Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical cap...Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical capacity of 372 mA·h·g^(−1),thus hindering further development toward high-capacity and large-scale applications.Alkaline earth metal iron-based oxides are considered a promising candidate to replace graphite because of their low preparation cost,good thermal stability,superior stability,and high electrochemical performance.Nonetheless,many issues and challenges remain to be addressed.Herein,we systematically summarize the research progress of alkaline earth metal iron-based oxides as LIB anodes.Meanwhile,the material and structural properties,synthesis methods,electrochemical reaction mechanisms,and improvement strategies are introduced.Finally,existing challenges and future research directions are discussed to accelerate their practical application in commercial LIBs.展开更多
Although lithium(Li)metal delivers the highest theoretical capacity as a battery anode,its high reactivity can generate Li dendrites and"dead"Li during cycling,resulting in poor reversibility and low Li util...Although lithium(Li)metal delivers the highest theoretical capacity as a battery anode,its high reactivity can generate Li dendrites and"dead"Li during cycling,resulting in poor reversibility and low Li utilization.Inducing uniform Li plating/stripping is the core of solving these problems.Herein,we design a highly lithiophilic carbon film with an outer sheath of the nanoneedle arrays to induce homogeneous Li plating/stripping.The excellent conductivity and 3D framework of the carbon film not only offer fast charge transport across the entire electrode but also mitigate the volume change of Li metal during cycling.The abundant lithiophilic sites ensure stable Li plating/stripping,thereby inhibiting the Li dendritic growth and"dead"Li formation.The resulting composite anode allows for stable Li stripping/plating under 0.5 mA cm^(-2) with a capacity of 0.5 mA h cm^(-2) for 4000 h and 3 mA cm^(-2) with a capacity of3 mA h cm^(-2) for 1000 h.The Ex-SEM analysis reveals that lithiophilic property is different at the bottom,top,or channel in the structu re,which can regulate a bottom-up uniform Li deposition behavior.Full cells paired with LFP show a stable capacity of 155 mA h g^(-1) under a current density of 0.5C.The pouch cell can keep powering light-emitting diode even under 180°bending,suggesting its good flexibility and great practical applications.展开更多
Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the...Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.展开更多
The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano i...The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of∼35 nm is designed accurately by magnetron sputtering technology to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously“attacking”the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby significantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of electrolyte/Li anode interface promotes the homogeneous deposition of Li^(+)and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO_(4)|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9%for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs.展开更多
Two-dimensional(2D) metal oxide nanosheets have attracted much attention as potential electrode materials for rechargeable batteries in recent years. This is primarily due to their natural abundance, environmental c...Two-dimensional(2D) metal oxide nanosheets have attracted much attention as potential electrode materials for rechargeable batteries in recent years. This is primarily due to their natural abundance, environmental compatibility, and low cost as well as good electrochemical properties. Despite the fact that most metal oxides possess low conductivity, the introduction of some conductive heterogeneous components, such as nano-carbon, carbon nanotubes(CNTs), and graphene, to form metal oxide-based hybrids,can effectively overcome this drawback. In this mini review, we will summarize the recent advances of three typical 2D metal oxide nanomaterials, namely, binary metal oxides, ternary metal oxides, and hybrid metal oxides, which are used for the electrochemical applications of next-generation rechargeable batteries, mainly for lithium-ion batteries(LIBs) and sodium-ion batteries(SIBs). Hence, this review intends to functionalize as a good reference for the further research on 2D nanomaterials and the further development of energy-storage devices.展开更多
With graphite currently leading as the most viable anode for potassium-ion batteries(KIBs),other materials have been left relatively underexamined.Transition metal oxides are among these,with many positive attributes ...With graphite currently leading as the most viable anode for potassium-ion batteries(KIBs),other materials have been left relatively underexamined.Transition metal oxides are among these,with many positive attributes such as synthetic maturity,longterm cycling stability and fast redox kinetics.Therefore,to address this research deficiency we report herein a layered potassium titanium niobate KTiNbO5(KTNO)and its rGO nanocomposite(KTNO/rGO)synthesised via solvothermal methods as a high-performance anode for KIBs.Through effective distribution across the electrically conductive rGO,the electrochemical performance of the KTNO nanoparticles was enhanced.The potassium storage performance of the KTNO/rGO was demonstrated by its first charge capacity of 128.1 mAh g^(−1) and reversible capacity of 97.5 mAh g^(−1) after 500 cycles at 20 mA g^(−1),retaining 76.1%of the initial capacity,with an exceptional rate performance of 54.2 mAh g^(−1)at 1 A g^(−1).Furthermore,to investigate the attributes of KTNO in-situ XRD was performed,indicating a low-strain material.Ex-situ X-ray photoelectron spectra further investigated the mechanism of charge storage,with the titanium showing greater redox reversibility than the niobium.This work suggests this lowstrain nature is a highly advantageous property and well worth regarding KTNO as a promising anode for future high-performance KIBs.展开更多
This study explores how the chemical interaction between magnesium hydride(MgH_(2))and the additive CrO_(3) influences the hydrogen/lithium storage characteristics of MgH_(2).We have observed that a 5 wt.%CrO_(3) addi...This study explores how the chemical interaction between magnesium hydride(MgH_(2))and the additive CrO_(3) influences the hydrogen/lithium storage characteristics of MgH_(2).We have observed that a 5 wt.%CrO_(3) additive reduces the dehydrogenation activation energy of MgH_(2) by 68 kJ/mol and lowers the required dehydrogenation temperature by 80℃.CrO_(3) added MgH_(2) was also tested as an anode in an Li ion battery,and it is possible to deliver over 90%of the total theoretical capacity(2038 mAh/g).Evidence for improved reversibility in the battery reaction is found only after the incorporation of additives with MgH_(2).In depth characterization study by X-ray diffraction(XRD)technique provides convincing evidence that the CrO_(3) additive interacts with MgH_(2) and produces Cr/MgO byproducts.Gibbs free energy analyses confirm the thermodynamic feasibility of conversion from MgH_(2)/CrO_(3) to MgO/Cr,which is well supported by the identification of Cr(0)in the powder by X ray photoelectron spectroscopy(XPS)technique.Through high resolution transmission electron microscopy(HRTEM)and energy dispersive spectroscopy(EDS)we found evidence for the presence of 5 nm size Cr nanocrystals on the surface of MgO rock salt nanoparticles.There is also convincing ground to consider that MgO rock salt accommodates Cr in the lattice.These observations support the argument that creation of active metal–metal dissolved rock salt oxide interface may be vital for improving the reactivity of MgH_(2),both for the improved storage of hydrogen and lithium.展开更多
In recent times,future energy storage systems demand a multitude of functionalities beyond their traditional energy storage capabilities.In line with this technological shift,there is active research and development o...In recent times,future energy storage systems demand a multitude of functionalities beyond their traditional energy storage capabilities.In line with this technological shift,there is active research and development of electrochromic-energy storage systems designed to visualize electrochemical charging and discharging processes.The conventional electrochromic-energy storage devices primarily integrated supercapacitors,known for their high power density,to enable rapid color contrast.However,the low energy density of supercapacitors restricts overall energy storage capacity,acting as a significant barrier to expanding the application range of such systems.In this review,we introduce electrochromic zinc(Zn)-ion battery systems,which effectively overcome the limitation of low energy density,and provide illustrative examples of their applicability across diverse fields.Although many recent research works are present for electrochromic Zn-ion batteries,little review has so far taken place.Our objective is to discuss on the current progress and future directions for electrochromic Zn-ion batteries,which are applicable for wearable electronics applications and energy storage systems.This review provides an initial milestone for future researchers in electrochromic energy storage and zinc-ion batteries,which will lead to a stream of future works related to them.展开更多
The widespread interest in layered P2-type Mn-based cathode materials for sodium-ion batteries(SIBs)stems from their cost-effectiveness and abundant resources.However,the inferior cycle stability and mediocre rate per...The widespread interest in layered P2-type Mn-based cathode materials for sodium-ion batteries(SIBs)stems from their cost-effectiveness and abundant resources.However,the inferior cycle stability and mediocre rate performance impede their further development in practical applications.Herein,we devised a wet chemical precipitation method to deposit an amorphous aluminum phosphate(AlPO_(4),denoted as AP)protective layer onto the surface of P2-type Na_(0.55)Ni_(0.1)Co_(0.7)Mn_(0.8)O_(2)(NCM@AP).The resulting NCM@5AP electrode,with a 5 wt%coating,exhibits extended cycle life(capacity retention of78.4%after 200 cycles at 100 mA g^(-1))and superior rate performance(98 mA h g^(-1)at 500 mA g^(-1))compared to pristine NCM.Moreover,our investigation provides comprehensive insights into the phase stability and active Na^(+)ion kinetics in the NCM@5AP composite electrode,shedding light on the underlying mechanisms responsible for the enhanced performance observed in the coated electrode.展开更多
Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.H...Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.展开更多
Recently,poly(ethylene oxide)(PEO)-based solid polymer electrolytes have been attracting great attention,and efforts are currently underway to develop PEO-based composite electrolytes for next generation high performa...Recently,poly(ethylene oxide)(PEO)-based solid polymer electrolytes have been attracting great attention,and efforts are currently underway to develop PEO-based composite electrolytes for next generation high performance all-solid-state lithium metal batteries.In this article,a novel sandwich structured solid-state PEO composite electrolyte is developed for high performance all-solid-state lithium metal batteries.The PEO-based composite electrolyte is fabricated by hot-pressing PEO,LiTFSI and Ti_(3)C_(2)T_(x) MXene nanosheets into glass fiber cloth(GFC).The as-prepared GFC@PEO-MXene electrolyte shows high mechanical properties,good electrochemical stability,and high lithium-ion migration number,which indicates an obvious synergistic effect from the microscale GFC and the nanoscale MXene.Such as,the GFC@PEO-1 wt%MXene electrolyte shows a high tensile strength of 43.43 MPa and an impressive Young's modulus of 496 MPa,which are increased by 1205%and 6048%over those of PEO.Meanwhile,the ionic conductivity of GFC@PEO-1 wt%MXene at 60℃ reaches 5.01×10^(-2) S m^(-1),which is increased by around 200%compared with that of GFC@PEO electrolyte.In addition,the Li/Li symmetric battery based on GFC@PEO-1 wt%MXene electrolyte shows an excellent cycling stability over 800 h(0.3 mA cm^(-2),0.3 mAh cm^(-2)),which is obviously longer than that based on PEO and GFC@PEO electrolytes due to the better compatibility of GFC@PEO-1 wt%MXene electrolyte with Li anode.Furthermore,the solid-state Li/LiFePO_(4) battery with GFC@PEO-1 wt%MXene as electrolyte demonstrates a high capacity of 110.2–166.1 mAh g^(-1) in a wide temperature range of 25–60C,and an excellent capacity retention rate.The developed sandwich structured GFC@PEO-1 wt%MXene electrolyte with the excellent overall performance is promising for next generation high performance all-solid-state lithium metal batteries.展开更多
The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both hav...The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.展开更多
Potassium ion batteries(PIBs)are emerging as potential next-generation energy storage systems on account of their low cost and high theoretical energy density.Nevertheless,they also face challenges of low specific cap...Potassium ion batteries(PIBs)are emerging as potential next-generation energy storage systems on account of their low cost and high theoretical energy density.Nevertheless,they also face challenges of low specific capacity and suboptimal cycling stability.Herein,we synthesize a cocoon-like P3-type K_(0.5)Mn_(0.7)Ni_(0.3)O_(2)(KMNO)cathode material by a self-template method.The KMNO cocoons possess a hierarchical layered architecture composed of nanoparticle stacking,which can accelerate the transport kinetics of potassium ions,mitigate the stress caused by K^(+)intercalation and deintercalation,and improve structural stability.In addition,Ni can not only alleviate the Jahn-Teller distortion and suppress the phase transition to stabilize the structure,but also act as an electrochemically active element,providing the capacity of two electrons from Ni2+to Ni4+.Combining the advantages of structure and nickel substitution,the P3-type KMNO cocoons are used for electrochemical performance testing of PIB cathodes,delivering an excellent rate capability of 57.1 m A h g^(-1)at 500 m A g^(-1)and a remarkable cycling stability of 77.0%over 300 cycles at 100 m A g^(-1).Impressively,the KMNO cocoons//pitch-derived soft carbon assembled full battery exhibits superior electrochemical performance with a reversible capacity of 79.7 m A h g^(-1)at 50 m A g^(-1).Moreover,ex-situ XRD also further reveals a solid solution phase reaction with a volume change of only 1.46%.This work furnishes a suitable approach to fabricating highperformance layered oxide cathodes for PIBs with outstanding cycling stability and rate capability.展开更多
As lithium(Li)-ion batteries expand their applications,operating over a wide temperature range becomes increasingly important.However,the lowtemperature performance of conventional graphite anodes is severely hampered...As lithium(Li)-ion batteries expand their applications,operating over a wide temperature range becomes increasingly important.However,the lowtemperature performance of conventional graphite anodes is severely hampered by the poor diffusion kinetics of Li ions(Li^(+)).Here,zinc oxide(ZnO) nanoparticles are incorporated into the expanded graphite to improve Li^(+)diffusion kinetics,resulting in a significant improvement in lowtemperature performance.The ZnO-embedded expanded graphite anodes are investigated with different amounts of ZnO to establish the structurecharge storage mechanism-performance relationship with a focus on lowtemperature applications.Electrochemical analysis reveals that the ZnOembedded expanded graphite anode with nano-sized ZnO maintains a large portion of the diffusion-controlled charge storage mechanism at an ultra-low temperature of-50℃ Due to this significantly enhanced Li^(+)diffusion rate,a full cell with the ZnO-embedded expanded graphite anode and a LiNi_(0.88)Co_(0.09)Al_(0.03)O_(2)cathode delivers high capacities of 176 mAh g^(-1)at20℃ and 86 mAh g^(-1)at-50℃ at a high rate of 1 C.The outstanding low-temperature performance of the composite anode by improving the Li^(+)diffusion kinetics provides important scientific insights into the fundamental design principles of anodes for low-temperature Li-ion battery operation.展开更多
In this manuscript, we have demonstrated the delicate design and synthesis of bimetallic oxides nanoparticles derived from metal–oleate complex embedded in 3D graphene networks(MnO/CoMn_2O_4 GN), as an anode mater...In this manuscript, we have demonstrated the delicate design and synthesis of bimetallic oxides nanoparticles derived from metal–oleate complex embedded in 3D graphene networks(MnO/CoMn_2O_4 GN), as an anode material for lithium ion batteries. The novel synthesis of the MnO/CoMn_2O_4 GN consists of thermal decomposition of metal–oleate complex containing cobalt and manganese metals and oleate ligand, forming bimetallic oxides nanoparticles, followed by a selfassembly route with reduced graphene oxides. The MnO/CoMn_2O_4 GN composite, with a unique architecture of bimetallic oxides nanoparticles encapsulated in 3D graphene networks, rationally integrates several benefits including shortening the di usion path of Li^+ ions, improving electrical conductivity and mitigating volume variation during cycling. Studies show that the electrochemical reaction processes of MnO/Co Mn_2O_4 GN electrodes are dominated by the pseudocapacitive behavior, leading to fast Li^+ charge/discharge reactions. As a result, the MnO/CoMn_2O_4 GN manifests high initial specific capacity, stable cycling performance, and excellent rate capability.展开更多
The future of high-energy density electrochemical energy storage systems relies on the advancement of rechargeable batteries that utilize reactive metals as anodes.In the alkaline metal,secondary battery systems becau...The future of high-energy density electrochemical energy storage systems relies on the advancement of rechargeable batteries that utilize reactive metals as anodes.In the alkaline metal,secondary battery systems because of abundant resource,high capacity and low redox potential,potassium(K)metal secondary battery(KMB)is expected to replace the existing lithiumion battery as a versatile platform for high-energy density,cost-effective energy storage devices.However,the difficulty in processing metal K results in nonstandard electrodes and hinders the development of KMBs.Furthermore,the mobility of the K metal anode due to its unique lowmelting point character at elevated temperatures in practical conditions leads to severe instability and risks in chemical/electrochemical processes.Herein,we fabricate a processable and moldable composite K metal anode by encapsulating K into reduced graphene oxide(rGO).The composite electrode can be engineered into various shapes discretionarily with precise sizes and stabilize the K metal anode at relatively high temperatures.Remarkably,the composite anode exhibits excellent cycling performance at high current density(8 mA cm^(-2)) with dendrite-free morphology.Paired with a Prussian blue cathode,the rGO-K composite anode shows much improved electrochemical performance and extended lifetime.展开更多
The development of clean renewable energy and energy storage devices is of great significance under the present energy crisis and environmental pollution background.Aqueous zinc-ion battery(ZIB)has become one of the m...The development of clean renewable energy and energy storage devices is of great significance under the present energy crisis and environmental pollution background.Aqueous zinc-ion battery(ZIB)has become one of the most promising energy storage devices due to its high capacity,safety and low cost.However,the application of ZIB cathode is usually limited by low capacity and poor stability.Herein,we propose a novel heterostructure MnO/MnV_(2)O_(4)composite material composed of MOF derivatives and spinel with dual active components as cathode for ZIBs.Benefited from substantial framework of MOF derivatives and the synergistic effect of heterostructures,MnO/MnV_(2)O_(4)exhibits excellent rate performance(342 m Ah/g at 0.1 A/g,261 mAh/g at 15 A/g)and cycling performance(198.9 mAh/g at 10 A/g after 2000 cycles)in3 mol/L Zn(CF_(3)SO_(3))2electrolytes.This work extends the range of developing high-performance cathodes for ZIBs under high current density and is expected to enlighten the optimization of commercial energy storage devices.展开更多
A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of th...A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes.Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.%CAB(PL-CAB-10%)exhibits high ionic conductivity(8.42×10~(-4)S/cm at 60℃),high Li+transference number(0.46),wide electrochemical window(4.91 V),good thermal stability,and outstanding mechanical properties.Furthermore,PL-CAB-10%exhibits excellent cycle stability in both Li-Li symmetric battery and Li/PL-CAB-10%/LiFePO4 asymmetric battery setups.These enhanced performances are primarily attributable to the introduction of the versatile CAB.The abundant metal sites in CAB can react with TFSI~-and PEO through Lewis acid-base interactions,promoting LiTFSI dissociation and improving ionic conductivity.Additionally,regular pores in CAB provide uniformly distributed sites for cation plating during cycling.展开更多
Two-dimensional(2D)materials have attracted a great deal of research interest because of their unique electrical,magnetic,optical,mechanical,and catalytic properties for various applications.To date,however,it is stil...Two-dimensional(2D)materials have attracted a great deal of research interest because of their unique electrical,magnetic,optical,mechanical,and catalytic properties for various applications.To date,however,it is still difficult to fabricate most functional oxides as 2D materials unless they have a layered structure.Herein,we report a one-step universal strategy for preparing versatile non-layered oxide nanosheets by directly annealing the mixture of metal nitrate and dimethyl imidazole(2-MI).The 2-MI plays the key role for 2D oxides since 2-MI owns a very low molten point and sublimation temperature,in which its molten liquid can coordinate with metal ions,forming a metal-organic framework,and easily puffing by its gas molecules.A total of 17 materials were prepared by this strategy,including non-layered metal oxide nanosheets as well as metal/metal oxide loaded nitrogen-doped carbon nanosheets.The as-prepared cobalt particle-loaded nitrogen-doped carbon nanosheets(Co@N/C)exhibit remarkable bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalytic activity and durability.Besides,the Zn-air battery utilizing a Co@N/C catalyst exhibits high power density of 174.3 mW·cm^(-2).This facile strategy opens up a new way for large-scale synthesis of 2D oxides that holds great potential to push 2D oxides for practical applications.展开更多
Polyethylene oxide(PEO)-based solid-state electrolytes are considered ideal for electrolyte materials in solid-state lithium metal batteries(SSLMBs).However,practical applications are hindered by the lower conductivit...Polyethylene oxide(PEO)-based solid-state electrolytes are considered ideal for electrolyte materials in solid-state lithium metal batteries(SSLMBs).However,practical applications are hindered by the lower conductivity and poor interfacial stability.Here,we propose a strategy to construct a three-dimensional(3D)fiber network of metal-organic frameworks(MOFs).Composite solid electrolytes(CSEs)with continuous ion transport pathways were fabricated by filling a PEO polymer matrix in fibers containing interconnected MOFs.This 3D fiber network provides a fast Li+transport path and effectively improves the ionic conductivity(1.36×10^(-4) S·cm^(-1),30℃).In addition,the network of interconnected MOFs not only effectively traps the anions,but also provides sufficient mechanical strength to prevent the growth of Li dendrites.Benefiting from the advantages of structural design,the CSEs stabilize the Li/electrolyte interface and extend the cycle life of the Li-symmetric cells to 3000 h.The assembled SSLMBs exhibit excellent cycling performance at both room and high temperatures.In addition,the constructed pouch cells can provide an areal capacity of 0.62 mA·h·cm^(-2),which can still operate under extreme conditions.This work provides a new strategy for the design of CSEs with continuous structure and stable operation of SSLMBs.展开更多
基金The authors acknowledge the support of the Shenyang University of Technology(QNPY202209-4)the National Natural Science Foundation of China(21571132)+1 种基金Jiangsu University Advanced Talent Fund(5501710002)the Education Department of Liaoning Province(JYTQN2023285).
文摘Anode materials are an essential part of lithium-ion batteries(LIBs),which determine the performance and safety of LIBs.Currently,graphite,as the anode material of commercial LIBs,is limited by its low theoretical capacity of 372 mA·h·g^(−1),thus hindering further development toward high-capacity and large-scale applications.Alkaline earth metal iron-based oxides are considered a promising candidate to replace graphite because of their low preparation cost,good thermal stability,superior stability,and high electrochemical performance.Nonetheless,many issues and challenges remain to be addressed.Herein,we systematically summarize the research progress of alkaline earth metal iron-based oxides as LIB anodes.Meanwhile,the material and structural properties,synthesis methods,electrochemical reaction mechanisms,and improvement strategies are introduced.Finally,existing challenges and future research directions are discussed to accelerate their practical application in commercial LIBs.
基金supported by the National Natural Science Foundation of China(31870570)the Science and Technology Plan of Fujian Provincial,China(2020H4026,2022G02020 and 2022H6002)+1 种基金the Science and Technology Plan of Xiamen(3502Z20203005)the Scientific Research Start-up Funding for Special Professor of Minjiang Scholars。
文摘Although lithium(Li)metal delivers the highest theoretical capacity as a battery anode,its high reactivity can generate Li dendrites and"dead"Li during cycling,resulting in poor reversibility and low Li utilization.Inducing uniform Li plating/stripping is the core of solving these problems.Herein,we design a highly lithiophilic carbon film with an outer sheath of the nanoneedle arrays to induce homogeneous Li plating/stripping.The excellent conductivity and 3D framework of the carbon film not only offer fast charge transport across the entire electrode but also mitigate the volume change of Li metal during cycling.The abundant lithiophilic sites ensure stable Li plating/stripping,thereby inhibiting the Li dendritic growth and"dead"Li formation.The resulting composite anode allows for stable Li stripping/plating under 0.5 mA cm^(-2) with a capacity of 0.5 mA h cm^(-2) for 4000 h and 3 mA cm^(-2) with a capacity of3 mA h cm^(-2) for 1000 h.The Ex-SEM analysis reveals that lithiophilic property is different at the bottom,top,or channel in the structu re,which can regulate a bottom-up uniform Li deposition behavior.Full cells paired with LFP show a stable capacity of 155 mA h g^(-1) under a current density of 0.5C.The pouch cell can keep powering light-emitting diode even under 180°bending,suggesting its good flexibility and great practical applications.
基金the financial supports from the KeyArea Research and Development Program of Guangdong Province (2020B090919001)the National Natural Science Foundation of China (22078144)the Guangdong Natural Science Foundation for Basic and Applied Basic Research (2021A1515010138 and 2023A1515010686)。
文摘Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.
基金supported by the National Natural Science Foundation of China(22279116 and U20A20253)the Natural Science Foundationof Zhejiang Province(LD22E020006 and LQ24E020012)+3 种基金the Science and Technology Development of Zhejiang Province(2023C01231 and 2024C01095)the Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation(LBMHD24E020001)the China Postdoctoral Science Foundation(2020M671785 and 2020T130597)the Fundamental Research Funds for the Provincial Universities of Zhejiang(2022YW54).
文摘The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of∼35 nm is designed accurately by magnetron sputtering technology to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously“attacking”the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby significantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of electrolyte/Li anode interface promotes the homogeneous deposition of Li^(+)and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO_(4)|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9%for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs.
基金supported by an Australian Research Council(ARC)Discovery Early Career Researcher Award(DECRA)project(DE150100280)an ARC Discovery Project(DP160102627)an ARC Future Fellowship Project(FT160100281)
文摘Two-dimensional(2D) metal oxide nanosheets have attracted much attention as potential electrode materials for rechargeable batteries in recent years. This is primarily due to their natural abundance, environmental compatibility, and low cost as well as good electrochemical properties. Despite the fact that most metal oxides possess low conductivity, the introduction of some conductive heterogeneous components, such as nano-carbon, carbon nanotubes(CNTs), and graphene, to form metal oxide-based hybrids,can effectively overcome this drawback. In this mini review, we will summarize the recent advances of three typical 2D metal oxide nanomaterials, namely, binary metal oxides, ternary metal oxides, and hybrid metal oxides, which are used for the electrochemical applications of next-generation rechargeable batteries, mainly for lithium-ion batteries(LIBs) and sodium-ion batteries(SIBs). Hence, this review intends to functionalize as a good reference for the further research on 2D nanomaterials and the further development of energy-storage devices.
基金Y.X.acknowledges the financial support of the Engineering and Physical Sciences Research Council(EP/X000087/1,EP/V000152/1)Leverhulme Trust(RPG-2021-138)Royal Society(IEC\NSFC\223016).
文摘With graphite currently leading as the most viable anode for potassium-ion batteries(KIBs),other materials have been left relatively underexamined.Transition metal oxides are among these,with many positive attributes such as synthetic maturity,longterm cycling stability and fast redox kinetics.Therefore,to address this research deficiency we report herein a layered potassium titanium niobate KTiNbO5(KTNO)and its rGO nanocomposite(KTNO/rGO)synthesised via solvothermal methods as a high-performance anode for KIBs.Through effective distribution across the electrically conductive rGO,the electrochemical performance of the KTNO nanoparticles was enhanced.The potassium storage performance of the KTNO/rGO was demonstrated by its first charge capacity of 128.1 mAh g^(−1) and reversible capacity of 97.5 mAh g^(−1) after 500 cycles at 20 mA g^(−1),retaining 76.1%of the initial capacity,with an exceptional rate performance of 54.2 mAh g^(−1)at 1 A g^(−1).Furthermore,to investigate the attributes of KTNO in-situ XRD was performed,indicating a low-strain material.Ex-situ X-ray photoelectron spectra further investigated the mechanism of charge storage,with the titanium showing greater redox reversibility than the niobium.This work suggests this lowstrain nature is a highly advantageous property and well worth regarding KTNO as a promising anode for future high-performance KIBs.
基金supported by the projects UIDB/00481/2020 and UIDP/00481/2020-Fundação para a Ciência e a Tecnologia,DOI 10.54499/UIDB/00481/2020(https://doi.org/10.54499/UIDB/00481/2020)and DOI 10.54499/UIDP/00481/2020(https://doi.org/10.54499/UIDP/00481/2020)supported by CENTRO-01-0145-FEDER-022083-Centro Portugal Regional Operational Programme(Centro 2020),under the PORTUGAL 2020 Partnership Agreement,through the European Regional Development Fund(ERDF).This article is a result of the Innovation Pact“NGS-New Generation Storage”(C644936001-00000045)+3 种基金by“NGS”Consortium,co-financed by NextGeneration EU,through the Incentive System“Agendas para a Inovação Empresarial”(“Agendas for Business Innovation”)within the Recovery and Resilience Plan(PRR).D.P acknowledges FCT,Portugal for the financial support with reference CEECIND/04158/2017(https://doi.org/10.54499/CEECIND/04158/2017/CP1459/CT0029)funding from the SMART-ER project,funded by the European Union’s Horizon 2020 research and innovation programme under Grant Agreement#101016888.support granted by the Recovery and Resilience Plan(PRR)and by the Next Generation EU European Funds to Universidade de Aveiro,through the Agenda for Business Innovation“NGS-Next Generation Storage”(Project no 02/C05-i01.01/2022 with the application C644936001-00000045).
文摘This study explores how the chemical interaction between magnesium hydride(MgH_(2))and the additive CrO_(3) influences the hydrogen/lithium storage characteristics of MgH_(2).We have observed that a 5 wt.%CrO_(3) additive reduces the dehydrogenation activation energy of MgH_(2) by 68 kJ/mol and lowers the required dehydrogenation temperature by 80℃.CrO_(3) added MgH_(2) was also tested as an anode in an Li ion battery,and it is possible to deliver over 90%of the total theoretical capacity(2038 mAh/g).Evidence for improved reversibility in the battery reaction is found only after the incorporation of additives with MgH_(2).In depth characterization study by X-ray diffraction(XRD)technique provides convincing evidence that the CrO_(3) additive interacts with MgH_(2) and produces Cr/MgO byproducts.Gibbs free energy analyses confirm the thermodynamic feasibility of conversion from MgH_(2)/CrO_(3) to MgO/Cr,which is well supported by the identification of Cr(0)in the powder by X ray photoelectron spectroscopy(XPS)technique.Through high resolution transmission electron microscopy(HRTEM)and energy dispersive spectroscopy(EDS)we found evidence for the presence of 5 nm size Cr nanocrystals on the surface of MgO rock salt nanoparticles.There is also convincing ground to consider that MgO rock salt accommodates Cr in the lattice.These observations support the argument that creation of active metal–metal dissolved rock salt oxide interface may be vital for improving the reactivity of MgH_(2),both for the improved storage of hydrogen and lithium.
基金supported by funding from Bavarian Center for Battery Technology(Bay Batt),Bayerisch-Tschechische Hochschulagentur(BTHA)(BTHA-AP-2022-45,BTHA-AP-2023-5,BTHA-AP2023-12,and BTHA-AP-2023-38)the University of BayreuthDeakin University Joint Ph.D.Program,Bayerische Forschungallianz(Bay FOR)(Bay Int An_UBT_2023_84)+2 种基金BK21 program from National Research Foundation of Korea,Erasmus+program from the European Union,Ministry of Education,Science and Technology as part of the Higher Education for Economic Transformation(HEET)Project(World Bank)Verband der Chemischen Industrie(Fonds der Chemischen Industrie,No.661740)collaboration project funding from Kangwon National University and LINC 3.0 Research Center,and the Deutsche Forschungsgemeinschaft(DFG,project number:533115776)。
文摘In recent times,future energy storage systems demand a multitude of functionalities beyond their traditional energy storage capabilities.In line with this technological shift,there is active research and development of electrochromic-energy storage systems designed to visualize electrochemical charging and discharging processes.The conventional electrochromic-energy storage devices primarily integrated supercapacitors,known for their high power density,to enable rapid color contrast.However,the low energy density of supercapacitors restricts overall energy storage capacity,acting as a significant barrier to expanding the application range of such systems.In this review,we introduce electrochromic zinc(Zn)-ion battery systems,which effectively overcome the limitation of low energy density,and provide illustrative examples of their applicability across diverse fields.Although many recent research works are present for electrochromic Zn-ion batteries,little review has so far taken place.Our objective is to discuss on the current progress and future directions for electrochromic Zn-ion batteries,which are applicable for wearable electronics applications and energy storage systems.This review provides an initial milestone for future researchers in electrochromic energy storage and zinc-ion batteries,which will lead to a stream of future works related to them.
基金financially supported by the Australian Research Council(ARC) through the Future Fellowship(FT180100705)the financial support from China Scholarship Council+3 种基金the support from UTS-HUST Key Technology Partner Seed Fundthe support from Open Project of State Key Laboratory of Advanced Special Steel,the Shanghai Key Laboratory of Advanced Ferrometallurgy,Shanghai University(SKLASS 2021-04)the Science and Technology Commission of Shanghai Municipality(22010500400)“Joint International Laboratory on Environmental and Energy Frontier Materials”and“Innovation Research Team of High–Level Local Universities in Shanghai”in Shanghai University。
文摘The widespread interest in layered P2-type Mn-based cathode materials for sodium-ion batteries(SIBs)stems from their cost-effectiveness and abundant resources.However,the inferior cycle stability and mediocre rate performance impede their further development in practical applications.Herein,we devised a wet chemical precipitation method to deposit an amorphous aluminum phosphate(AlPO_(4),denoted as AP)protective layer onto the surface of P2-type Na_(0.55)Ni_(0.1)Co_(0.7)Mn_(0.8)O_(2)(NCM@AP).The resulting NCM@5AP electrode,with a 5 wt%coating,exhibits extended cycle life(capacity retention of78.4%after 200 cycles at 100 mA g^(-1))and superior rate performance(98 mA h g^(-1)at 500 mA g^(-1))compared to pristine NCM.Moreover,our investigation provides comprehensive insights into the phase stability and active Na^(+)ion kinetics in the NCM@5AP composite electrode,shedding light on the underlying mechanisms responsible for the enhanced performance observed in the coated electrode.
基金funded by the National Natural Science Foundation of China(Grant Nos.22279092 and 5202780089).
文摘Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.
基金support of the Fundamental Research Funds for the Central Universities(No.2022CDJQY-004)the Fund for Innovative Research Groups of Natural Science Foundation of Hebei Province(No.A2020202002).
文摘Recently,poly(ethylene oxide)(PEO)-based solid polymer electrolytes have been attracting great attention,and efforts are currently underway to develop PEO-based composite electrolytes for next generation high performance all-solid-state lithium metal batteries.In this article,a novel sandwich structured solid-state PEO composite electrolyte is developed for high performance all-solid-state lithium metal batteries.The PEO-based composite electrolyte is fabricated by hot-pressing PEO,LiTFSI and Ti_(3)C_(2)T_(x) MXene nanosheets into glass fiber cloth(GFC).The as-prepared GFC@PEO-MXene electrolyte shows high mechanical properties,good electrochemical stability,and high lithium-ion migration number,which indicates an obvious synergistic effect from the microscale GFC and the nanoscale MXene.Such as,the GFC@PEO-1 wt%MXene electrolyte shows a high tensile strength of 43.43 MPa and an impressive Young's modulus of 496 MPa,which are increased by 1205%and 6048%over those of PEO.Meanwhile,the ionic conductivity of GFC@PEO-1 wt%MXene at 60℃ reaches 5.01×10^(-2) S m^(-1),which is increased by around 200%compared with that of GFC@PEO electrolyte.In addition,the Li/Li symmetric battery based on GFC@PEO-1 wt%MXene electrolyte shows an excellent cycling stability over 800 h(0.3 mA cm^(-2),0.3 mAh cm^(-2)),which is obviously longer than that based on PEO and GFC@PEO electrolytes due to the better compatibility of GFC@PEO-1 wt%MXene electrolyte with Li anode.Furthermore,the solid-state Li/LiFePO_(4) battery with GFC@PEO-1 wt%MXene as electrolyte demonstrates a high capacity of 110.2–166.1 mAh g^(-1) in a wide temperature range of 25–60C,and an excellent capacity retention rate.The developed sandwich structured GFC@PEO-1 wt%MXene electrolyte with the excellent overall performance is promising for next generation high performance all-solid-state lithium metal batteries.
基金the Natural Science Foundation of China (22005250)National Key R D Program of China (2022YFB2502000)FWO (12ZV320N)。
文摘The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges.
基金supported by the National Natural Science Foundation of China(22179063)。
文摘Potassium ion batteries(PIBs)are emerging as potential next-generation energy storage systems on account of their low cost and high theoretical energy density.Nevertheless,they also face challenges of low specific capacity and suboptimal cycling stability.Herein,we synthesize a cocoon-like P3-type K_(0.5)Mn_(0.7)Ni_(0.3)O_(2)(KMNO)cathode material by a self-template method.The KMNO cocoons possess a hierarchical layered architecture composed of nanoparticle stacking,which can accelerate the transport kinetics of potassium ions,mitigate the stress caused by K^(+)intercalation and deintercalation,and improve structural stability.In addition,Ni can not only alleviate the Jahn-Teller distortion and suppress the phase transition to stabilize the structure,but also act as an electrochemically active element,providing the capacity of two electrons from Ni2+to Ni4+.Combining the advantages of structure and nickel substitution,the P3-type KMNO cocoons are used for electrochemical performance testing of PIB cathodes,delivering an excellent rate capability of 57.1 m A h g^(-1)at 500 m A g^(-1)and a remarkable cycling stability of 77.0%over 300 cycles at 100 m A g^(-1).Impressively,the KMNO cocoons//pitch-derived soft carbon assembled full battery exhibits superior electrochemical performance with a reversible capacity of 79.7 m A h g^(-1)at 50 m A g^(-1).Moreover,ex-situ XRD also further reveals a solid solution phase reaction with a volume change of only 1.46%.This work furnishes a suitable approach to fabricating highperformance layered oxide cathodes for PIBs with outstanding cycling stability and rate capability.
基金supported by an Early Career Faculty Grant from NASA’s Space Technology Research Grants Program (80NSSC18K1509)supported by the Institute for Electronics and Nanotechnology Seed Grant and performed in part at the Georgia Tech Institute for Electronics and Nanotechnology, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which was supported by the National Science Foundation (ECCS-2025462)
文摘As lithium(Li)-ion batteries expand their applications,operating over a wide temperature range becomes increasingly important.However,the lowtemperature performance of conventional graphite anodes is severely hampered by the poor diffusion kinetics of Li ions(Li^(+)).Here,zinc oxide(ZnO) nanoparticles are incorporated into the expanded graphite to improve Li^(+)diffusion kinetics,resulting in a significant improvement in lowtemperature performance.The ZnO-embedded expanded graphite anodes are investigated with different amounts of ZnO to establish the structurecharge storage mechanism-performance relationship with a focus on lowtemperature applications.Electrochemical analysis reveals that the ZnOembedded expanded graphite anode with nano-sized ZnO maintains a large portion of the diffusion-controlled charge storage mechanism at an ultra-low temperature of-50℃ Due to this significantly enhanced Li^(+)diffusion rate,a full cell with the ZnO-embedded expanded graphite anode and a LiNi_(0.88)Co_(0.09)Al_(0.03)O_(2)cathode delivers high capacities of 176 mAh g^(-1)at20℃ and 86 mAh g^(-1)at-50℃ at a high rate of 1 C.The outstanding low-temperature performance of the composite anode by improving the Li^(+)diffusion kinetics provides important scientific insights into the fundamental design principles of anodes for low-temperature Li-ion battery operation.
基金financial support from National Natural Science Foundation of China (No. 21373006 and No. 51801030)the Science and Technology Program of Suzhou (SYG201732)+4 种基金the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)the project of Scientific and Technologic Infrastructure of Suzhou (SZS201708)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China (17KJB430029)One-hundred Young Talents (Class A) of Guangdong University of Technology (No. 220413198)Natural Science Foundation of Guangdong Providence (No. 2018A030310571)
文摘In this manuscript, we have demonstrated the delicate design and synthesis of bimetallic oxides nanoparticles derived from metal–oleate complex embedded in 3D graphene networks(MnO/CoMn_2O_4 GN), as an anode material for lithium ion batteries. The novel synthesis of the MnO/CoMn_2O_4 GN consists of thermal decomposition of metal–oleate complex containing cobalt and manganese metals and oleate ligand, forming bimetallic oxides nanoparticles, followed by a selfassembly route with reduced graphene oxides. The MnO/CoMn_2O_4 GN composite, with a unique architecture of bimetallic oxides nanoparticles encapsulated in 3D graphene networks, rationally integrates several benefits including shortening the di usion path of Li^+ ions, improving electrical conductivity and mitigating volume variation during cycling. Studies show that the electrochemical reaction processes of MnO/Co Mn_2O_4 GN electrodes are dominated by the pseudocapacitive behavior, leading to fast Li^+ charge/discharge reactions. As a result, the MnO/CoMn_2O_4 GN manifests high initial specific capacity, stable cycling performance, and excellent rate capability.
基金support from National Natural Science Foundation of China(Grant Nos.51872196)Natural Science Foundation of Tianjin,China(Grant No.17JCJQJC44100)+3 种基金National Postdoctoral Program for Innovative Talent(No.BX20190232)China Postdoctoral Science Foundation(No.2019M660059)Jiangxi Provincial Natural Science Foundation(Grant no.20202ACBL214007)Opening Project of Key Laboratory of Materials Processing and Mold.
文摘The future of high-energy density electrochemical energy storage systems relies on the advancement of rechargeable batteries that utilize reactive metals as anodes.In the alkaline metal,secondary battery systems because of abundant resource,high capacity and low redox potential,potassium(K)metal secondary battery(KMB)is expected to replace the existing lithiumion battery as a versatile platform for high-energy density,cost-effective energy storage devices.However,the difficulty in processing metal K results in nonstandard electrodes and hinders the development of KMBs.Furthermore,the mobility of the K metal anode due to its unique lowmelting point character at elevated temperatures in practical conditions leads to severe instability and risks in chemical/electrochemical processes.Herein,we fabricate a processable and moldable composite K metal anode by encapsulating K into reduced graphene oxide(rGO).The composite electrode can be engineered into various shapes discretionarily with precise sizes and stabilize the K metal anode at relatively high temperatures.Remarkably,the composite anode exhibits excellent cycling performance at high current density(8 mA cm^(-2)) with dendrite-free morphology.Paired with a Prussian blue cathode,the rGO-K composite anode shows much improved electrochemical performance and extended lifetime.
基金supported by the Key Projects of Intergovernmental International Cooperation in Key R&D Programs of the Ministry of Science and Technology of China(No.2021YFE0115800)the National Science Funding Committee of China(No.U20A20250)。
文摘The development of clean renewable energy and energy storage devices is of great significance under the present energy crisis and environmental pollution background.Aqueous zinc-ion battery(ZIB)has become one of the most promising energy storage devices due to its high capacity,safety and low cost.However,the application of ZIB cathode is usually limited by low capacity and poor stability.Herein,we propose a novel heterostructure MnO/MnV_(2)O_(4)composite material composed of MOF derivatives and spinel with dual active components as cathode for ZIBs.Benefited from substantial framework of MOF derivatives and the synergistic effect of heterostructures,MnO/MnV_(2)O_(4)exhibits excellent rate performance(342 m Ah/g at 0.1 A/g,261 mAh/g at 15 A/g)and cycling performance(198.9 mAh/g at 10 A/g after 2000 cycles)in3 mol/L Zn(CF_(3)SO_(3))2electrolytes.This work extends the range of developing high-performance cathodes for ZIBs under high current density and is expected to enlighten the optimization of commercial energy storage devices.
基金supported by the National Natural Science Foundation of China(No.21501015)the Hunan Provincial Natural Science Foundation,China(No.2022JJ30604)Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation,China(No.2022CL01)。
文摘A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes.Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.%CAB(PL-CAB-10%)exhibits high ionic conductivity(8.42×10~(-4)S/cm at 60℃),high Li+transference number(0.46),wide electrochemical window(4.91 V),good thermal stability,and outstanding mechanical properties.Furthermore,PL-CAB-10%exhibits excellent cycle stability in both Li-Li symmetric battery and Li/PL-CAB-10%/LiFePO4 asymmetric battery setups.These enhanced performances are primarily attributable to the introduction of the versatile CAB.The abundant metal sites in CAB can react with TFSI~-and PEO through Lewis acid-base interactions,promoting LiTFSI dissociation and improving ionic conductivity.Additionally,regular pores in CAB provide uniformly distributed sites for cation plating during cycling.
基金supported by the National Key Research and Development Program of China(No.2022YFA1203500)the National Natural Science Foundation of China(Nos.51972124 and 51902115)the Opening Project of Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing&Finishing(No.223009025).
文摘Two-dimensional(2D)materials have attracted a great deal of research interest because of their unique electrical,magnetic,optical,mechanical,and catalytic properties for various applications.To date,however,it is still difficult to fabricate most functional oxides as 2D materials unless they have a layered structure.Herein,we report a one-step universal strategy for preparing versatile non-layered oxide nanosheets by directly annealing the mixture of metal nitrate and dimethyl imidazole(2-MI).The 2-MI plays the key role for 2D oxides since 2-MI owns a very low molten point and sublimation temperature,in which its molten liquid can coordinate with metal ions,forming a metal-organic framework,and easily puffing by its gas molecules.A total of 17 materials were prepared by this strategy,including non-layered metal oxide nanosheets as well as metal/metal oxide loaded nitrogen-doped carbon nanosheets.The as-prepared cobalt particle-loaded nitrogen-doped carbon nanosheets(Co@N/C)exhibit remarkable bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalytic activity and durability.Besides,the Zn-air battery utilizing a Co@N/C catalyst exhibits high power density of 174.3 mW·cm^(-2).This facile strategy opens up a new way for large-scale synthesis of 2D oxides that holds great potential to push 2D oxides for practical applications.
基金support from the China Postdoctoral Science Foundation(Nos.2022TQ0173 and 2023M731922).
文摘Polyethylene oxide(PEO)-based solid-state electrolytes are considered ideal for electrolyte materials in solid-state lithium metal batteries(SSLMBs).However,practical applications are hindered by the lower conductivity and poor interfacial stability.Here,we propose a strategy to construct a three-dimensional(3D)fiber network of metal-organic frameworks(MOFs).Composite solid electrolytes(CSEs)with continuous ion transport pathways were fabricated by filling a PEO polymer matrix in fibers containing interconnected MOFs.This 3D fiber network provides a fast Li+transport path and effectively improves the ionic conductivity(1.36×10^(-4) S·cm^(-1),30℃).In addition,the network of interconnected MOFs not only effectively traps the anions,but also provides sufficient mechanical strength to prevent the growth of Li dendrites.Benefiting from the advantages of structural design,the CSEs stabilize the Li/electrolyte interface and extend the cycle life of the Li-symmetric cells to 3000 h.The assembled SSLMBs exhibit excellent cycling performance at both room and high temperatures.In addition,the constructed pouch cells can provide an areal capacity of 0.62 mA·h·cm^(-2),which can still operate under extreme conditions.This work provides a new strategy for the design of CSEs with continuous structure and stable operation of SSLMBs.