Given the rise in the popularity of wearable electronics that are able to deform into desirable configurations while maintaining electrochemical functionality,stretchable and flexible(hybrid)supercapacitors(SCs)have b...Given the rise in the popularity of wearable electronics that are able to deform into desirable configurations while maintaining electrochemical functionality,stretchable and flexible(hybrid)supercapacitors(SCs)have become increasingly of interest as innovative energy storage devices.Their outstanding power density,long lifetime with low capacitance loss,and appropriate energy density,in particular in hybrid cases make them ideal candidates for flexible electronics.The aim of this review paper is to provide an in-depth discussion of these stretchable and flexible SCs ranging from fabrication to electro-mechanical properties.This review paper begins with a short overview of the fundamentals of charge storage mechanisms and different types of multivalent metal-ion hybrid SCs.The research methods leading up to the current state of these stretchable and flexible SCs are then presented.This is followed by an in-depth presentation of the challenges associated with the fabrication methods for different configurations.Proposed novel strategies to maximize the elastic and electrochemical properties of stretchable/flexible or quasi-solid-state SCs are classified and the pros and cons associated with each are shown.The advances in mechanical properties and the expected advancements for the future of these SCs are discussed in the last section.展开更多
Construction of advanced electrode materials with unique performance for supercapacitors(SCs)is essential to achieving high implementation in the commercial market.Here,we report a novel peripheral octamethyl-substitu...Construction of advanced electrode materials with unique performance for supercapacitors(SCs)is essential to achieving high implementation in the commercial market.Here,we report a novel peripheral octamethyl-substituted nickel(Ⅱ)phthalocyanine(Ni Me_(2)Pc)-based nanocomposite as the electrode material of all-solid-state SCs.The highly redox-active NiMe_(2)Pc/carboxylated carbon nanotube(CNTCOOH)dendritic nanocomposite provides rapid electron/electrolyte ion-transport pathways and exhibits excellent structural stability,resulting in high-capacity activity and impressive cycling stability.The composite prepared with the optimized weight ratio of Ni Me_(2)Pc:CNT-COOH(6:10)showed the highest specific capacitance of 330.5 F g^(-1)at 0.25 A g^(-1).The constructed NiMe_(2)Pc/CNT-COOH-based all-solid-state symmetric SC device showed excellent performance with a maximum energy density of 22.8 Wh kg^(-1)and outstanding cycling stability(111.6%retained after 35,000 cycles).Moreover,flexible carbon cloth significantly enhanced the energy density of the NiMe_(2)Pc/CNT-COOH all-solid-state symmetric device to 52.1 Wh kg^(-1)with 95.4%capacitance retention after 35,000 cycles,and it could be applied to highperformance flexible electronics applications.These findings provide a novel strategy to design phthalocyanine-based electrode materials for next-generation flexible SC devices.展开更多
Solid-state batteries are commonly acknowledged as the forthcoming evolution in energy storage technologies.Recent development progress for these rechargeable batteries has notably accelerated their trajectory toward ...Solid-state batteries are commonly acknowledged as the forthcoming evolution in energy storage technologies.Recent development progress for these rechargeable batteries has notably accelerated their trajectory toward achieving commercial feasibility.In particular,all-solid-state lithium-sulfur batteries(ASSLSBs)that rely on lithium-sulfur reversible redox processes exhibit immense potential as an energy storage system,surpassing conventional lithium-ion batteries.This can be attributed predominantly to their exceptional energy density,extended operational lifespan,and heightened safety attributes.Despite these advantages,the adoption of ASSLSBs in the commercial sector has been sluggish.To expedite research and development in this particular area,this article provides a thorough review of the current state of ASSLSBs.We delve into an in-depth analysis of the rationale behind transitioning to ASSLSBs,explore the fundamental scientific principles involved,and provide a comprehensive evaluation of the main challenges faced by ASSLSBs.We suggest that future research in this field should prioritize plummeting the presence of inactive substances,adopting electrodes with optimum performance,minimizing interfacial resistance,and designing a scalable fabrication approach to facilitate the commercialization of ASSLSBs.展开更多
MXenes are a family of two-dimensional(2D)layered transition metal carbides/nitrides that show promising potential for energy storage applications due to their high-specific surface areas,excellent electron conductivi...MXenes are a family of two-dimensional(2D)layered transition metal carbides/nitrides that show promising potential for energy storage applications due to their high-specific surface areas,excellent electron conductivity,good hydrophilicity,and tunable terminations.Among various types of MXenes,Ti_(3)C_(2)T_(x) is the most widely studied for use in capacitive energy storage applications,especially in supercapacitors(SCs).However,the stacking and oxidation of MXene sheets inevitably lead to a significant loss of electrochemically active sites.To overcome such challenges,carbon materials are frequently incorporated into MXenes to enhance their electrochemical properties.This review introduces the common strategies used for synthesizing Ti_(3)C_(2)T_(x),followed by a comprehensive overview of recent developments in Ti_(3)C_(2)T_(x)/carbon composites as electrode materials for SCs.Ti_(3)C_(2)T_(x)/carbon composites are categorized based on the dimensions of carbons,including 0D carbon dots,1D carbon nanotubes and fibers,2D graphene,and 3D carbon materials(activated carbon,polymer-derived carbon,etc.).Finally,this review also provides a perspective on developing novel MXenes/carbon composites as electrodes for application in SCs.展开更多
Poly(ethylene oxide)(PEO)-based polymer electrolytes show the prospect in all-solid-state lithium metal batteries;however,they present limitations of low room-temperature ionic conductivity,and interfacial incompatibi...Poly(ethylene oxide)(PEO)-based polymer electrolytes show the prospect in all-solid-state lithium metal batteries;however,they present limitations of low room-temperature ionic conductivity,and interfacial incompatibility with high voltage cathodes.Therefore,a salt engineering of 1,1,2,2,3,3-hexafluoropropane-1,3-disulfonimide lithium salt(LiHFDF)/LiTFSI system was developed in PEO-based electrolyte,demonstrating to effectively regulate Li ion transport and improve the interfacial stability under high voltage.We show,by manipulating the interaction between PEO matrix and TFSI^(-)-HFDF^(-),the optimized solid-state polymer electrolyte achieves maximum Li+conduction of 1.24×10^(-4)S cm^(-1)at 40℃,which is almost 3 times of the baseline.Also,the optimized polymer electrolyte demonstrates outstanding stable cycling in the LiFePO_(4)/Li and LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)/Li(3.0-4.4 V,200 cycles)based all-solid-state lithium batteries at 40℃.展开更多
This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applicati...This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applications using an experimental/theorical approach.The surface modification of CF by rGO and/or by PPy electrodeposited at 10,25 and 50 mV s^(-1) was thoroughly examined physicochemical and electrochemically.Composite electrodes comprising CF-rGo-PPy,synthesized via electropolymerization at 25 mV s^(-1),demonstrated a remarkable increase in capacitance,showcasing~742 F g^(-1) compared to 153 F g^(-1) for CF.SEM,N_(2)-surface area,XPS,and TD-DFT approach revealed that the higher capacitance observed in CF-rGo-PPy electrodes underscores the influence of morphology and charged nitrogen species on the electrochemical performance of these modified electrodes.Notably,this electrode material achieves a specific capacitance retention of~96%of their initial capacitance after 10000 cycles at 0.5 A g^(-1) measured in a two-electrodes cell configuration.This work also discusses the influence of the scan rate used for pyrrole electropolymerization on the pseudocapacitance contribution of PPy and its possible effect on the porosity of the material.These results highlight the importance of appropriate electropolymerization conditions that allow obtaining the synergistic effect between CF,rGO and PPy.展开更多
Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries.In this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg elec...Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries.In this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg electrolyte that prepared by a NH_(3)redistribution between 3D framework-γ-Mg(BH_(4))_(2)and Mg(BH_(4))_(2)·6NH_(3).Amorphous Mg(BH_(4))_(2)·2NH_(3)exhibits a high Mg-ion conductivity of 5×10^(-4)S cm^(-1)at 75℃,which is attributed to the fast migration of abundant Mg vacancies according to the theoretical calculations.Moreover,amorphous Mg(BH_(4))_(2)·2NH_(3)shows an apparent electrochemical stability window of 0-1.4 V with the help of in-situ formed interphases,which can prevent further side reactions without hindering the Mg-ion transfer.Based on the above superiorities,amorphous Mg(BH_(4))_(2)·2NH_(3)enables the stable cycling of all-solid-state Mg cells,as the critical current density reaches 3.2 mA cm^(-2)for Mg symmetrical cells and the reversible specific capacity reaches 141 mAh g^(-1)with a coulombic efficiency of 91.7%(first cycle)for Mg||TiS_(2)cells.展开更多
In recent years,paper-based functional materials have received extensive attention in the field of energy storage due to their advantages of rich and adjustable porous network structure and good flexibility.As an impo...In recent years,paper-based functional materials have received extensive attention in the field of energy storage due to their advantages of rich and adjustable porous network structure and good flexibility.As an important energy storage device,paper-based supercapacitors have important application prospects in many fields and have also received extensive attention from researchers in recent years.At present,researchers have modified and regulated paper-based materials by different means such as structural design and material composition to enhance their electrochemical storage capacity.The development of paper-based supercapacitors provides an important direction for the development of green and sustainable energy.Therefore,it is of great significance to summarize the relevant work of paper-based supercapacitors for their rapid development and application.In this review,the recent research progress of paper-based supercapacitors based on cellulose was summarized in terms of various cellulose-based composites,preparation skills,and electrochemical performance.Finally,some opinions on the problems in the development of this field and the future development trend were proposed.It is hoped that this review can provide valuable references and ideas for the rapid development of paper-based energy storage devices.展开更多
The development of self-charging supercapacitor power cells(SCSPCs)has profound implications for smart electronic devices used in different fields.Here,we epitaxially electrodeposited Mo-and Fe-codoped MnO_(2)films on...The development of self-charging supercapacitor power cells(SCSPCs)has profound implications for smart electronic devices used in different fields.Here,we epitaxially electrodeposited Mo-and Fe-codoped MnO_(2)films on piezoelectric ZnO nanoarrays(NAs)grown on the flexible carbon cloth(denoted ZnO@Mo-Fe-MnO_(2)NAs).A self-charging supercapacitor power cell device was assembled with the Mo-and Fe-codoped MnO_(2)nanoarray electrode and poly(vinylidenefluoride-co-trifluoroethylene)(PVDF-Trfe)piezoelectric film doped with BaTiO_(3)(BTO)and carbon nanotubes(CNTs)(denoted PVDF-Trfe/CNTs/BTO).The self-charging supercapacitor power cell device exhibited an energy density of 30μWh cm^(-2)with a high power density of 40 mW cm^(-2)and delivered an excellent self-charging performance of 363 mV(10 N)driven by both the piezoelectric ZnO nanoarrays and the poly(vinylidenefluoride-co-trifluoroethylene)piezoelectric film doped with BaTiO_(3)and carbon nanotubes.More intriguingly,the device could also be self-charged by 184 mV due to residual stress alone and showed excellent energy conversion efficiency and low self-discharge rate.This work illustrates for the first time the self-charging mechanism involving electrolyte ion migration driven by both electrodes and films.A comprehensive analysis strongly confirmed the important contribution of the piezoelectric ZnO nanoarrays in the self-charging process of the self-charging supercapacitor power cell device.This work provides novel directions and insights for the development of selfcharging supercapacitor power cells.展开更多
Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to dras...Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.展开更多
Supercapacitors(SCs)are considered promising energy storge systems because of their outstanding power density,fast charge and discharge rate and long-term cycling stability.The exploitation of cheap and efficient elec...Supercapacitors(SCs)are considered promising energy storge systems because of their outstanding power density,fast charge and discharge rate and long-term cycling stability.The exploitation of cheap and efficient electrode materials is the key to improve the performance of supercapacitors.As the battery-type materials,transition metal phosphides(TMPs)possess high theoretical specific capacity,good electrical conductivity and superior structural stability,which have been extensively studied to be electrode materials for supercapacitors.In this review,we summarize the up-to-date progress on TMPs materials from diversified synthetic methods,diverse nanostructures and several prominent TMPs and their composites in application of supercapacitors.In the end,we also propose the remaining challenges toward the rational discovery and synthesis of high-performance TMP electrodes materials for energy storage.展开更多
All-solid-state batteries(ASSBs)are a class of safer and higher-energy-density materials compared to conventional devices,from which solid-state electrolytes(SSEs)are their essential components.To date,investigations ...All-solid-state batteries(ASSBs)are a class of safer and higher-energy-density materials compared to conventional devices,from which solid-state electrolytes(SSEs)are their essential components.To date,investigations to search for high ion-conducting solid-state electrolytes have attracted broad concern.However,obtaining SSEs with high ionic conductivity is challenging due to the complex structural information and the less-explored structure-performance relationship.To provide a solution to these challenges,developing a database containing typical SSEs from available experimental reports would be a new avenue to understand the structureperformance relationships and find out new design guidelines for reasonable SSEs.Herein,a dynamic experimental database containing>600 materials was developed in a wide range of temperatures(132.40–1261.60 K),including mono-and divalent cations(e.g.,Li^(+),Na^(+),K^(+),Ag^(+),Ca^(2+),Mg^(2+),and Zn^(2+))and various types of anions(e.g.,halide,hydride,sulfide,and oxide).Data-mining was conducted to explore the relationships among different variates(e.g.,transport ion,composition,activation energy,and conductivity).Overall,we expect that this database can provide essential guidelines for the design and development of high-performance SSEs in ASSB applications.This database is dynamically updated,which can be accessed via our open-source online system.展开更多
Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and ...Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer-thin SPE layer-cathode integration(MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore,the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+deposition and excellent cycling stability. High capacity(142.8 mAh g-1), stable operation of 140 cycles(capacity decay per cycle, 0.065%), and low polarization potential(0.5 C) are obtained in this Li|MXene-PEO-LFP cell,which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery.展开更多
Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlatio...Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.展开更多
A commentary on pressure-induced pre-lithiation towards Si anodes in allsolid-state Li-ion batteries(ASSLIBs)using sulfide electrolytes(SEs)is presented.First,feasible pre-lithiation technologies for Si anodes in SE-b...A commentary on pressure-induced pre-lithiation towards Si anodes in allsolid-state Li-ion batteries(ASSLIBs)using sulfide electrolytes(SEs)is presented.First,feasible pre-lithiation technologies for Si anodes in SE-based ASSLIBs especially the significant pressure-induced pre-lithiation strategies are briefly reviewed.Then,a recent achievement by Meng et al.in this field is elaborated in detail.Finally,the significance of Meng’s work is discussed.展开更多
The application of Li-rich Mn-based cathodes, the most promising candidates for high-energy-density Liion batteries, in all-solid-state batteries can further enhance the safety and stability of battery systems.However...The application of Li-rich Mn-based cathodes, the most promising candidates for high-energy-density Liion batteries, in all-solid-state batteries can further enhance the safety and stability of battery systems.However, the utilization of high-capacity Li-rich cathodes has been limited by sluggish kinetics and severe interfacial issues in all-solid-state batteries. Here, a multi-functional interface modification strategy involving dispersed submicron single-crystal structure and multi-functional surface modification layer obtained through in-situ interfacial chemical reactions was designed to improve the electrochemical performance of Li-rich Mn-based cathodes in all-solid-state batteries. The design of submicron single-crystal structure promotes the interface contact between the cathode particles and the solid-state electrolyte,and thus constructs a more complete ion and electron conductive network in the composite cathode.Furthermore, the Li-gradient layer and the lithium molybdate coating layer constructed on the surface of single-crystal Li-rich particles accelerate the transport of Li ions at the interface, suppress the side reactions between cathodes and electrolyte, and inhibit the oxygen release on the cathode surface. The optimized Li-rich cathode materials exhibit excellent electrochemical performance in halide all-solid-state batteries. This study emphasizes the vital importance of reaction kinetics and interfacial stability of Lirich cathodes in all-solid-state batteries and provides a facile modification strategy to enhance the electrochemical performance of all-solid-state batteries based on Li-rich cathodes.展开更多
The stacking and aggregation of graphene nanosheets have been obstacles to their application as electrode materials for microelectronic devices.This study deploys a one-step,scalable,facile electrochemical exfoliation...The stacking and aggregation of graphene nanosheets have been obstacles to their application as electrode materials for microelectronic devices.This study deploys a one-step,scalable,facile electrochemical exfoliation technique to fabricate nitrogen(N)and chlorine(Cl)co-doped graphene nanosheets(i.e.,N-Cl-G)via the application of constant voltage on graphite in a mixture of 0.1 mol/L H_(2)SO_(4)and 0.1 mol/L NH_(4)Cl without using dangerous and exhaustive operation.The introduction of Cl(with its large radius)and N,both with high electrical negativity,facilitates the modulation of the electronic structure of graphene and creation of rich structural defects in it.Consequently,in the as-constructed supercapacitors,N-Cl-G exhibits a high specific capacitance of 77 F/g at 0.2 A/g and remarkable cycling stability with 91.7%retention of initial capacitance after 20,000 cycles at 10 A/g.Furthermore,a symmetrical supercapacitor assembled with N-Cl-G as the positive and negative electrodes(denoted as N-Cl-G//N-Cl-G)exhibits an energy density of 3.38 Wh/kg at a power density of 600 W/kg and superior cycling stability with almost no capacitance loss after 5000 cycles at 5 A/g.This study provides a scalable protocol for the facile fabrication of high-performance co-doped graphene as an electrode material candidate for supercapacitors.展开更多
Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,i...Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial application.Herein,we report a liquid metal-coated lithium metal(LM@Li)anode strategy to improve the contact between lithium metal and a Li6PS5Cl inorganic electrolyte.The LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2mA cm^(-2) and a significantly higher critical current density of 9.8 mAcm^(-2) at 25°C.In addition,a full battery assembled with a high-capacity composite LiNbO3@-LiNi_(0.7)Co_(0.2)Mn_(0.1)O_(2)(LNO@NCM721)cathode shows stable cycling performance.Experimental and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.展开更多
All-solid-state lithium-sulfur batteries(ASSLSBs) have become one of the most potential candidates for the next-generation high-energy systems due to their intrinsic safety and high theoretical energy density.However,...All-solid-state lithium-sulfur batteries(ASSLSBs) have become one of the most potential candidates for the next-generation high-energy systems due to their intrinsic safety and high theoretical energy density.However, PEO-based ASSLSBs face the dilemma of insufficient Coulombic efficiency and long-term stability caused by the coupling problems of dendrite growth of anode and polysulfide shuttle of cathode. In this work, 1,3,5-trioxane(TOX) is used as a functional additive to design a PEO-based composite solidstate electrolyte(denoted as TOX-CSE), which realizes the stable long-term cycle of an ASSLSB. The results show that TOX can in-situ decompose on the anode to form a composite solid electrolyte interphase(SEI) layer with rich-organic component. It yields a high average modulus of 5.0 GPa, greatly improving the mechanical stability of the SEI layer and thus inhibiting the growth of dendrites. Also,the robust SEI layer can act as a barrier to block the side reaction between polysulfides and lithium metal.As a result, a Li-Li symmetric cell assembled with a TOX-CSE exhibits prolonged cycling stability over 2000 h at 0.2 m A cm^(-2). The ASSLSB also shows a stable cycling performance of 500 cycles at 0.5 C.This work reveals the structure–activity relationship between the mechanical property of interface layer and the battery's cycling stability.展开更多
Solid polymer electrolytes(SPEs)are highly promising for realizing high-capacity,low-cost,and safe Li metal batteries.However,the Li dendritic growth and side reactions between Li and SPEs also plague these systems.He...Solid polymer electrolytes(SPEs)are highly promising for realizing high-capacity,low-cost,and safe Li metal batteries.However,the Li dendritic growth and side reactions between Li and SPEs also plague these systems.Herein,a fluorinated lithium salt coating(FC)with organic-inorganic gradient and soft–rigid feature is introduced on Li surface as an artificial protective layer by the in-situ reaction between Li metal and fluorinated carboxylic acid.The FC layer can improve the interface stability and wettability between Li and SPEs,assist the transport of Li ions,and guide Li nucleation,contributing to a dendrite-free Li deposition and long-lifespan Li metal batteries.The symmetric cell with FC-Li anodes exhibits a high areal capacity of 1 mAh cm^(-2)at 0.5 mA cm^(-2),and an ultra-long lifespan of 2000 h at a current density of 0.1 mA cm^(-2).Moreover,the full cell paired with the LiFePO4 cathode exhibits improved cycling stability,remaining 83.7%capacity after 500 cycles at 1 C.When matching with the S cathode,the FC layer can prevent the shuttle effect,contributing to stable and high-capacity Li–S battery.This work provided a promising way for the construction of stable all-solid-state lithium metal batteries with prolonged lifespan.展开更多
文摘Given the rise in the popularity of wearable electronics that are able to deform into desirable configurations while maintaining electrochemical functionality,stretchable and flexible(hybrid)supercapacitors(SCs)have become increasingly of interest as innovative energy storage devices.Their outstanding power density,long lifetime with low capacitance loss,and appropriate energy density,in particular in hybrid cases make them ideal candidates for flexible electronics.The aim of this review paper is to provide an in-depth discussion of these stretchable and flexible SCs ranging from fabrication to electro-mechanical properties.This review paper begins with a short overview of the fundamentals of charge storage mechanisms and different types of multivalent metal-ion hybrid SCs.The research methods leading up to the current state of these stretchable and flexible SCs are then presented.This is followed by an in-depth presentation of the challenges associated with the fabrication methods for different configurations.Proposed novel strategies to maximize the elastic and electrochemical properties of stretchable/flexible or quasi-solid-state SCs are classified and the pros and cons associated with each are shown.The advances in mechanical properties and the expected advancements for the future of these SCs are discussed in the last section.
基金supported by the National Natural Science Foundation of China(Grant Nos.21975116 and 51950410598)the Major Program of Guangdong Basic and Applied Research(Grant No.2019B121205001)+2 种基金Shenzhen NSQKJJ(Grant No.K20799112)the Shenzhen Science and Technology Innovation Committee(Project No.JCYJ20170412154426330)the‘‘Climbing Program”Special Funds(Project No.pdjh2021c0027)。
文摘Construction of advanced electrode materials with unique performance for supercapacitors(SCs)is essential to achieving high implementation in the commercial market.Here,we report a novel peripheral octamethyl-substituted nickel(Ⅱ)phthalocyanine(Ni Me_(2)Pc)-based nanocomposite as the electrode material of all-solid-state SCs.The highly redox-active NiMe_(2)Pc/carboxylated carbon nanotube(CNTCOOH)dendritic nanocomposite provides rapid electron/electrolyte ion-transport pathways and exhibits excellent structural stability,resulting in high-capacity activity and impressive cycling stability.The composite prepared with the optimized weight ratio of Ni Me_(2)Pc:CNT-COOH(6:10)showed the highest specific capacitance of 330.5 F g^(-1)at 0.25 A g^(-1).The constructed NiMe_(2)Pc/CNT-COOH-based all-solid-state symmetric SC device showed excellent performance with a maximum energy density of 22.8 Wh kg^(-1)and outstanding cycling stability(111.6%retained after 35,000 cycles).Moreover,flexible carbon cloth significantly enhanced the energy density of the NiMe_(2)Pc/CNT-COOH all-solid-state symmetric device to 52.1 Wh kg^(-1)with 95.4%capacitance retention after 35,000 cycles,and it could be applied to highperformance flexible electronics applications.These findings provide a novel strategy to design phthalocyanine-based electrode materials for next-generation flexible SC devices.
基金funded by the Ministry of Science and ICT through the National Research Foundation of Korea(202300262366)the Basic Research Lab(RS-2023-00219710)the Ministry of Commerce,Industry,and Energy(20025720)of Korea.
文摘Solid-state batteries are commonly acknowledged as the forthcoming evolution in energy storage technologies.Recent development progress for these rechargeable batteries has notably accelerated their trajectory toward achieving commercial feasibility.In particular,all-solid-state lithium-sulfur batteries(ASSLSBs)that rely on lithium-sulfur reversible redox processes exhibit immense potential as an energy storage system,surpassing conventional lithium-ion batteries.This can be attributed predominantly to their exceptional energy density,extended operational lifespan,and heightened safety attributes.Despite these advantages,the adoption of ASSLSBs in the commercial sector has been sluggish.To expedite research and development in this particular area,this article provides a thorough review of the current state of ASSLSBs.We delve into an in-depth analysis of the rationale behind transitioning to ASSLSBs,explore the fundamental scientific principles involved,and provide a comprehensive evaluation of the main challenges faced by ASSLSBs.We suggest that future research in this field should prioritize plummeting the presence of inactive substances,adopting electrodes with optimum performance,minimizing interfacial resistance,and designing a scalable fabrication approach to facilitate the commercialization of ASSLSBs.
基金supported by the Basic Scientific Research Funds for Colleges and Universities affiliated to Hebei Province(JST2022005)Thanks are given to the financial support from the National Natural Science Foundation of China(22005099).
文摘MXenes are a family of two-dimensional(2D)layered transition metal carbides/nitrides that show promising potential for energy storage applications due to their high-specific surface areas,excellent electron conductivity,good hydrophilicity,and tunable terminations.Among various types of MXenes,Ti_(3)C_(2)T_(x) is the most widely studied for use in capacitive energy storage applications,especially in supercapacitors(SCs).However,the stacking and oxidation of MXene sheets inevitably lead to a significant loss of electrochemically active sites.To overcome such challenges,carbon materials are frequently incorporated into MXenes to enhance their electrochemical properties.This review introduces the common strategies used for synthesizing Ti_(3)C_(2)T_(x),followed by a comprehensive overview of recent developments in Ti_(3)C_(2)T_(x)/carbon composites as electrode materials for SCs.Ti_(3)C_(2)T_(x)/carbon composites are categorized based on the dimensions of carbons,including 0D carbon dots,1D carbon nanotubes and fibers,2D graphene,and 3D carbon materials(activated carbon,polymer-derived carbon,etc.).Finally,this review also provides a perspective on developing novel MXenes/carbon composites as electrodes for application in SCs.
基金supported by National Natural Science Foundation of China(Grant No.U1930113),ChinaNational Natural Science Foundation of China(52072036)
文摘Poly(ethylene oxide)(PEO)-based polymer electrolytes show the prospect in all-solid-state lithium metal batteries;however,they present limitations of low room-temperature ionic conductivity,and interfacial incompatibility with high voltage cathodes.Therefore,a salt engineering of 1,1,2,2,3,3-hexafluoropropane-1,3-disulfonimide lithium salt(LiHFDF)/LiTFSI system was developed in PEO-based electrolyte,demonstrating to effectively regulate Li ion transport and improve the interfacial stability under high voltage.We show,by manipulating the interaction between PEO matrix and TFSI^(-)-HFDF^(-),the optimized solid-state polymer electrolyte achieves maximum Li+conduction of 1.24×10^(-4)S cm^(-1)at 40℃,which is almost 3 times of the baseline.Also,the optimized polymer electrolyte demonstrates outstanding stable cycling in the LiFePO_(4)/Li and LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)/Li(3.0-4.4 V,200 cycles)based all-solid-state lithium batteries at 40℃.
基金CONCYTEC and PROCIENCIA agencies from Peru in the framework of the call for Basic Research Projects2019-01[contract number401-2019-FONDECYT].
文摘This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applications using an experimental/theorical approach.The surface modification of CF by rGO and/or by PPy electrodeposited at 10,25 and 50 mV s^(-1) was thoroughly examined physicochemical and electrochemically.Composite electrodes comprising CF-rGo-PPy,synthesized via electropolymerization at 25 mV s^(-1),demonstrated a remarkable increase in capacitance,showcasing~742 F g^(-1) compared to 153 F g^(-1) for CF.SEM,N_(2)-surface area,XPS,and TD-DFT approach revealed that the higher capacitance observed in CF-rGo-PPy electrodes underscores the influence of morphology and charged nitrogen species on the electrochemical performance of these modified electrodes.Notably,this electrode material achieves a specific capacitance retention of~96%of their initial capacitance after 10000 cycles at 0.5 A g^(-1) measured in a two-electrodes cell configuration.This work also discusses the influence of the scan rate used for pyrrole electropolymerization on the pseudocapacitance contribution of PPy and its possible effect on the porosity of the material.These results highlight the importance of appropriate electropolymerization conditions that allow obtaining the synergistic effect between CF,rGO and PPy.
基金the support of the National Natural Science Foundation of China(51971146,51971147,52171218 and 52271222)the Shanghai Municipal Science and Technology Commission(21010503100)+3 种基金the Major Program for the Scientific Research Innovation Plan of Shanghai Education Commission(2019-01-07-00-07E00015)the Shanghai Outstanding Academic Leaders Plan,the Guangxi Key Laboratory of Information Materials(Guilin University of Electronic Technology,201017-K)the Shanghai Rising-Star Program(20QA1407100)the General Program of Natural Science Foundation of Shanghai(20ZR1438400)
文摘Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries.In this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg electrolyte that prepared by a NH_(3)redistribution between 3D framework-γ-Mg(BH_(4))_(2)and Mg(BH_(4))_(2)·6NH_(3).Amorphous Mg(BH_(4))_(2)·2NH_(3)exhibits a high Mg-ion conductivity of 5×10^(-4)S cm^(-1)at 75℃,which is attributed to the fast migration of abundant Mg vacancies according to the theoretical calculations.Moreover,amorphous Mg(BH_(4))_(2)·2NH_(3)shows an apparent electrochemical stability window of 0-1.4 V with the help of in-situ formed interphases,which can prevent further side reactions without hindering the Mg-ion transfer.Based on the above superiorities,amorphous Mg(BH_(4))_(2)·2NH_(3)enables the stable cycling of all-solid-state Mg cells,as the critical current density reaches 3.2 mA cm^(-2)for Mg symmetrical cells and the reversible specific capacity reaches 141 mAh g^(-1)with a coulombic efficiency of 91.7%(first cycle)for Mg||TiS_(2)cells.
基金supported by the fund of the National Natural Science Foundation of China(22078184,22171170)the China Postdoctoral Science Foundation(2019M653853XB)+1 种基金the Natural Science Advance Research Foundation of Shaanxi University of Science and Technology(2018QNBJ-03)Major Scientific and Technological Innovation Projects in Shandong Province(2019TSLH0316)
文摘In recent years,paper-based functional materials have received extensive attention in the field of energy storage due to their advantages of rich and adjustable porous network structure and good flexibility.As an important energy storage device,paper-based supercapacitors have important application prospects in many fields and have also received extensive attention from researchers in recent years.At present,researchers have modified and regulated paper-based materials by different means such as structural design and material composition to enhance their electrochemical storage capacity.The development of paper-based supercapacitors provides an important direction for the development of green and sustainable energy.Therefore,it is of great significance to summarize the relevant work of paper-based supercapacitors for their rapid development and application.In this review,the recent research progress of paper-based supercapacitors based on cellulose was summarized in terms of various cellulose-based composites,preparation skills,and electrochemical performance.Finally,some opinions on the problems in the development of this field and the future development trend were proposed.It is hoped that this review can provide valuable references and ideas for the rapid development of paper-based energy storage devices.
基金the support by the Key Research and Development Program of Jiangxi Province(20203BBE53069)the National Key R&D Program of China(2017YFA0208200)+5 种基金the National Natural Science Foundation of China(51862026,22022505,and 21872069)the Fundamental Research Funds for the Central Universities of China(02051438026,020514380272 and 020514380274)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220008)the Natural Science Foundation of Jiangxi Province(20192ACBL21048)the Nanjing International Col aboration Research Program(202201007 and 2022SX00000955)the Suzhou Gusu Leading Talent Program of Science and Technology Innovation and Entrepreneurship in Wujiang District(ZXL2021273)
文摘The development of self-charging supercapacitor power cells(SCSPCs)has profound implications for smart electronic devices used in different fields.Here,we epitaxially electrodeposited Mo-and Fe-codoped MnO_(2)films on piezoelectric ZnO nanoarrays(NAs)grown on the flexible carbon cloth(denoted ZnO@Mo-Fe-MnO_(2)NAs).A self-charging supercapacitor power cell device was assembled with the Mo-and Fe-codoped MnO_(2)nanoarray electrode and poly(vinylidenefluoride-co-trifluoroethylene)(PVDF-Trfe)piezoelectric film doped with BaTiO_(3)(BTO)and carbon nanotubes(CNTs)(denoted PVDF-Trfe/CNTs/BTO).The self-charging supercapacitor power cell device exhibited an energy density of 30μWh cm^(-2)with a high power density of 40 mW cm^(-2)and delivered an excellent self-charging performance of 363 mV(10 N)driven by both the piezoelectric ZnO nanoarrays and the poly(vinylidenefluoride-co-trifluoroethylene)piezoelectric film doped with BaTiO_(3)and carbon nanotubes.More intriguingly,the device could also be self-charged by 184 mV due to residual stress alone and showed excellent energy conversion efficiency and low self-discharge rate.This work illustrates for the first time the self-charging mechanism involving electrolyte ion migration driven by both electrodes and films.A comprehensive analysis strongly confirmed the important contribution of the piezoelectric ZnO nanoarrays in the self-charging process of the self-charging supercapacitor power cell device.This work provides novel directions and insights for the development of selfcharging supercapacitor power cells.
基金supported by the National Natural Science Foundation of China(52174247 and 22302066)“Hejian”Innovative Talent Project of Hunan Province(No.2022RC1088)+1 种基金the Hunan Provincial Natural Science Foundation(2023JJ40255)the Scientific Research Foundation of Hunan Provincial Education(22B0599 and 23A0442)。
文摘Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.
基金supported by National Undergraduate Training Programs for Innovations[grant number 202210225259]the Outstanding Youth Project of Natural Science Foundation in Heilongjiang Province(YQ2022E040)+3 种基金the Shandong Provincial Natural Science Foundation(ZR2022ME166)the Postdoctoral Scientific Research Developmental Fund of Heilongjiang Province(LBH-Q20023)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2020197)the 111 Project(B20088).
文摘Supercapacitors(SCs)are considered promising energy storge systems because of their outstanding power density,fast charge and discharge rate and long-term cycling stability.The exploitation of cheap and efficient electrode materials is the key to improve the performance of supercapacitors.As the battery-type materials,transition metal phosphides(TMPs)possess high theoretical specific capacity,good electrical conductivity and superior structural stability,which have been extensively studied to be electrode materials for supercapacitors.In this review,we summarize the up-to-date progress on TMPs materials from diversified synthetic methods,diverse nanostructures and several prominent TMPs and their composites in application of supercapacitors.In the end,we also propose the remaining challenges toward the rational discovery and synthesis of high-performance TMP electrodes materials for energy storage.
基金supported by the Ensemble Grant for Early Career Researchers 2022 and the 2023 Ensemble Continuation Grant of Tohoku University,the Hirose Foundation,the Iwatani Naoji Foundation,and the AIMR Fusion Research Grantsupported by JSPS KAKENHI Nos.JP23K13599,JP23K13703,JP22H01803,and JP18H05513+2 种基金the Center for Computational Materials Science,Institute for Materials Research,Tohoku University for the use of MASAMUNEIMR(Nos.202212-SCKXX0204 and 202208-SCKXX-0212)the Institute for Solid State Physics(ISSP)at the University of Tokyo for the use of their supercomputersthe China Scholarship Council(CSC)fund to pursue studies in Japan.
文摘All-solid-state batteries(ASSBs)are a class of safer and higher-energy-density materials compared to conventional devices,from which solid-state electrolytes(SSEs)are their essential components.To date,investigations to search for high ion-conducting solid-state electrolytes have attracted broad concern.However,obtaining SSEs with high ionic conductivity is challenging due to the complex structural information and the less-explored structure-performance relationship.To provide a solution to these challenges,developing a database containing typical SSEs from available experimental reports would be a new avenue to understand the structureperformance relationships and find out new design guidelines for reasonable SSEs.Herein,a dynamic experimental database containing>600 materials was developed in a wide range of temperatures(132.40–1261.60 K),including mono-and divalent cations(e.g.,Li^(+),Na^(+),K^(+),Ag^(+),Ca^(2+),Mg^(2+),and Zn^(2+))and various types of anions(e.g.,halide,hydride,sulfide,and oxide).Data-mining was conducted to explore the relationships among different variates(e.g.,transport ion,composition,activation energy,and conductivity).Overall,we expect that this database can provide essential guidelines for the design and development of high-performance SSEs in ASSB applications.This database is dynamically updated,which can be accessed via our open-source online system.
基金This work is supported by National Natural Science Founda-tion of China(U2004199)National Key Research and Devel-opment Program of China(2018YFD0200606)+1 种基金China Postdoctoral Science Foundation(2021T140615),Natural Sci-enceFoundationofHenanProvince(212300410285)Young Talent Support Project of Henan Province(2021HYTP028).
文摘Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer-thin SPE layer-cathode integration(MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore,the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+deposition and excellent cycling stability. High capacity(142.8 mAh g-1), stable operation of 140 cycles(capacity decay per cycle, 0.065%), and low polarization potential(0.5 C) are obtained in this Li|MXene-PEO-LFP cell,which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery.
基金support from the National Science Foundation of China(22078190)the National Key R&D Plan of China(2020YFB1505802).
文摘Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.
基金supported by grants from the National Natural Science Foundation of China(Grant Nos.52072136,52272201,52172229,51972257)Yanchang Petroleum-WHUT Joint Program(yc-whlg-2022ky-05)Fundamental Research Funds for the Central Universities(104972024RSCrc0006)for financial support.
文摘A commentary on pressure-induced pre-lithiation towards Si anodes in allsolid-state Li-ion batteries(ASSLIBs)using sulfide electrolytes(SEs)is presented.First,feasible pre-lithiation technologies for Si anodes in SE-based ASSLIBs especially the significant pressure-induced pre-lithiation strategies are briefly reviewed.Then,a recent achievement by Meng et al.in this field is elaborated in detail.Finally,the significance of Meng’s work is discussed.
基金National Key R&D Program of China (2023YFB2503900)National Natural Science Foundation of China (22222904, 22179133 and 12374176)CAS Project for Young Scientists in Basic Research (YSBR-058)。
文摘The application of Li-rich Mn-based cathodes, the most promising candidates for high-energy-density Liion batteries, in all-solid-state batteries can further enhance the safety and stability of battery systems.However, the utilization of high-capacity Li-rich cathodes has been limited by sluggish kinetics and severe interfacial issues in all-solid-state batteries. Here, a multi-functional interface modification strategy involving dispersed submicron single-crystal structure and multi-functional surface modification layer obtained through in-situ interfacial chemical reactions was designed to improve the electrochemical performance of Li-rich Mn-based cathodes in all-solid-state batteries. The design of submicron single-crystal structure promotes the interface contact between the cathode particles and the solid-state electrolyte,and thus constructs a more complete ion and electron conductive network in the composite cathode.Furthermore, the Li-gradient layer and the lithium molybdate coating layer constructed on the surface of single-crystal Li-rich particles accelerate the transport of Li ions at the interface, suppress the side reactions between cathodes and electrolyte, and inhibit the oxygen release on the cathode surface. The optimized Li-rich cathode materials exhibit excellent electrochemical performance in halide all-solid-state batteries. This study emphasizes the vital importance of reaction kinetics and interfacial stability of Lirich cathodes in all-solid-state batteries and provides a facile modification strategy to enhance the electrochemical performance of all-solid-state batteries based on Li-rich cathodes.
基金supported by National Science Foundation of China(No.52201254)Natural Science Foundation of Shandong Province(Nos.ZR2020MB090,ZR2020MB027,and ZR2020QE012)+1 种基金the project of“20 Items of University”of Jinan(No.202228046)the Taishan Scholar Project of Shandong Province(No.tsqn202306226)。
文摘The stacking and aggregation of graphene nanosheets have been obstacles to their application as electrode materials for microelectronic devices.This study deploys a one-step,scalable,facile electrochemical exfoliation technique to fabricate nitrogen(N)and chlorine(Cl)co-doped graphene nanosheets(i.e.,N-Cl-G)via the application of constant voltage on graphite in a mixture of 0.1 mol/L H_(2)SO_(4)and 0.1 mol/L NH_(4)Cl without using dangerous and exhaustive operation.The introduction of Cl(with its large radius)and N,both with high electrical negativity,facilitates the modulation of the electronic structure of graphene and creation of rich structural defects in it.Consequently,in the as-constructed supercapacitors,N-Cl-G exhibits a high specific capacitance of 77 F/g at 0.2 A/g and remarkable cycling stability with 91.7%retention of initial capacitance after 20,000 cycles at 10 A/g.Furthermore,a symmetrical supercapacitor assembled with N-Cl-G as the positive and negative electrodes(denoted as N-Cl-G//N-Cl-G)exhibits an energy density of 3.38 Wh/kg at a power density of 600 W/kg and superior cycling stability with almost no capacitance loss after 5000 cycles at 5 A/g.This study provides a scalable protocol for the facile fabrication of high-performance co-doped graphene as an electrode material candidate for supercapacitors.
基金financially supported by the Shenzhen Science and Technology Program (Grant No.KQTD20200820113045083,ZDSYS20190902093220279,and JCYJ20220818102403007)the National Natural Science Foundation of China (52201257)the Shenzhen Research Fund for Returned Scholars (DD11409017).
文摘Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety.Nonetheless,inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial application.Herein,we report a liquid metal-coated lithium metal(LM@Li)anode strategy to improve the contact between lithium metal and a Li6PS5Cl inorganic electrolyte.The LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2mA cm^(-2) and a significantly higher critical current density of 9.8 mAcm^(-2) at 25°C.In addition,a full battery assembled with a high-capacity composite LiNbO3@-LiNi_(0.7)Co_(0.2)Mn_(0.1)O_(2)(LNO@NCM721)cathode shows stable cycling performance.Experimental and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.
基金National Natural Science Foundation of China (Grant Nos. 22178125 and 21875071)。
文摘All-solid-state lithium-sulfur batteries(ASSLSBs) have become one of the most potential candidates for the next-generation high-energy systems due to their intrinsic safety and high theoretical energy density.However, PEO-based ASSLSBs face the dilemma of insufficient Coulombic efficiency and long-term stability caused by the coupling problems of dendrite growth of anode and polysulfide shuttle of cathode. In this work, 1,3,5-trioxane(TOX) is used as a functional additive to design a PEO-based composite solidstate electrolyte(denoted as TOX-CSE), which realizes the stable long-term cycle of an ASSLSB. The results show that TOX can in-situ decompose on the anode to form a composite solid electrolyte interphase(SEI) layer with rich-organic component. It yields a high average modulus of 5.0 GPa, greatly improving the mechanical stability of the SEI layer and thus inhibiting the growth of dendrites. Also,the robust SEI layer can act as a barrier to block the side reaction between polysulfides and lithium metal.As a result, a Li-Li symmetric cell assembled with a TOX-CSE exhibits prolonged cycling stability over 2000 h at 0.2 m A cm^(-2). The ASSLSB also shows a stable cycling performance of 500 cycles at 0.5 C.This work reveals the structure–activity relationship between the mechanical property of interface layer and the battery's cycling stability.
基金support by the National Natural Science Foundation of China(grant no.51772206).
文摘Solid polymer electrolytes(SPEs)are highly promising for realizing high-capacity,low-cost,and safe Li metal batteries.However,the Li dendritic growth and side reactions between Li and SPEs also plague these systems.Herein,a fluorinated lithium salt coating(FC)with organic-inorganic gradient and soft–rigid feature is introduced on Li surface as an artificial protective layer by the in-situ reaction between Li metal and fluorinated carboxylic acid.The FC layer can improve the interface stability and wettability between Li and SPEs,assist the transport of Li ions,and guide Li nucleation,contributing to a dendrite-free Li deposition and long-lifespan Li metal batteries.The symmetric cell with FC-Li anodes exhibits a high areal capacity of 1 mAh cm^(-2)at 0.5 mA cm^(-2),and an ultra-long lifespan of 2000 h at a current density of 0.1 mA cm^(-2).Moreover,the full cell paired with the LiFePO4 cathode exhibits improved cycling stability,remaining 83.7%capacity after 500 cycles at 1 C.When matching with the S cathode,the FC layer can prevent the shuttle effect,contributing to stable and high-capacity Li–S battery.This work provided a promising way for the construction of stable all-solid-state lithium metal batteries with prolonged lifespan.