.0)with a current density of 1C.展开更多
The escalating demand for advanced energy storage solutions has positioned lithium metal anodes at the forefront of battery technology research.However,the practical implementation of lithium metal anodes is impeded b...The escalating demand for advanced energy storage solutions has positioned lithium metal anodes at the forefront of battery technology research.However,the practical implementation of lithium metal anodes is impeded by challenges such as dendrite formation and the inherent instability of the native oxide layer.This study introduces a novel liquid-source plasma technique to create a high-quality solid electrolyte interphase(SEI)composed of LiBr and LiBO_(2).According to first-principal calculation,LiBO_(2)optimizes the electrochemical dynamics and LiBr improves Li diffusion at the interfaces,thus protecting the Li metal from severe Li dendrite growth.This well-designed artificial SEI endows the Li metal with remarkable cycling stability over 550 cycles at a current density of 1 m A/cm^(2),significantly superior to the bare Li anode.Meanwhile,the full cell paired with a high-voltage LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode delivers long-term stability with capacity retention(78%after 200 cycles)at 1 C and excellent rate performance.The findings highlight the importance of interface engineering in optimizing battery performance and longevity.展开更多
Lithium metal is a compelling choice as an anode material for high-energy-density batteries,attributed to its elevated theoretical specific energy and low redox potential.Nevertheless,challenges arise due to its susce...Lithium metal is a compelling choice as an anode material for high-energy-density batteries,attributed to its elevated theoretical specific energy and low redox potential.Nevertheless,challenges arise due to its susceptibility to high-volume changes and the tendency for dendritic development during cycling,leading to restricted cycle life and diminished Coulombic efficiency(CE).Here,we innovatively engineered a kind of porous biocarbon to serve as the framework for a lithium metal anode,which boasts a heightened specific surface area and uniformly dispersed ZnO active sites,directly derived from metasequoia cambium.The porous structure efficiently mitigates local current density and alleviates the volume expansion of lithium.Also,incorporating the ZnO lithiophilic site notably reduces the nucleation overpotential to a mere 16 mV,facilitating the deposition of lithium in a compact form.As a result,this innovative material ensures an impressive CE of 98.5%for lithium plating/stripping over 500 cycles,a remarkable cycle life exceeding 1200 h in a Li symmetrical cell,and more than 82%capacity retention ratio after an astonishing 690 cycles in full cells.In all,such a rationally designed Li composite anode effectively mitigates volume change,enhances lithophilicity,and reduces local current density,thereby inhibiting dendrite formation.The preparation of a highperformance lithium anode frame proves the feasibility of using biocarbon in a lithium anode frame.展开更多
Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and l...Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.展开更多
Lithium(Li) metal is considered as the most promising anode material for the next-generation high performance Li batteries.However,the uncontrollable dendritic growth impedes its commercial application.Herein,we desig...Lithium(Li) metal is considered as the most promising anode material for the next-generation high performance Li batteries.However,the uncontrollable dendritic growth impedes its commercial application.Herein,we design a 3 D Si@carbon nanofibers(CNFs)@ZnO-ZnO-Cu skeleton(SCZ) for guiding the homogeneous bottom-growth of Li metal.The top LixSi@CNFs and bottom LiyZn@CNFs layers could form conductivity and overpotential gradient to avoid the "top-growth" of Li metal.Moreover,the top lithiophilic LixSi@CNFs layer could regulate the nucleation and deposition of Li-ions even if the lithium dendrites grow out of the skeleton under high capacity Li deposition(30 mAh cm^(-2)).As a result,the SCZ-Li||LiFePO_(4) full cell delivers a high capacity of ~104 mAh g^(-1)(~94.82% capacity retention) after 2000 cycles at 5 C, elucidating the potential application of the 3 D double-gradient Li metal composite anode.展开更多
In the light of wireless and non-fossil society based on portable electronics, electric vehicles, and smart grids, secondary batteries with higher energy density, faster charge, and safer operation are pursued persist...In the light of wireless and non-fossil society based on portable electronics, electric vehicles, and smart grids, secondary batteries with higher energy density, faster charge, and safer operation are pursued persistently [1]. Nowadays, commercial lithium(Li)-ion batteries have been practically applied in our daily life. However,the energy density of Li-ion batteries based on intercalation chemistry is approaching to the theoretical value due to the limited specific capacity of graphite anode(372 mA h g-1) [2].展开更多
The interfacial stability of lithium metal anodes dictated by solid electrolyte interphase(SEI) is essential for long-cycling high-energy-density lithium–sulfur batteries. Nevertheless, critical components of SEI for...The interfacial stability of lithium metal anodes dictated by solid electrolyte interphase(SEI) is essential for long-cycling high-energy-density lithium–sulfur batteries. Nevertheless, critical components of SEI for interfacial stabilization are particularly indistinct. Herein, the effect of various sulfur-containing components in SEI for stabilizing lithium metal anodes is disclosed in lithium–sulfur batteries. High-valence sulfur-containing species(Li_(2)SO_(3) and Li_(2)SO_(4)) in SEI are conducive to uniform lithium deposition and stabilizing lithium metal anodes. In contrast, low-valence sulfur-containing species(Li_(2)S_(3) and Li_(2)S_(4)) in SEI result in aggressive lithium dendrites and dead lithium. This work identifies the role of sulfurcontaining components in SEI for stabilizing lithium metal anodes and provides rational design principles of SEI for protecting lithium metal anodes in practical lithium–sulfur batteries.展开更多
Unambiguous understanding in lithium anode failure mechanism calls for a comprehensive methodology to investigate the coupled morphological,electrochemical and mechanical behaviors during the stripping process.In this...Unambiguous understanding in lithium anode failure mechanism calls for a comprehensive methodology to investigate the coupled morphological,electrochemical and mechanical behaviors during the stripping process.In this work,a mechanistic investigation of the pitting behavior of lithium metal in an electrolyte containing lithium polysulfides in lithium sulfur batteries was developed.It is found that lithium polysulfides could aggravate the nonuniform stripping of lithium electrodes.展开更多
Lithium-sulfur(Li-S) battery is considered as a promising energy storage system to realize high energy density.Nevertheless,unstable lithium metal anode emerges as the bottleneck toward practical applications,especial...Lithium-sulfur(Li-S) battery is considered as a promising energy storage system to realize high energy density.Nevertheless,unstable lithium metal anode emerges as the bottleneck toward practical applications,especially with limited anode excess required in a working full cell.In this contribution,a mixed diisopropyl ether-based(mixed-DIPE) electrolyte was proposed to effectively protect lithium metal anode in Li-S batteries with sulfurized polyacrylonitrile(SPAN) cathodes.The mixed-DIPE electrolyte improves the compatibility to lithium metal and suppresses the dissolution of lithium polysulfides,rendering significantly improved cycling stability.Concretely,Li | Cu half-cells with the mixed-DIPE electrolyte cycled stably for 120 cycles,which is nearly five times longer than that with routine carbonate-based electrolyte.Moreover,the mixedDIPE electrolyte contributed to a doubled life span of 156 cycles at 0.5 C in Li | SPAN full cells with ultrathin 50 μm Li metal anodes compared with the routine electrolyte.This contribution affords an effective electrolyte formula for Li metal anode protection and is expected to propel the practical applications of high-energy-density Li-S batteries.展开更多
基金Project(2016YFB0300801)supported by the National Key Research and Development Program of ChinaProject(2012CB619502)supported by the National Basic Research Program of China
文摘Lithium metal is one of the most promising anode materials for rechargeable battery with high energy density,but its practical use is still hindered by two main problems,namely,lithium dendrite growth and low Coulombic efficiency.To address the issues,cesium nitrate(CsNO3)is selected as the additive to modify the electrolyte for lithium secondary battery.Here we report electrochemical performance of lithium secondary battery with different concentration of CsNO3 as electrolyte additive.The study result demonstrates that Coulombic efficiency of Li–Cu cells and the lifetime of symmetric lithium cells contained CsNO3 additive are improved greatly.Li–Cu cell with 0.05 mol/L CsNO3 and 0.15 mol/L LiNO3 as electrolyte additive presents the best electrochemical performance,having the highest Coulombic efficiency of around 97%and the lowest interfacial resistance.With increasing the concentration of CsNO3 as electrolyte additive,the electrochemical performance of cells becomes poor.Meanwhile,the morphology of lithium deposited films with CsNO3-modified electrolyte become smoother and more uniform compared with the basic electrolyte.
基金supported by the National Natural Science Foundation of China(22078251)the National Key R&D Program of China(2021YFB2012000)+1 种基金the Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices of Ministry of Education,Jianghan University(JDGD-202211)the Graduate Innovation Fund of Wuhan Institute of Technology(CX2021014)。
文摘The uncontrolled dendrite growth of lithium metal anodes(LMAs)caused by unstable anode/electrolyte interface and uneven lithium deposition have impeded the practical applications of lithium metal batteries(LMBs).Constructing a robust artificial solid electrolyte interphase(SEI)and regulating the lithium deposition behavior is an effective strategy to address these issues.Herein,a three-dimensional(3D)lithium anode with gradient Li_(3)N has been in-situ fabricated on carbon-based framework by thermal diffusion method(denoted as CC/Li/Li_(3)N).Density functional theory(DFT)calculations reveal that Li_(3)N can effectively promote the transport of Li^(+)due to the low energy barrier of Li^(+)diffusion.As expected,the Li_(3)N-rich conformal artificial SEI film can not only effectively stabilize the interface and avoid parasitic reactions,but also facilitate fast Li^(+)transport across the SEI layer.The anode matrix with uniformly distributed Li3N can enable homogenous deposition of Li,thus preventing Li dendrite propagation.Benefiting from these merits,the CC/Li/Li_(3)N anode achieves ultralong-term cycling for>1000 h at a current density of 2 m A cm^(-2)and dendrite-free Li deposition at an ultrahigh rate of 20 m A cm^(-2).Moreover,the full cells coupled with LiFePO4cathodes show extraordinary cycling stability for>300 cycles in liquidelectrolyte-based batteries and display a high-capacity retention of 96.7%after 100 cycles in solid-state cells,demonstrating the promising prospects for the practical applications of LMBs.
基金supported by the National Key Research and Development Program of China(Grant No.2016YFB0100100)the National Natural Science Foundation of China(Grants Nos.52315206 and 51502334)the Fund from Beijing Municipal Science&Technology Commission,China(Grants No.D171100005517001)
文摘The effects of different coating layers on lithium metal anode formed by reacting with different controlled atmospheres（argon,CO_2–O_2（2：1）,N_2,and CO_2–O_2–N_2（2：1：3））have been investigated.The obtained XRD,second ion mass spectroscopy（SIMS）,and scanning probe microscope（SPM）results demonstrate the formation of coating layers composed of Li_2CO_3,Li_3N,and the mixture of them on lithium tablets,respectively.The Li/Li symmetrical cell and Li/S cell are assembled to prove the advantages of the protected lithium tablet on electrochemical performance.The comparison of SEM and SIMS characterizations before/after cycles clarifies that an SEI-like composition formed on the lithium tablets could modulate the interfacial stabilization between the lithium foil and the ether electrolyte.
基金supported by National Natural Science Foundation of China(Nos.21701083,22279112)Fok Ying-Tong Education Foundation of China(No.171064)Natural Science Foundation of Hebei Province(Nos.B2022203018,B2018203297).
文摘In the development of 3D conductive frameworks for lithium metal anode(LMA),two models have been proposed:top growth model and bottom-up growth model.However,Li tends to accumulate on the top of these 3D frameworks with homogenous lithiophilicity(top growth)and Li dendrite still forms.To address this issue,some researchers have focused on developing 3D frameworks with gradient lithio-philicity,which realized bottom-up growth of Li.Nevertheless,partial Li nucleation sites on the top of these frameworks were missed.Inspired by the two models talked above,this work firstly proposed a novel intermittent lithiophilic model for lithium deposition.To demonstrate the feasibility of this model,a bimetallic metal-organic frameworks derived ZnMn_(2)O_(4)-MnO nanoparticles were grown on carbon cloth for LMA.It can cycle stably under ultra-high current and areal capacity(10 mA/cm^(2),10 mAh/cm^(2)).The in-situ optical microscopy(OM)was conducted to observe the Li deposition behavior,no dendrite was found during 80 h in ester-based electrolyte while the pure Li only cycled for 2h.What is more,it can also be well-coupled with LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathode and solid-state electrolyte,which further prove the advantages of the intermittent model for the development of LMAs with high safety and high energy density.
基金financially supported by the Natural Science Foundation of Hunan Province(2020JJ5653)the National Natural Science Foundation of China(21875282,22102212)+1 种基金the National University of Defense Technology Scientific Research Project(ZK20-44)financial support from the Ministry of Science and Higher Education of the Russian Federation(075-15-2022-1150)。
文摘Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuing higher energy density,of which application has been challenged due to the unstable interface caused by the non-uniform electrodeposition as well as high chemical activity.Operating at higher temperature can be recommended to uniform electrodeposition of Li metal.Nevertheless,the intrinsic side-reaction between Li metal anode and electrolyte is inevitably aggravated and thus fosters the failure of Li metal anode rapidly with uneven electrodeposition.Here,a kind of temperature-tolerated ionic liquid(1-methyl-3-ethylimidazole bis(fluorosulfo nyl)imide/lithium bis(trifluoromethylsulfo nyl)imide,EF/LT)based electrolyte that matrixed with poly(vinylidene fluoride-hexafluoropropylene) was designed to maintain the interfacial stabilization of Li metal due to the weak interfacial reaction and uniform electrodeposition at high temperature of 80℃.It is the matter that the 660-h cycle with lower polarization is achieved with EF/LT-based electrolyte at temperature of 80 ℃ and the full cell embraces outstanding cyclic performance,without capacity fading within 100 cycles.Delighting,a door for practical application of Li metal anode for higher energy density as the carbon neutrality progresses in the blooming human society has been opened gradually.
基金financially supported by the Beijing Municipal Science and Technology Project(Nos.Z171100000917021 and Z181100004518003)。
文摘Lithium(Li)metal is the most promising electrode for next-gene ration rechargeable batteries.In order to push the commercialization of the lithium metal batteries,a kind of nitrogen(N)-doped composite graphene(NCG)adopted as the Li plating host was prepared to regulate Li metal nucleation and suppress dendrite growth.Furthermore,a new kind of sandwich-type composite lithium metal(STCL)electrode was developed to improve its application.The STCL electrode can be used as convenient as a piece of Li foil but no dendrite growth.In a symmetric battery,the STCL electrode cycled for more than 4500 h with the overpotential of less than 40 mV.And due to the creative design,the STCL promises the Li-S battery with a prolonged cycling lifespan.
基金support from the National Natural Science Foundation of China(No.U2333210)the Sichuan Science and Technology Program,China(No.21SYSX0011)。
文摘Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.
基金supported by the Qingdao Jiuhuanxinyue New Energy Technology Co.,Ltd.the Guangdong Basic and Applied Basic Research Foundation(Grant No.2021B1515120071)+2 种基金the 21C Innovation Laboratory,Contemporary Amperex Technology Ltd.(Grant No.21C-OP-202112)the financial support from the Guangdong Basic and Applied Basic Research Foundation(Grant No.2024A1515011873)the Shenzhen Science and Technology Program(Grant No.JCYJ20220531095212027).
文摘Li metal is widely recognized as the desired anode for next-generation energy storage,Li metal batteries,due to its highest theoretical capacity and lowest potential.Nonetheless,it suffers from unstable electrochemical behaviors like dendrite growth and side reactions in practical application.Herein,we report a highly stable anode with collector,Li_(5)Mg@Cu,realized by the melting-rolling process.The Li_(5)Mg@Cu anode delivers ultrahigh cycle stability for 2000 and 1000 h at the current densities of 1 and 2 mA cm^(-2),respectively in symmetric cells.Meanwhile,the Li_(5)Mg@Cu|LFP cell exhibits a high-capacity retention of 91.8% for 1000 cycles and 78.8% for 2000 cycles at 1 C.Moreover,we investigate the suppression effects of Mg on the dendrite growth by studying the performance of Li_(x)Mg@Cu electrodes with different Mg contents(2.0-16.7 at%).The exchange current density,surface energy,Li^(+)diffusion coefficient,and chemical stability of Li_(x)Mg@Cu concretely reveal this improving suppression effect when Mg content becomes higher.In addition,a Mg-rich phase with“hollow brick”morphology forming in the high Mg content Li_(x)Mg@Cu guides the uniform deposition of Li.This study reveals the suppression effects of Mg on Li dendrites growth and offers a perspective for finding the optimal component of Li-Mg alloys.
基金financially supported by the National Natural Science Foundation of China(52472093,52176185)the Department of Science and Technology of Hubei Province of China(2022CFA069,2022BAA086)。
文摘The disorganized lithium dendrites and unstable solid electrolyte interphase(SEI)severely impede the practical application of lithium metal batteries(LMBs).Herein,the N-Zn-F coordinated triazine-based covalent organic framework(TTA-COF-ZnF_(2))is fabricated for the first time as an artificial SEI layer on the surface of lithium metal anodes(LMAs)to handle these issues.Zn-N coordination in onedimensional(1D)ordered COF can increase lithiophilic sites,reduce the Li-nucleation barrier,and regulate the Li+local coordination environment by optimizing surface charge density around the Zn metal.The electron-rich state induced by strong electron-withdrawing F-groups constructs electronegative nanochannels,which trigger efficient Li+desolvation.These beneficial attributes boost Li^(+)transfer,and homogenize Li^(+)flux,leading to uniform Li deposition.Besides,the lithiophilic triazine ring polar groups in TTA-COF-ZnF_(2)further facilitate the Li^(+)migration.The latent working mechanism of adjusting Li deposition behaviors and stabilizing LMAs for TTA-COF-ZnF_(2)is illustrated by detailed in-situ/ex-situ characterizations and density functional theory(DFT)calculations.As expected,TTA-COF-ZnF_(2)-modified Li|Cu half cells deliver a higher Coulombic efficiency(CE)of 98.4% over 250 cycles and lower nucleation overpotential(11 mV)at 1 mA cm^(-2),while TTA-COF-ZnF_(2)@Li symmetric cells display a long lifespan over3785 h at 2 mA cm^(-2).The TTA-COF-ZnF_(2)@Li|S full cells exert ultra high capacity retention of 81%(837 mA h g^(-1))after 600 cycles at 1C.Besides,the TTA-COF-ZnF_(2)@Li|LFP full cells with a high loading of 7.1 mg cm^(-2)exert ultrahigh capacity retention of 89%(108 mAh g^(-1))after 700 cycles at 5C.This synergistic strategy in N-Zn-F coordinated triazine-based COF provides a new insight to regulate the uniform platins/stripping behaviors for developing ultra-stable and dendrite-free LMBs.
基金supported by the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.GTL24011-000)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS-2023-00272863)supported by Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea Government(MOTIE)(P0012748,HRD Program for Industrial Innovation)。
文摘This study presents a novel Li metal host material with a unique hollow nano-spherical structure that incorporates Ag nano-seeds into a graphitic carbon nitride(g-C_(3)N_(4))shell layer,referred to as g-C_(3)N_(4)@Ag hollow spheres.The g-C_(3)N_(4)@Ag spheres provide a managed internal site for Li metal encapsulation and promote stable Li plating.The g-C_(3)N_(4) spheres are uniformly coated using polydopamine,which has an adhesive nature,to enhance lithium plating/stripping stability.The strategic presence of Ag nano-seeds eliminates the nucleation barrier,properly directing Li growth within the hollow spheres.This design facilitates highly reversible and consistent lithium deposition,offering a promising direction for the production of high-performance lithium metal anodes.These well-designed g-C_(3)N_(4)@Ag hollow spheres ensure stable Li plating/stripping kinetics over more than 500 cycles with a high coulombic efficiency of over 97%.Furthermore,a full cell made using LiNi_(0.90)Co_(0.07)Mn_(0.03)O_(2) and Li-g-C_(3)N_(4)@Ag host electrodes demonstrated highly competitive performance over 200 cycles,providing a guide for the implementation of this technology in advanced lithium metal batteries.
基金Financial support from National Key R&D Program(2022YFB2404600)Natural Science Foundation of China(Key Project of 52131306)+1 种基金Project on Carbon Emission Peak and Neutrality of Jiangsu Province(BE2022031-4)the Big Data Computing Center of Southeast University are greatly appreciated.
文摘The replacement of non-aqueous organic electrolytes with solid-state electrolytes(SSEs)in solid-state lithium metal batteries(SLMBs)is considered a promising strategy to address the constraints of lithium-ion batteries,especially in terms of energy density and reliability.Nevertheless,few SLMBs can deliver the required cycling performance and long-term stability for practical use,primarily due to suboptimal interface properties.Given the diverse solidification pathways leading to different interface characteristics,it is crucial to pinpoint the source of interface deterioration and develop appropriate remedies.This review focuses on Li|SSE interface issues between lithium metal anode and SSE,discussing recent advancements in the understanding of(electro)chemistry,the impact of defects,and interface evolutions that vary among different SSE species.The state-ofthe-art strategies concerning modified SEI,artificial interlayer,surface architecture,and composite structure are summarized and delved into the internal relationships between interface characteristics and performance enhancements.The current challenges and opportunities in characterizing and modifying the Li|SSE interface are suggested as potential directions for achieving practical SLMBs.
基金supported by Yunnan Natural Science Foundation Project(No.202202AG050003)Yunnan Fundamental Research Projects(Nos.202101BE070001-018 and 202201AT070070)+1 种基金the National Youth Talent Support Program of Yunnan Province China(No.YNQR-QNRC-2020-011)Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects(No.2023-XMDJ-00617107)。
文摘Lithium metal has emerged as a highly promising anode material for enhancing the energy density of secondary batteries,attributed to its high theoretical specific capacity and low electrochemical potential.However,safety concerns related to lithium dendrite-induced short circuits and suboptimal electrochemical performance have impeded the commercial viability of lithium metal batteries.Current research efforts primarily focus on altering the solvated structure of Li+by modifying the current collector or introducing electrolyte additives to lower the nucleation barrier,expedite the desolvation process,and suppress the growth of lithium dendrites.Nevertheless,an integrated approach that combines the advantages of these two strategies remains elusive.In this study,we successfully employed metal-organic salt additives with lithophilic properties to accelerate the desolvation process,reduce the nucleation barrier of Li+,and modulate its solvated structure.This approach enhanced the inorganic compound content in the solid electrolyte interphase(SEI)on lithium foil surfaces,leading to stable Li+deposition and stripping.Specifically,Li||Cu cells demonstrated excellent cycle life and Coulombic efficiency(97.28%and 98.59%,respectively)at 0.5 m A/cm^(2)@0.5 m Ah/cm^(2)and 1 m A/cm^(2)@1 m Ah/cm^(2)for 410 and 240 cycles,respectively.Li||Li symmetrical cells showed no short circuit at 1 m A/cm^(2)@1 m Ah/cm^(2)for 1150 h,and Li||LFP full cells retained 68.9%of their capacity(104.6 m Ah/g)after 250 cycles at N/P(1.1:1.0)with a current density of 1C.
基金supported by National Natural Science Foundation of China(Nos.52372235,52073252,52002052,U20A20253,21972127,22279116)Key Scientific Research Project of Hangzhou(No.2024SZD1B12)+5 种基金Science and Technology Department of Zhejiang Province(Nos.2023C01231,Q23E020046,LD22E020006LY21E020005)Key Research and Development Project of Science and Technology Department of Sichuan Province(No.2022YFSY0004)Natural Science Foundation of Zhejiang Province(No.LQ23E020009)Sichuan Natural Science(No.2024NSFSC0951)Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology),Ministry of Education(No.KFM 202303)。
文摘The escalating demand for advanced energy storage solutions has positioned lithium metal anodes at the forefront of battery technology research.However,the practical implementation of lithium metal anodes is impeded by challenges such as dendrite formation and the inherent instability of the native oxide layer.This study introduces a novel liquid-source plasma technique to create a high-quality solid electrolyte interphase(SEI)composed of LiBr and LiBO_(2).According to first-principal calculation,LiBO_(2)optimizes the electrochemical dynamics and LiBr improves Li diffusion at the interfaces,thus protecting the Li metal from severe Li dendrite growth.This well-designed artificial SEI endows the Li metal with remarkable cycling stability over 550 cycles at a current density of 1 m A/cm^(2),significantly superior to the bare Li anode.Meanwhile,the full cell paired with a high-voltage LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode delivers long-term stability with capacity retention(78%after 200 cycles)at 1 C and excellent rate performance.The findings highlight the importance of interface engineering in optimizing battery performance and longevity.
基金supported by the National Natural Science Foundation of China(22179005,92372207)Fundamental Research Funds for the Central Universities(2022CX01017).
文摘Lithium metal is a compelling choice as an anode material for high-energy-density batteries,attributed to its elevated theoretical specific energy and low redox potential.Nevertheless,challenges arise due to its susceptibility to high-volume changes and the tendency for dendritic development during cycling,leading to restricted cycle life and diminished Coulombic efficiency(CE).Here,we innovatively engineered a kind of porous biocarbon to serve as the framework for a lithium metal anode,which boasts a heightened specific surface area and uniformly dispersed ZnO active sites,directly derived from metasequoia cambium.The porous structure efficiently mitigates local current density and alleviates the volume expansion of lithium.Also,incorporating the ZnO lithiophilic site notably reduces the nucleation overpotential to a mere 16 mV,facilitating the deposition of lithium in a compact form.As a result,this innovative material ensures an impressive CE of 98.5%for lithium plating/stripping over 500 cycles,a remarkable cycle life exceeding 1200 h in a Li symmetrical cell,and more than 82%capacity retention ratio after an astonishing 690 cycles in full cells.In all,such a rationally designed Li composite anode effectively mitigates volume change,enhances lithophilicity,and reduces local current density,thereby inhibiting dendrite formation.The preparation of a highperformance lithium anode frame proves the feasibility of using biocarbon in a lithium anode frame.
基金supported by the Yunnan Fundamental Research Projects(Grant Nos.202401AU070163 and 202501AT070298)the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects(Grant No.2023-XMDJ-00617107)+5 种基金the University Service Key Industry Project of Yunnan Province(Grant No.FWCY-ZD2024005)the Expert Workstation Support Project of Yunnan Province(Grant No.202405AF140069)the Scientific Research Foundation of Kunming University of Science and Technology(Grant No.20220122)the Analysis and Test Foundation of Kunming University of Science and Technology(Grant No.2023T20220122)the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2025QN02057)the Ordos City Strategic Pioneering Science and Technology Special Program for New Energy(Grant No.DC2400003365).
文摘Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.
基金financial support from the National Natural Science Foundation of China(Grant Nos.51701169,51871188 and 51931006)the National Key R&D Program of China(Grant No.2016YFA0202602)+1 种基金the Natural Science Foundation of Fujian Province of China(No.2019J06003)the "Double-First Class" Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen University。
文摘Lithium(Li) metal is considered as the most promising anode material for the next-generation high performance Li batteries.However,the uncontrollable dendritic growth impedes its commercial application.Herein,we design a 3 D Si@carbon nanofibers(CNFs)@ZnO-ZnO-Cu skeleton(SCZ) for guiding the homogeneous bottom-growth of Li metal.The top LixSi@CNFs and bottom LiyZn@CNFs layers could form conductivity and overpotential gradient to avoid the "top-growth" of Li metal.Moreover,the top lithiophilic LixSi@CNFs layer could regulate the nucleation and deposition of Li-ions even if the lithium dendrites grow out of the skeleton under high capacity Li deposition(30 mAh cm^(-2)).As a result,the SCZ-Li||LiFePO_(4) full cell delivers a high capacity of ~104 mAh g^(-1)(~94.82% capacity retention) after 2000 cycles at 5 C, elucidating the potential application of the 3 D double-gradient Li metal composite anode.
基金supported by the National Key Research and Development Program (2016YFA0202500 and 2016YFA0200102)the National Natural Science Foundation of China (21676160, 21825501, and U1801257)Tsinghua University Initiative Scientific Research Program。
文摘In the light of wireless and non-fossil society based on portable electronics, electric vehicles, and smart grids, secondary batteries with higher energy density, faster charge, and safer operation are pursued persistently [1]. Nowadays, commercial lithium(Li)-ion batteries have been practically applied in our daily life. However,the energy density of Li-ion batteries based on intercalation chemistry is approaching to the theoretical value due to the limited specific capacity of graphite anode(372 mA h g-1) [2].
基金supported by the Beijing Municipal Natural Science Foundation (Z20J00043)the National Natural Science Foundation of China (22061132002, 21825501)+4 种基金the China Postdoctoral Science Foundation (2021M700404)the Seed Fund of Shanxi Research Institute for Clean Energy (SXKYJF015)the Beijing Municipal Natural Science Foundation (JQ20004, L182021)the Beijing Institute of Technology Research Fund Program for Young Scholarsthe Tsinghua University Initiative Scientific Research Program。
文摘The interfacial stability of lithium metal anodes dictated by solid electrolyte interphase(SEI) is essential for long-cycling high-energy-density lithium–sulfur batteries. Nevertheless, critical components of SEI for interfacial stabilization are particularly indistinct. Herein, the effect of various sulfur-containing components in SEI for stabilizing lithium metal anodes is disclosed in lithium–sulfur batteries. High-valence sulfur-containing species(Li_(2)SO_(3) and Li_(2)SO_(4)) in SEI are conducive to uniform lithium deposition and stabilizing lithium metal anodes. In contrast, low-valence sulfur-containing species(Li_(2)S_(3) and Li_(2)S_(4)) in SEI result in aggressive lithium dendrites and dead lithium. This work identifies the role of sulfurcontaining components in SEI for stabilizing lithium metal anodes and provides rational design principles of SEI for protecting lithium metal anodes in practical lithium–sulfur batteries.
基金supported by the National Key Research and Development Program of China(Grant No.2017YFA0206700,2017YFA0402802)the National Natural Science Foundation of China(Grant.No.21776265)Anhui Provincial Natural Science Foundation(Grant No.1908085ME122)。
文摘Unambiguous understanding in lithium anode failure mechanism calls for a comprehensive methodology to investigate the coupled morphological,electrochemical and mechanical behaviors during the stripping process.In this work,a mechanistic investigation of the pitting behavior of lithium metal in an electrolyte containing lithium polysulfides in lithium sulfur batteries was developed.It is found that lithium polysulfides could aggravate the nonuniform stripping of lithium electrodes.
基金supported by National Key Research and Development Program(2016YFA0202500 and 2016YFA0200102)National Natural Science Foundation of China(21776019,21825501,and U1801257)the Tsinghua University Initiative Scientific Research Program
文摘Lithium-sulfur(Li-S) battery is considered as a promising energy storage system to realize high energy density.Nevertheless,unstable lithium metal anode emerges as the bottleneck toward practical applications,especially with limited anode excess required in a working full cell.In this contribution,a mixed diisopropyl ether-based(mixed-DIPE) electrolyte was proposed to effectively protect lithium metal anode in Li-S batteries with sulfurized polyacrylonitrile(SPAN) cathodes.The mixed-DIPE electrolyte improves the compatibility to lithium metal and suppresses the dissolution of lithium polysulfides,rendering significantly improved cycling stability.Concretely,Li | Cu half-cells with the mixed-DIPE electrolyte cycled stably for 120 cycles,which is nearly five times longer than that with routine carbonate-based electrolyte.Moreover,the mixedDIPE electrolyte contributed to a doubled life span of 156 cycles at 0.5 C in Li | SPAN full cells with ultrathin 50 μm Li metal anodes compared with the routine electrolyte.This contribution affords an effective electrolyte formula for Li metal anode protection and is expected to propel the practical applications of high-energy-density Li-S batteries.
