Energy Materials and Devices(EMD)is a quarterly academic journal sponsored by Tsinghua University.The journal aims to present the up-to-date scientific achievements of high creativity and great significance in the cut...Energy Materials and Devices(EMD)is a quarterly academic journal sponsored by Tsinghua University.The journal aims to present the up-to-date scientific achievements of high creativity and great significance in the cutting-edge field of energy materials and devices.Contributions from all over the world are welcomed.展开更多
Aqueous zinc-based energy storage systems offer high theoretical specific capacity,low cost,intrinsic safety,and environmental compatibility,positioning them as promising candidates for next-generation energy storage ...Aqueous zinc-based energy storage systems offer high theoretical specific capacity,low cost,intrinsic safety,and environmental compatibility,positioning them as promising candidates for next-generation energy storage and conversion technologies.However,issues such as zinc dendrite growth,hydrogen evolution reaction(HER),and surface passivation hinder their practical deployment.To address these challenges,a hollow nanotubular magnesium silicate(denoted MgSi)interfacial layer was constructed on the zinc metal anode(Zn@MgSi).The unique layer structure and negatively charged surface of MgSi facilitate the desolvation of[Zn(H_(2)O)_(6)]^(2+)by stripping water molecules,while temporarily immobilizing Zn^(2+)to suppress random diffusion.The combined effects of the electric field-guided Zn^(2+)distribution and rapid ion transport through the layer structure co-regulate Zn^(2+)flux,leading to uniform,dendrite-free zinc deposition.Consequently,the Zn@MgSi symmetric cell demonstrates a high Zn^(2+)transference number(0.64),extended cycling life exceeding 1600 h at 1 mA cm^(−2),and stable operation for 200 h at 5 mA cm^(−2).Furthermore,zinc-ion hybrid capacitors employing Zn@MgSi electrodes exhibit excellent cycling stability over 5000 cycles.This work highlights the efficacy of artificial interfacial layers in stabilizing zinc metal anodes and provides valuable insights into the development of advanced aqueous zinc-ion energy storage systems.展开更多
Composite solid-state electrolytes have received significant attention due to their combined advantages as inorganic and polymer electrolytes.However,conventional ceramic fillers offer limited ion conductivity enhance...Composite solid-state electrolytes have received significant attention due to their combined advantages as inorganic and polymer electrolytes.However,conventional ceramic fillers offer limited ion conductivity enhancement for composite solid-state electrolytes due to the space-charge layer between the polymer matrix and ceramic phase.In this study,we develop a ferroelectric ceramic ion conductor(LiTaO_(3))as a func-tional filler to simultaneously alleviate the space-charge layer and provide an extra Li+transport pathway.The obtained composite solid-state electrolyte comprising LiTaO_(3)filler and poly(vinylidene difluoride)matrix(P-LTO15)achieves an ionic conductivity of 4.90×10^(−4)S cm−1 and a Li+transference number of 0.45.The polar-ized ferroelectric LiTaO_(3)creates a uniform electric field and promotes homogenous Li plating/stripping,providing the Li symmetrical batteries with an ultrastable cycle life for 4000 h at 0.1 mA cm^(−2)and a low polar-ization overpotential(~50 mV).Furthermore,the solid-state NCM811/P-LTO15/Li full batteries achieve an ultralong cycling performance(1400 cycles)at 1 C and a high discharge capacity of 102.1 mAh g^(−1)at 5 C.This work sheds light on the design of functional ceramic fillers for composite solid-state electrolytes to effec-tively enhance ion conductivity and battery performance.展开更多
Composite solid electrolytes(CSEs)are considered among the most promising candidates for solid-state batteries.However,their practical application is hindered by low ionic conductivity and a limited lithium-ion transf...Composite solid electrolytes(CSEs)are considered among the most promising candidates for solid-state batteries.However,their practical application is hindered by low ionic conductivity and a limited lithium-ion transference number,primarily owing to the insufficient mobility of Li+.In this work,we design a heterojunc-tion nanoparticle composed of bimetallic zeolitic imidazolate frameworks(ZIFs)coupled with amorphous tita-nium oxide(TiO_(2)@Zn/Co–ZIF)as a filler to fabricate a composite solid-state electrolyte(PVZT).The amor-phous TiO_(2) coating facilitates salt dissociation through Lewis acid–base interactions with the anions of the lithium salt.Meanwhile,the Zn/Co–ZIF framework not only provides additional selective pathways for Li+transport but also effectively restricts anion migration through its confined pore size.The synergistic effect results in a high room-temperature ionic conductivity(8.8×10^(-4) S·cm^(-1))and a lithium-ion transference number of 0.47 for PVZT.A symmetrical cell using PVZT demonstrates stable Li+deposition/stripping for over 1100 h at a current density of 0.1 mA·cm^(-2).Additionally,a LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)/Li full cell using PVZT retains 75.0%of its capacity after 1200 cycles at a 2 C rate.This work offers valuable insights into the design of func-tional fillers for CSEs with highly efficient ion transport.展开更多
Molybdenum disulfide(MoS_(2))has garnered significant attention as a potential substitute for Pt catalysts in the hydrogen evolution reaction(HER).Furthermore,there is a need to explore cost-effective and efficient el...Molybdenum disulfide(MoS_(2))has garnered significant attention as a potential substitute for Pt catalysts in the hydrogen evolution reaction(HER).Furthermore,there is a need to explore cost-effective and efficient elec-trocatalysts that can perform well across different pH levels.In this study,a straightforward hydrothermal method is presented to synthesize Ni,Co-doped MoS_(2)nanosheets on carbon fiber paper(Ni,Co-MoS_(2)/CFP)for HER in various pH environments.The findings suggest that strategic doping not only alters the structure and composition of Ni,Co-MoS_(2)/CFP but also enhances its inherent electrocatalytic activity while facilitating the transformation of the MoS_(2)phase.The overpotentials observed for Ni,Co-MoS_(2)/CFP are 95.6,154,and 144 mV(at 10 mA cm−2)under alkaline,acidic,and neutral environments respectively.The exceptional perfor-mance of Ni,Co-MoS_(2)/CFP in HER can be attributed to the introduction of nickel and cobalt dopants which increase porosity and expose more active sites.This one-step doping technique presents a novel approach to modulating catalytic activity across all pH ranges.展开更多
The intensifying challenges posed by climate change and the depletion of fossil fuels have spurred concerted global efforts to develop alternative energy storage solutions.Aqueous zinc-ion batteries(AZIBs)have emerged...The intensifying challenges posed by climate change and the depletion of fossil fuels have spurred concerted global efforts to develop alternative energy storage solutions.Aqueous zinc-ion batteries(AZIBs)have emerged as promising candidates for large-scale electrochemical energy storage systems because of their intrinsic safety,cost-effectiveness,and environmental sustainability.However,Zn dendrite growth consis-tently poses a remarkable challenge to the performance improvement and commercial viability of AZIBs.The use of three-dimensional porous Zn anodes instead of planar Zn plates has been demonstrated as an effec-tive strategy to regulate the deposition/stripping behavior of Zn2+ions,thereby inhibiting the dendrite growth.Here,the merits of porous Zn anodes were summarized,and a comprehensive overview of the recent advancements in the engineering of porous Zn metal anodes was provided,with a particular emphasis on the structural orderliness and critical role of porous structure modulation in enhancing battery performance.Furthermore,strategic insights into the design of porous Zn anodes were presented to facilitate the practical implementation of AZIBs for grid-scale energy storage applications.展开更多
With the boom in electric vehicles(EVs),there is an increasing demand for high-performance lithium-ion batteries.Lithium manganese iron phosphate(LMFP)has emerged as an enhanced variation of LiFePO4(LFP),offering an e...With the boom in electric vehicles(EVs),there is an increasing demand for high-performance lithium-ion batteries.Lithium manganese iron phosphate(LMFP)has emerged as an enhanced variation of LiFePO4(LFP),offering an energy density 10%–20%greater than that of LFP.Structural distortion caused by the Jahn–Teller effect decreases the capacity and voltage platform,thus restricting the commercialization of this material.Herein,ideas to overcome these challenges,including the crystal structure of LMFP and strategies to mitigate the Jahn–Teller distortion,are first explored.Then,the migration pathways of Li+during charging and discharging and the phase transition mechanisms that affect the material’s performance are discussed.Next,the optimal Mn:Fe ratio for achieving the desired performance is described.The influences of various synthesis and modification methods on the morphology and structure of LMFP are reviewed.Additionally,different modification techniques,such as doping and coating,to enhance the performance of LMFP are highlighted.Finally,an overview of the current state of research on the recycling and reuse of LMFP is provided.By addressing these key topics,this paper offers a theoretical foundation for the further development of LMFP,thus contributing to its eventual commercialization.展开更多
With the exponential growth of portable electronic devices and wearable technologies,batteries are currently required to deliver not only high energy density and extended cycling performance but also enhanced safety a...With the exponential growth of portable electronic devices and wearable technologies,batteries are currently required to deliver not only high energy density and extended cycling performance but also enhanced safety and exceptional durability.Inspired by the self-repair mechanism observed in natural systems,a self-healing strategy shows great application potential in enabling batteries to resist external physical and chemical damage.In this review,we provide a detailed exploration of the application of self-healing materials in battery components,including electrodes,electrolytes,and encapsulation layers.We also analyze the advantages and limitations of various self-healing mechanisms,highlighting their roles in optimizing battery performance.By presenting a comprehensive synthesis of existing research,the potential pathways for advancing the development of self-healing batteries are identified,as well as the key challenges and opportunities within this field.This review aims to promote the practical integration of self-healing batteries in smart and flexible electronic devices,paving the way for safer,more reliable,and long-lasting energy storage systems.展开更多
Wide-bandgap(WB)mixed-halide perovskite solar cells(PSCs)play a crucial role in perovskite-based tandem solar cells(TSCs),enabling them to exceed the Shockley-Queisser limits of single-junction solar cells.Nonetheless...Wide-bandgap(WB)mixed-halide perovskite solar cells(PSCs)play a crucial role in perovskite-based tandem solar cells(TSCs),enabling them to exceed the Shockley-Queisser limits of single-junction solar cells.Nonetheless,the lack of stability in WB perovskite films due to photoinduced phase segregation undermines the stability of WB PSCs and their TSCs,thus impeding the commercialization of perovskite-based TSCs.Many efforts have been made to suppress photoinduced phase segregation in WB perovskite films and significant progresses have been obtained.In this review,we elaborate the mechanisms behind photoinduced phase segregation and its impact on the photovoltaic performance and stability of devices.The importance role of advanced characterization techniques in confirming the photoinduced phase segregation are comprehensively summarized.Beyond that,the effective strategies to alleviate photoinduced phase segregation in WB mixed halide PSCs are systematically assessed.Finally,the prospects for developing highly efficient and stable WB PSCs in tandem application are also presented.展开更多
Here we report an interesting phenomenon that lithium plating from pre-cycling of Li-ion cells at low temperature could reduce degradation and extend cycle life at high temperature.This study confirmed the phenomenon ...Here we report an interesting phenomenon that lithium plating from pre-cycling of Li-ion cells at low temperature could reduce degradation and extend cycle life at high temperature.This study confirmed the phenomenon in both single-layer cells and multi-layer cells.It revealed that compression of the multi-layer cells must be maintained during cycling for the phenomenon to be observed.Without compression,lowtemperature pre-cycling would accelerate high-temperature degradation of the multi-layer cells.This finding helped to clarify the contradictions in previous studies on the effects of low-temperature pre-cycling.A comparison between low-temperature pre-cycling with 1C charging and 0.2C charging confirmed that lithium plating from low-temperature pre-cycling is necessary for the observed benefits.Furthermore,post-mortem analysis of single-layer cells showed a thick deposition layer on the anode of pre-cycled cells,which could be attributed to reactions from lithium plating and the electrolyte.展开更多
Zinc-ion batteries(ZIBs)have garnered significant interest owing to their intrinsic safety,environmental compatibility,and low cost.However,nonuniform Zn deposition and parasitic side reactions during cycling lead to ...Zinc-ion batteries(ZIBs)have garnered significant interest owing to their intrinsic safety,environmental compatibility,and low cost.However,nonuniform Zn deposition and parasitic side reactions during cycling lead to rapid capacity decay and potential short-circuiting.To address these challenges,we developed a carboxymethyl cellulose-zinc(CMC-Zn)hydrogel electrolyte with self-release capability using a metal-ion crosslinking approach.The dynamically reversible CMC-Zn network continuously supplies active Zn^(2+)during cycling,compensating for electrode consumption in real time.Abundant carboxylate and hydroxyl groups regulate uniform zinc nucleation and growth,while the hydrogen-bonding network synergistically suppresses side reactions,as reflected by a low hydrogen-evolution potential(−0.281 V)and reduced corrosion current density(0.03 mA cm^(−2)).With these advantages,Zn||Zn symmetric cells achieve an ultralong lifespan of 6,400 h at 0.5 mA cm^(−2),and Zn||Cu half-cells deliver a stable coulombic efficiency of 99.1%over 4,200 cycles.In fullcell testing,self-released Zn^(2+)contributes 29%of the overall capacity,enabling Zn||PANI cells to retain 75%capacity after 2,000 cycles and exhibit a rate-performance recovery of 97.4%.A corresponding flexible ZIB maintains stable operation under various deformation conditions,highlighting the strong potential of CMC-Zn hydrogel electrolytes for next-generation flexible energy-storage devices.展开更多
The attainment of carbon neutrality requires the development of aqueous energy conversion and storage devices.However,these devices exhibit limited performance due to the permeability-selectivity trade-off of permsele...The attainment of carbon neutrality requires the development of aqueous energy conversion and storage devices.However,these devices exhibit limited performance due to the permeability-selectivity trade-off of permselective membranes as core components.Herein,we report the application of a synergistic approach utilizing two-dimensional nanoribbons-entangled nanosheets to rationally balance the permeability and selec-tivity in permselective membranes.The nanoribbons and nanosheets can be self-assembled into a nanoflu-idic membrane with a distinctive“island-bridge”configuration,where the nanosheets serve as isolated islands offering adequate ionic selectivity owing to their high surface charge density,meanwhile bridge-like nanorib-bons with low surface charge density but high aspect ratio remarkably enhance the membrane’s permeability and water stability,as verified by molecular simulations and experimental investigations.Using this approach,we developed a high-performance graphene oxide(GO)nanosheet/GO nanoribbon(GONR)nanofluidic membrane and achieved an ultrahigh power density of 18.1 W m^(-2) in a natural seawater|river water osmotic power generator,along with a high Coulombic efficiency and an extended lifespan in zinc metal batteries.The validity of our island-bridge structural design is also demonstrated for other nanosheet/nanoribbon composite membranes,providing a promising path for developing reliable aqueous energy conversion and storage devices.展开更多
Rechargeable aqueous zinc-ion batteries(ZIBs)have gained attention as promising candidates for nextgeneration large-scale energy storage systems due to their advantages of improved safety,environmental sustainability,...Rechargeable aqueous zinc-ion batteries(ZIBs)have gained attention as promising candidates for nextgeneration large-scale energy storage systems due to their advantages of improved safety,environmental sustainability,and low cost.However,the zinc metal anode in aqueous ZIBs faces critical challenges,including dendrite growth,hydrogen evolution reactions,and corrosion,which severely compromise Coulombic efficiency and cycling stability,hindering their broader adoption.This review first explores the fundamental mechanisms underlying these challenges and then examines current strategies to address them,focusing on structural design,surface modifications,electrolyte optimization,and alloying treatments.Finally,potential future directions are discussed,outlining a pathway toward achieving high-performance aqueous ZIBs.展开更多
As lithium-ion batteries(LIBs)become increasingly widespread,ensuring their safety has become a primary concern.Particularly,battery aging has been reported to significantly impact major battery safety behaviors,inclu...As lithium-ion batteries(LIBs)become increasingly widespread,ensuring their safety has become a primary concern.Particularly,battery aging has been reported to significantly impact major battery safety behaviors,including the internal short circuit(ISC)and thermal runaway(TR).Over the past decade,despite consider-able research into the thermal hazards of aged batteries,the complexity of battery aging and TR mecha-nisms,along with the challenges posed by extreme experimental conditions,necessitates a systematic under-standing.Aiming to provide a comprehensive review of safety issues related to aged batteries,this paper begins by exploring the fundamental aging mechanisms and factors that accelerate aging.It then investi-gates how aging affects battery safety issues,including swelling and off-gassing behaviors.Furthermore,we discuss the impact of aging on TR problems induced by abusive conditions,covering safety issues from inter-nal sources to external abusive scenarios.This review offers valuable insights into understanding and predict-ing the thermal hazards of aged LIBs,which provides guidelines for designing and manufacturing safer LIBs and accurate and rapid battery safety prognostics in the future.展开更多
Two-dimensional(2D)nitrogen-doped graphene(NG)films have attracted considerable attention as promis-ing metal-free electrochemical catalysts for the oxygen reduction reaction(ORR).Thermal evaporation is a versatile th...Two-dimensional(2D)nitrogen-doped graphene(NG)films have attracted considerable attention as promis-ing metal-free electrochemical catalysts for the oxygen reduction reaction(ORR).Thermal evaporation is a versatile thin film deposition technique.However,the conventional thermal evaporation techniques present challenges in producing nitrogen-rich NG thin films because of the difficulties of a controllable manner for doping graphene with N atoms.To address this,we designed a vacuum thermal evaporation system for the large-scale preparation of 2D NG thin films.Using poly(2,5-benzimidazole)(ABPBI)as a nitrogen and carbon precursor,we deposited nitrogen-rich NG thin films with a size of 50×50 mm^(2) and controllable thickness within the range of 0.5–1.5 nm.The 2D NG samples exhibited a uniform thin film structure with moderate defects.The nitrogen-rich ABPBI precursor and defects,as well as the beneficial morphology and structure,endowed the optimal catalyst(2D NG-900)with a comparable ORR activity and superior stability compared with the commercial Pt/C(20 wt%)catalyst.This paper proposes a feasible strategy for fabricating 2D NG films as effective metal-free catalysts for the ORR.展开更多
Lithium-ion batteries are essential for modern energy storage,yet achieving simultaneous high-temperature and high-voltage operation remains challenging due to interfacial compatibility.In this study,we introduce a po...Lithium-ion batteries are essential for modern energy storage,yet achieving simultaneous high-temperature and high-voltage operation remains challenging due to interfacial compatibility.In this study,we introduce a polyetherimide(PEI)-polyimide(PI)functional coating on the separator that enhances wettability,thermal stability,and mechanical strength,while markedly improving cathode stability under harsh conditions.By integrating theoretical calculations with experimental validation,we demonstrate that the PEI/PI coating modulates the solvation structure of lithium-ions,thereby facilitating the interfacial desolvation process.More importantly,the PEI/PI layer regulates electrolyte decomposition at the interface,promoting the formation of a uniform and thermally stable cathode-electrolyte interphase.Consequently,LiCoO_(2)cathodes exhibit improved cycling performance at 60°C.Overall,this work underscores the pivotal role of separator coatings in governing interfacial chemistry and provides a viable strategy for designing high-performance lithium-ion batteries capable of enduring both high temperatures and high.展开更多
Owing to their high volumetric capacity,low cost and high safety,rechargeable aluminum batteries have become promising candidates for energy applications.However,the high charge density of Al^(3+)leads to strong coulo...Owing to their high volumetric capacity,low cost and high safety,rechargeable aluminum batteries have become promising candidates for energy applications.However,the high charge density of Al^(3+)leads to strong coulombic interactions between anions and the cathode,resulting in sluggish diffusion kinetics and irreversible collapse of the cathode structure.Furthermore,AlCl_(3)-based ionic liquids,which are commonly used as electrolytes in such batteries,corrode battery components and are prone to side reactions.The above problems lead to low capacity and poor cycling stability.Herein,we propose a reduced graphene oxide(rGO)cathode with a three-dimensional porous structure prepared using a simple and scalable method.The lamellar edges and oxygen-containing group defects of rGO synergistically provide abundant ion storage sites and enhance ion transfer kinetics.We matched the prepared rGO cathode with noncorrosive electrolyte 0.5 mol·L^(-1) Al(OTF)_(3)/[BMIM]OTF and Al metal to construct a high-performance battery,Al||rGO-150,with good cycling stability for 2700 cycles.Quasi-in-situ physicochemical characterization results show that the ion storage mechanism is codominated by diffusion and capacitance.The capacity consists of the insertion of Al-based species cations as well as synergistic adsorption of Al(OTF)_(x)^((3-x)+)(x<3)and[BMIM]+.The present study promotes the fundamental and applied research on rechargeable aluminum batteries.展开更多
Owing to their intrinsic safety and low cost,aqueous zinc-ion batteries(AZIBs)have emerged as promising large-scale energy storage devices.Hydrogel electrolytes have been extensively studied because of their superior ...Owing to their intrinsic safety and low cost,aqueous zinc-ion batteries(AZIBs)have emerged as promising large-scale energy storage devices.Hydrogel electrolytes have been extensively studied because of their superior electrochemical performance their ability to endow AZIBs with excellent flexibility.However,traditional hydrogel electrolytes typically suffer from a narrow electrochemical stability potential window(ESPW)and poor cycling stability,primarily due to their high water content.In recent years,lean-water hydrogel electrolytes(L-WHEs)have been developed to address these issues.By confining free water molecules and regulating ion transport within the hydrogel network,L-WHEs can efficiently suppress side reactions,widen the ESPW,and enhance interfacial stability.This review systematically discusses the fundamental principles of L-WHEs,current strategies for developing practical L-WHEs,and recent research progress.Finally,future prospect and challenges in the development of high-performance L-WHEs are outlined.展开更多
Manganese dioxide(MnO_(2)),based on a two-electron-transfer deposition/dissolution chemistry,features an ultrahigh theoretical capacity(616 mAh·g^(−1)),a favorable redox potential(1.23 V vs.the standard hydrogen ...Manganese dioxide(MnO_(2)),based on a two-electron-transfer deposition/dissolution chemistry,features an ultrahigh theoretical capacity(616 mAh·g^(−1)),a favorable redox potential(1.23 V vs.the standard hydrogen electrode),inherent nontoxicity,and low cost,making it a promising cathode candidate for high-energy aqueous batteries.However,its practical application is hindered by limited electrochemical reversibility and cycling stability,primarily attributed to the formation and accumulation of electrochemically inactive Mn species commonly known as“dead Mn”.This perspective provides an in-depth analysis of the“dead Mn”dilemma inherent in Mn^(2+)/MnO_(2) chemistry.First,the fundamental causes of“dead Mn”—insufficient electron supply and imbalanced(insufficient or excessive)proton supply,are systematically analyzed,as they detract from active material utilization,cycle life,and energy density.Then,mitigation strategies are examined from three aspects:preventing“dead Mn”formation caused by insufficient electron supply,mitigating“dead Mn”formation related to imbalanced proton supply,and activating and regenerating existing“dead Mn”.Finally,future research directions are visualized to enhance the practical viability of Mn^(2+)/MnO_(2) deposition/dissolution chemistry,aiming to catalyze advancements in high-energy aqueous battery systems.展开更多
Solid polymer electrolytes(SPEs)have attracted considerable attention for solid-state lithium-metal batteries(LMBs)with high energy density and enhanced safety for future applications.In this study,an SPE was devel-op...Solid polymer electrolytes(SPEs)have attracted considerable attention for solid-state lithium-metal batteries(LMBs)with high energy density and enhanced safety for future applications.In this study,an SPE was devel-oped based on a poly(ethyl acrylate)(PEA)polymer matrix with the vinylene carbonate(VC)additive(defined as PEA-VC)for high-voltage solid-state LMBs.Results show that introducing the VC additive into the PEA-based SPE leads to high lithium-ion conductivity(1.57 mS/cm at 22°C),a high lithium-ion transference number(0.73),and a wide electrochemical stability window(up to 4.9 V vs.Li/Li^(+)).The remarkable compatibil-ity of the PEA-VC SPE with lithium metal anodes and high-voltage cathodes was demonstrated in Li//Li symmetric cells(800 h lifetime at a current density of 0.1 mA/cm^(2) at 22°C)and Li//LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)full cells(with a capacity retention of 77.8%after 100 cycles at 0.2C).The improved stability is attributed to the introduction of the VC additive,which helps form a robust cathode–electrolyte interphase,effectively suppressing parasitic interface side reactions.Overall,this study highlights the role of VC addi-tives in high-voltage and solid-state LMBs,offering a general yet effective approach for addressing the interfa-cial instability issue through an additive-engineering strategy.展开更多
文摘Energy Materials and Devices(EMD)is a quarterly academic journal sponsored by Tsinghua University.The journal aims to present the up-to-date scientific achievements of high creativity and great significance in the cutting-edge field of energy materials and devices.Contributions from all over the world are welcomed.
基金the Doctoral Research Startup Fund of Hubei University of Science and Technology(Grant No.BK202504)the Natural Science Foundation of Liaoning Province(Grant No.2023-MS-115).
文摘Aqueous zinc-based energy storage systems offer high theoretical specific capacity,low cost,intrinsic safety,and environmental compatibility,positioning them as promising candidates for next-generation energy storage and conversion technologies.However,issues such as zinc dendrite growth,hydrogen evolution reaction(HER),and surface passivation hinder their practical deployment.To address these challenges,a hollow nanotubular magnesium silicate(denoted MgSi)interfacial layer was constructed on the zinc metal anode(Zn@MgSi).The unique layer structure and negatively charged surface of MgSi facilitate the desolvation of[Zn(H_(2)O)_(6)]^(2+)by stripping water molecules,while temporarily immobilizing Zn^(2+)to suppress random diffusion.The combined effects of the electric field-guided Zn^(2+)distribution and rapid ion transport through the layer structure co-regulate Zn^(2+)flux,leading to uniform,dendrite-free zinc deposition.Consequently,the Zn@MgSi symmetric cell demonstrates a high Zn^(2+)transference number(0.64),extended cycling life exceeding 1600 h at 1 mA cm^(−2),and stable operation for 200 h at 5 mA cm^(−2).Furthermore,zinc-ion hybrid capacitors employing Zn@MgSi electrodes exhibit excellent cycling stability over 5000 cycles.This work highlights the efficacy of artificial interfacial layers in stabilizing zinc metal anodes and provides valuable insights into the development of advanced aqueous zinc-ion energy storage systems.
基金supported by the National Natural Science Foundation of China(No.52325206,U2001220 and 52203298)Key-Area Research and Development Program of Guangdong Province(No.2020B090919001)+2 种基金Shenzhen.Shenzhen Outstanding Talents Training FundAll-Solid-State Lithium Battery Electrolyte Engineering Research Center(XMHT20200203006)Shenzhen Technical Plan Project(Nos.RCJC20200714114436091,YJ20220530143012027,JCYJ20220818101003007,JCYJ20220818101003008).
文摘Composite solid-state electrolytes have received significant attention due to their combined advantages as inorganic and polymer electrolytes.However,conventional ceramic fillers offer limited ion conductivity enhancement for composite solid-state electrolytes due to the space-charge layer between the polymer matrix and ceramic phase.In this study,we develop a ferroelectric ceramic ion conductor(LiTaO_(3))as a func-tional filler to simultaneously alleviate the space-charge layer and provide an extra Li+transport pathway.The obtained composite solid-state electrolyte comprising LiTaO_(3)filler and poly(vinylidene difluoride)matrix(P-LTO15)achieves an ionic conductivity of 4.90×10^(−4)S cm−1 and a Li+transference number of 0.45.The polar-ized ferroelectric LiTaO_(3)creates a uniform electric field and promotes homogenous Li plating/stripping,providing the Li symmetrical batteries with an ultrastable cycle life for 4000 h at 0.1 mA cm^(−2)and a low polar-ization overpotential(~50 mV).Furthermore,the solid-state NCM811/P-LTO15/Li full batteries achieve an ultralong cycling performance(1400 cycles)at 1 C and a high discharge capacity of 102.1 mAh g^(−1)at 5 C.This work sheds light on the design of functional ceramic fillers for composite solid-state electrolytes to effec-tively enhance ion conductivity and battery performance.
基金supported by National Science Fund for Distinguished Young Scholars(Grant No.52325206)National Key Research and Development Program of China(Grant No.2021YFF0500600)+3 种基金National Natural Science Foundation of China(Grant Nos.U2001220 and 52203298)Shenzhen Technical Plan Project(Grant Nos.RCJC20200714114436091,JCYJ20220530143012027,JCYJ20220818101003008,and JCYJ20220818101003007)Tsinghua Shenzhen International Graduate School-Shenzhen Pengrui Young Faculty Program of Shenzhen Pengrui Foundation(Grant No.SZPR2023006)Shenzhen Science and Technology Program(Grant No.WDZC20231126160733001).
文摘Composite solid electrolytes(CSEs)are considered among the most promising candidates for solid-state batteries.However,their practical application is hindered by low ionic conductivity and a limited lithium-ion transference number,primarily owing to the insufficient mobility of Li+.In this work,we design a heterojunc-tion nanoparticle composed of bimetallic zeolitic imidazolate frameworks(ZIFs)coupled with amorphous tita-nium oxide(TiO_(2)@Zn/Co–ZIF)as a filler to fabricate a composite solid-state electrolyte(PVZT).The amor-phous TiO_(2) coating facilitates salt dissociation through Lewis acid–base interactions with the anions of the lithium salt.Meanwhile,the Zn/Co–ZIF framework not only provides additional selective pathways for Li+transport but also effectively restricts anion migration through its confined pore size.The synergistic effect results in a high room-temperature ionic conductivity(8.8×10^(-4) S·cm^(-1))and a lithium-ion transference number of 0.47 for PVZT.A symmetrical cell using PVZT demonstrates stable Li+deposition/stripping for over 1100 h at a current density of 0.1 mA·cm^(-2).Additionally,a LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)/Li full cell using PVZT retains 75.0%of its capacity after 1200 cycles at a 2 C rate.This work offers valuable insights into the design of func-tional fillers for CSEs with highly efficient ion transport.
基金supported by the State Key Labora-tory of Heavy Oil Processing(SKLHOP202101006)the Project of Marine Science and Technology Synergy Innovation Center(CXZX-04-04-29)the National Natural Science Foundation of China(22078365).
文摘Molybdenum disulfide(MoS_(2))has garnered significant attention as a potential substitute for Pt catalysts in the hydrogen evolution reaction(HER).Furthermore,there is a need to explore cost-effective and efficient elec-trocatalysts that can perform well across different pH levels.In this study,a straightforward hydrothermal method is presented to synthesize Ni,Co-doped MoS_(2)nanosheets on carbon fiber paper(Ni,Co-MoS_(2)/CFP)for HER in various pH environments.The findings suggest that strategic doping not only alters the structure and composition of Ni,Co-MoS_(2)/CFP but also enhances its inherent electrocatalytic activity while facilitating the transformation of the MoS_(2)phase.The overpotentials observed for Ni,Co-MoS_(2)/CFP are 95.6,154,and 144 mV(at 10 mA cm−2)under alkaline,acidic,and neutral environments respectively.The exceptional perfor-mance of Ni,Co-MoS_(2)/CFP in HER can be attributed to the introduction of nickel and cobalt dopants which increase porosity and expose more active sites.This one-step doping technique presents a novel approach to modulating catalytic activity across all pH ranges.
基金National Natural Science Foundation of China(Grant No.22309102)China Postdoctoral Science Foundation(Grant No.2022M711788)+3 种基金National Key Research and Development Program of China(Grant No.2022YFB2404500)Fundamental Research Project of Shenzhen(Grant No.JCYJ20230807111702005)the Australian Research Council through the ARC Discovery Project(Grant No.DP230101579)ACR Linkage Project(Grant No.LP200200926).
文摘The intensifying challenges posed by climate change and the depletion of fossil fuels have spurred concerted global efforts to develop alternative energy storage solutions.Aqueous zinc-ion batteries(AZIBs)have emerged as promising candidates for large-scale electrochemical energy storage systems because of their intrinsic safety,cost-effectiveness,and environmental sustainability.However,Zn dendrite growth consis-tently poses a remarkable challenge to the performance improvement and commercial viability of AZIBs.The use of three-dimensional porous Zn anodes instead of planar Zn plates has been demonstrated as an effec-tive strategy to regulate the deposition/stripping behavior of Zn2+ions,thereby inhibiting the dendrite growth.Here,the merits of porous Zn anodes were summarized,and a comprehensive overview of the recent advancements in the engineering of porous Zn metal anodes was provided,with a particular emphasis on the structural orderliness and critical role of porous structure modulation in enhancing battery performance.Furthermore,strategic insights into the design of porous Zn anodes were presented to facilitate the practical implementation of AZIBs for grid-scale energy storage applications.
基金supported by National Natural Science Foundation of China(Grant Nos.52302293 and 22272110)Innovation Project of Education Department of Guangdong Province(Grant No.2023KTSCX124)+2 种基金Shenzhen Science and Technology Program(Grant No.KJZD2023092311460401)Guangdong Higher Education Letter(Grant No.[2024]No.30)Shenzhen Key Laboratory of Applied Technologies of Super-Diamond and Functional Crystals(Grant No.ZDSYS20230626091303007).
文摘With the boom in electric vehicles(EVs),there is an increasing demand for high-performance lithium-ion batteries.Lithium manganese iron phosphate(LMFP)has emerged as an enhanced variation of LiFePO4(LFP),offering an energy density 10%–20%greater than that of LFP.Structural distortion caused by the Jahn–Teller effect decreases the capacity and voltage platform,thus restricting the commercialization of this material.Herein,ideas to overcome these challenges,including the crystal structure of LMFP and strategies to mitigate the Jahn–Teller distortion,are first explored.Then,the migration pathways of Li+during charging and discharging and the phase transition mechanisms that affect the material’s performance are discussed.Next,the optimal Mn:Fe ratio for achieving the desired performance is described.The influences of various synthesis and modification methods on the morphology and structure of LMFP are reviewed.Additionally,different modification techniques,such as doping and coating,to enhance the performance of LMFP are highlighted.Finally,an overview of the current state of research on the recycling and reuse of LMFP is provided.By addressing these key topics,this paper offers a theoretical foundation for the further development of LMFP,thus contributing to its eventual commercialization.
基金supported by the National Natural Science Foundation of China(Grant No.22479130)Natural Science Foundation of Henan(Grant No.252300421170)China Postdoctoral Science Foundation(Grant No.2023M743150).
文摘With the exponential growth of portable electronic devices and wearable technologies,batteries are currently required to deliver not only high energy density and extended cycling performance but also enhanced safety and exceptional durability.Inspired by the self-repair mechanism observed in natural systems,a self-healing strategy shows great application potential in enabling batteries to resist external physical and chemical damage.In this review,we provide a detailed exploration of the application of self-healing materials in battery components,including electrodes,electrolytes,and encapsulation layers.We also analyze the advantages and limitations of various self-healing mechanisms,highlighting their roles in optimizing battery performance.By presenting a comprehensive synthesis of existing research,the potential pathways for advancing the development of self-healing batteries are identified,as well as the key challenges and opportunities within this field.This review aims to promote the practical integration of self-healing batteries in smart and flexible electronic devices,paving the way for safer,more reliable,and long-lasting energy storage systems.
基金the National Natural Science Foundation of China(Grant No.62274018)the Xinjiang Construction Corps Key Areas of Science and Technology Research Project(Grant No.2023AB029)the Key Project of Chongqing Overseas Students Returning to China Entrepreneurship and Innovation Support Plan(Grant No.cx2023006).
文摘Wide-bandgap(WB)mixed-halide perovskite solar cells(PSCs)play a crucial role in perovskite-based tandem solar cells(TSCs),enabling them to exceed the Shockley-Queisser limits of single-junction solar cells.Nonetheless,the lack of stability in WB perovskite films due to photoinduced phase segregation undermines the stability of WB PSCs and their TSCs,thus impeding the commercialization of perovskite-based TSCs.Many efforts have been made to suppress photoinduced phase segregation in WB perovskite films and significant progresses have been obtained.In this review,we elaborate the mechanisms behind photoinduced phase segregation and its impact on the photovoltaic performance and stability of devices.The importance role of advanced characterization techniques in confirming the photoinduced phase segregation are comprehensively summarized.Beyond that,the effective strategies to alleviate photoinduced phase segregation in WB mixed halide PSCs are systematically assessed.Finally,the prospects for developing highly efficient and stable WB PSCs in tandem application are also presented.
基金supported by the startup funding of G.Z.from The University of Alabama in Huntsville(UAH).
文摘Here we report an interesting phenomenon that lithium plating from pre-cycling of Li-ion cells at low temperature could reduce degradation and extend cycle life at high temperature.This study confirmed the phenomenon in both single-layer cells and multi-layer cells.It revealed that compression of the multi-layer cells must be maintained during cycling for the phenomenon to be observed.Without compression,lowtemperature pre-cycling would accelerate high-temperature degradation of the multi-layer cells.This finding helped to clarify the contradictions in previous studies on the effects of low-temperature pre-cycling.A comparison between low-temperature pre-cycling with 1C charging and 0.2C charging confirmed that lithium plating from low-temperature pre-cycling is necessary for the observed benefits.Furthermore,post-mortem analysis of single-layer cells showed a thick deposition layer on the anode of pre-cycled cells,which could be attributed to reactions from lithium plating and the electrolyte.
基金supported by the China University of Petroleum(East China)Independent Innovation Research Program for Young Fund(Grant No.27RA2408006)China University of Petroleum(East China)College Students’Innovation and Entrepreneurship Training Program(Grant No.202506071CX).
文摘Zinc-ion batteries(ZIBs)have garnered significant interest owing to their intrinsic safety,environmental compatibility,and low cost.However,nonuniform Zn deposition and parasitic side reactions during cycling lead to rapid capacity decay and potential short-circuiting.To address these challenges,we developed a carboxymethyl cellulose-zinc(CMC-Zn)hydrogel electrolyte with self-release capability using a metal-ion crosslinking approach.The dynamically reversible CMC-Zn network continuously supplies active Zn^(2+)during cycling,compensating for electrode consumption in real time.Abundant carboxylate and hydroxyl groups regulate uniform zinc nucleation and growth,while the hydrogen-bonding network synergistically suppresses side reactions,as reflected by a low hydrogen-evolution potential(−0.281 V)and reduced corrosion current density(0.03 mA cm^(−2)).With these advantages,Zn||Zn symmetric cells achieve an ultralong lifespan of 6,400 h at 0.5 mA cm^(−2),and Zn||Cu half-cells deliver a stable coulombic efficiency of 99.1%over 4,200 cycles.In fullcell testing,self-released Zn^(2+)contributes 29%of the overall capacity,enabling Zn||PANI cells to retain 75%capacity after 2,000 cycles and exhibit a rate-performance recovery of 97.4%.A corresponding flexible ZIB maintains stable operation under various deformation conditions,highlighting the strong potential of CMC-Zn hydrogel electrolytes for next-generation flexible energy-storage devices.
基金National Key Research and Development Program of China(Grant No.2022YFB2404500)Shenzhen Outstanding Talents Training Fund,the Fundamental Research Project of Shenzhen(Grant No.JCYJ20230807111702005)+3 种基金Guangdong Provincial Natural Science Foundation of China(Grant No.2022A1515110936)Shenzhen Science and Technology Program(Grant No.ZDSYS20230626091100001)National Natural Science Foundation of China(Grant No.22309102)China Postdoctoral Science Foundation(Grant No.2022M711788).
文摘The attainment of carbon neutrality requires the development of aqueous energy conversion and storage devices.However,these devices exhibit limited performance due to the permeability-selectivity trade-off of permselective membranes as core components.Herein,we report the application of a synergistic approach utilizing two-dimensional nanoribbons-entangled nanosheets to rationally balance the permeability and selec-tivity in permselective membranes.The nanoribbons and nanosheets can be self-assembled into a nanoflu-idic membrane with a distinctive“island-bridge”configuration,where the nanosheets serve as isolated islands offering adequate ionic selectivity owing to their high surface charge density,meanwhile bridge-like nanorib-bons with low surface charge density but high aspect ratio remarkably enhance the membrane’s permeability and water stability,as verified by molecular simulations and experimental investigations.Using this approach,we developed a high-performance graphene oxide(GO)nanosheet/GO nanoribbon(GONR)nanofluidic membrane and achieved an ultrahigh power density of 18.1 W m^(-2) in a natural seawater|river water osmotic power generator,along with a high Coulombic efficiency and an extended lifespan in zinc metal batteries.The validity of our island-bridge structural design is also demonstrated for other nanosheet/nanoribbon composite membranes,providing a promising path for developing reliable aqueous energy conversion and storage devices.
基金National Natural Science Foundation of China(Grant No.22275114)Science and Technology Planning Project of Shenzhen Municipality(Grant No.WDZC20220817160017003)+2 种基金Cross-Disciplinary Research Fund of Tsinghua Shenzhen International Graduate School(SIGS),Tsinghua University(Grant No.JC2022003)Overseas Research Cooperation Fund Research Plan of Tsinghua SIGS(Grant No.HW2023006)Scientific Research Startup Fund of SIGS,Tsinghua University(Grant Nos.QD2021027C and QD2023001C).
文摘Rechargeable aqueous zinc-ion batteries(ZIBs)have gained attention as promising candidates for nextgeneration large-scale energy storage systems due to their advantages of improved safety,environmental sustainability,and low cost.However,the zinc metal anode in aqueous ZIBs faces critical challenges,including dendrite growth,hydrogen evolution reactions,and corrosion,which severely compromise Coulombic efficiency and cycling stability,hindering their broader adoption.This review first explores the fundamental mechanisms underlying these challenges and then examines current strategies to address them,focusing on structural design,surface modifications,electrolyte optimization,and alloying treatments.Finally,potential future directions are discussed,outlining a pathway toward achieving high-performance aqueous ZIBs.
基金support from the research project from FM and startup funds provided by the University of Delaware.
文摘As lithium-ion batteries(LIBs)become increasingly widespread,ensuring their safety has become a primary concern.Particularly,battery aging has been reported to significantly impact major battery safety behaviors,including the internal short circuit(ISC)and thermal runaway(TR).Over the past decade,despite consider-able research into the thermal hazards of aged batteries,the complexity of battery aging and TR mecha-nisms,along with the challenges posed by extreme experimental conditions,necessitates a systematic under-standing.Aiming to provide a comprehensive review of safety issues related to aged batteries,this paper begins by exploring the fundamental aging mechanisms and factors that accelerate aging.It then investi-gates how aging affects battery safety issues,including swelling and off-gassing behaviors.Furthermore,we discuss the impact of aging on TR problems induced by abusive conditions,covering safety issues from inter-nal sources to external abusive scenarios.This review offers valuable insights into understanding and predict-ing the thermal hazards of aged LIBs,which provides guidelines for designing and manufacturing safer LIBs and accurate and rapid battery safety prognostics in the future.
基金the National Natural Science Foundation of China(Grant No.22105114)the Fundamental Research Funds for the Central Universities(Grant No.2024MS014).
文摘Two-dimensional(2D)nitrogen-doped graphene(NG)films have attracted considerable attention as promis-ing metal-free electrochemical catalysts for the oxygen reduction reaction(ORR).Thermal evaporation is a versatile thin film deposition technique.However,the conventional thermal evaporation techniques present challenges in producing nitrogen-rich NG thin films because of the difficulties of a controllable manner for doping graphene with N atoms.To address this,we designed a vacuum thermal evaporation system for the large-scale preparation of 2D NG thin films.Using poly(2,5-benzimidazole)(ABPBI)as a nitrogen and carbon precursor,we deposited nitrogen-rich NG thin films with a size of 50×50 mm^(2) and controllable thickness within the range of 0.5–1.5 nm.The 2D NG samples exhibited a uniform thin film structure with moderate defects.The nitrogen-rich ABPBI precursor and defects,as well as the beneficial morphology and structure,endowed the optimal catalyst(2D NG-900)with a comparable ORR activity and superior stability compared with the commercial Pt/C(20 wt%)catalyst.This paper proposes a feasible strategy for fabricating 2D NG films as effective metal-free catalysts for the ORR.
基金supported by the Shenzhen Science and Technology Planning Project(Grant No.JSGG20220831095604008)the National Natural Science Foundation of China(Grant No.51902296)+2 种基金the National Center for International Research of Electric Vehicle Power Batteries and Materials(Grant No.2015B01015)the Guangdong Key Laboratory of Design and Calculation of New Energy Materials(Grant No.2017B030301013)the Shenzhen Key Laboratory of New Energy Resources Genome Preparation and Testing(Grant No.ZDSYS201707281026184).
文摘Lithium-ion batteries are essential for modern energy storage,yet achieving simultaneous high-temperature and high-voltage operation remains challenging due to interfacial compatibility.In this study,we introduce a polyetherimide(PEI)-polyimide(PI)functional coating on the separator that enhances wettability,thermal stability,and mechanical strength,while markedly improving cathode stability under harsh conditions.By integrating theoretical calculations with experimental validation,we demonstrate that the PEI/PI coating modulates the solvation structure of lithium-ions,thereby facilitating the interfacial desolvation process.More importantly,the PEI/PI layer regulates electrolyte decomposition at the interface,promoting the formation of a uniform and thermally stable cathode-electrolyte interphase.Consequently,LiCoO_(2)cathodes exhibit improved cycling performance at 60°C.Overall,this work underscores the pivotal role of separator coatings in governing interfacial chemistry and provides a viable strategy for designing high-performance lithium-ion batteries capable of enduring both high temperatures and high.
基金supported by the National Natural Science Foundation of China(Grant Nos.52222213,U23A20572)the Fundamental Research Funds for the Central Universities of China(Grant No.22lgqb01).
文摘Owing to their high volumetric capacity,low cost and high safety,rechargeable aluminum batteries have become promising candidates for energy applications.However,the high charge density of Al^(3+)leads to strong coulombic interactions between anions and the cathode,resulting in sluggish diffusion kinetics and irreversible collapse of the cathode structure.Furthermore,AlCl_(3)-based ionic liquids,which are commonly used as electrolytes in such batteries,corrode battery components and are prone to side reactions.The above problems lead to low capacity and poor cycling stability.Herein,we propose a reduced graphene oxide(rGO)cathode with a three-dimensional porous structure prepared using a simple and scalable method.The lamellar edges and oxygen-containing group defects of rGO synergistically provide abundant ion storage sites and enhance ion transfer kinetics.We matched the prepared rGO cathode with noncorrosive electrolyte 0.5 mol·L^(-1) Al(OTF)_(3)/[BMIM]OTF and Al metal to construct a high-performance battery,Al||rGO-150,with good cycling stability for 2700 cycles.Quasi-in-situ physicochemical characterization results show that the ion storage mechanism is codominated by diffusion and capacitance.The capacity consists of the insertion of Al-based species cations as well as synergistic adsorption of Al(OTF)_(x)^((3-x)+)(x<3)and[BMIM]+.The present study promotes the fundamental and applied research on rechargeable aluminum batteries.
基金National Natural Science Youth Foundation of China(Grant No.52302247)National Natural Science Foundation of China(Grant Nos.52072208 and 52261160384)+1 种基金Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2024A1515012996)Shenzhen Science and Technology Plan Basic Research(General project,No.JCYJ20230807122005011).
文摘Owing to their intrinsic safety and low cost,aqueous zinc-ion batteries(AZIBs)have emerged as promising large-scale energy storage devices.Hydrogel electrolytes have been extensively studied because of their superior electrochemical performance their ability to endow AZIBs with excellent flexibility.However,traditional hydrogel electrolytes typically suffer from a narrow electrochemical stability potential window(ESPW)and poor cycling stability,primarily due to their high water content.In recent years,lean-water hydrogel electrolytes(L-WHEs)have been developed to address these issues.By confining free water molecules and regulating ion transport within the hydrogel network,L-WHEs can efficiently suppress side reactions,widen the ESPW,and enhance interfacial stability.This review systematically discusses the fundamental principles of L-WHEs,current strategies for developing practical L-WHEs,and recent research progress.Finally,future prospect and challenges in the development of high-performance L-WHEs are outlined.
基金National Key Research and Development Program of China(Grant No.2022YFB2404500)the National Natural Science Foundation of China(Grant Nos.22479110,22109116 and 22121004)+3 种基金the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(Grant No.E411050316)the Natural Science Foundation of Tianjin(Grant No.23JCQNJC01750)the“Pandeng Plan”Project in Tianjin University(Grant No.2024XPD-0002)the Fundamental Research Funds for the Central Universities,and the Haihe Laboratory of Sustainable Chemical Transformations.
文摘Manganese dioxide(MnO_(2)),based on a two-electron-transfer deposition/dissolution chemistry,features an ultrahigh theoretical capacity(616 mAh·g^(−1)),a favorable redox potential(1.23 V vs.the standard hydrogen electrode),inherent nontoxicity,and low cost,making it a promising cathode candidate for high-energy aqueous batteries.However,its practical application is hindered by limited electrochemical reversibility and cycling stability,primarily attributed to the formation and accumulation of electrochemically inactive Mn species commonly known as“dead Mn”.This perspective provides an in-depth analysis of the“dead Mn”dilemma inherent in Mn^(2+)/MnO_(2) chemistry.First,the fundamental causes of“dead Mn”—insufficient electron supply and imbalanced(insufficient or excessive)proton supply,are systematically analyzed,as they detract from active material utilization,cycle life,and energy density.Then,mitigation strategies are examined from three aspects:preventing“dead Mn”formation caused by insufficient electron supply,mitigating“dead Mn”formation related to imbalanced proton supply,and activating and regenerating existing“dead Mn”.Finally,future research directions are visualized to enhance the practical viability of Mn^(2+)/MnO_(2) deposition/dissolution chemistry,aiming to catalyze advancements in high-energy aqueous battery systems.
基金supported by the startup funding of HLX and the Assistant Secretary for Energy Efficiency and Renewable Energy,Vehicle Technology Office of the U.S.Department of Energy(DOE)through the Advanced Battery Materials Research Program under contract No.DE-SC0012704.
文摘Solid polymer electrolytes(SPEs)have attracted considerable attention for solid-state lithium-metal batteries(LMBs)with high energy density and enhanced safety for future applications.In this study,an SPE was devel-oped based on a poly(ethyl acrylate)(PEA)polymer matrix with the vinylene carbonate(VC)additive(defined as PEA-VC)for high-voltage solid-state LMBs.Results show that introducing the VC additive into the PEA-based SPE leads to high lithium-ion conductivity(1.57 mS/cm at 22°C),a high lithium-ion transference number(0.73),and a wide electrochemical stability window(up to 4.9 V vs.Li/Li^(+)).The remarkable compatibil-ity of the PEA-VC SPE with lithium metal anodes and high-voltage cathodes was demonstrated in Li//Li symmetric cells(800 h lifetime at a current density of 0.1 mA/cm^(2) at 22°C)and Li//LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)full cells(with a capacity retention of 77.8%after 100 cycles at 0.2C).The improved stability is attributed to the introduction of the VC additive,which helps form a robust cathode–electrolyte interphase,effectively suppressing parasitic interface side reactions.Overall,this study highlights the role of VC addi-tives in high-voltage and solid-state LMBs,offering a general yet effective approach for addressing the interfa-cial instability issue through an additive-engineering strategy.
