Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials ...Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and sustainability.Despite the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing costs.This review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes(SSEs),as well as state-of-the-art progress in various promising cathodes(e.g.,FeS_(2),CuS,FeF_(3),FeF_(2),and S)in SSLBs.Furthermore,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical application.Significantly,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type cathodes.Finally,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.展开更多
Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated us...Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated using the conventional slurry casting approach frequently exhibit an exacerbated accumulation of carbon additives and binders on their surfaces,invariably leading to compromised electrochemical properties.In this study,we introduce a designed conductive agent/binder composite synthesized from carbon nanotube and polytetrafluoroethylene.This agent/binder composite facilitates production of dry-process-prepared ultra-thick electrodes endowed with a three-dimensional and uniformly distributed percolative architecture,ensuring superior electronic conductivity and remarkable mechanical resilience.Using this approach,ultra-thick LiCoO_(2)(LCO) electrodes demonstrated superior cycling performance and rate capabilities,registering an impressive loading capacity of up to 101.4 mg/cm^(2),signifying a 242% increase in battery energy density.In another analytical endeavor,time-of-flight secondary ion mass spectroscopy was used to clarify the distribution of cathode electrolyte interphase(CEI) in cycled LCO electrodes.The results provide unprecedented evidence explaining the intricate correlation between CEI generation and carbon distribution,highlighting the intrinsic advantages of the proposed dry-process approach in fine-tu ning the CEI,with excellent cycling performance in batteries equipped with ultra-thick electrodes.展开更多
The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly co...The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.展开更多
Na_(3)V_(2)(PO_(4))_(3)(NVP)is gifted with fast Na^(+)conductive NASICON structure.But it still suffers from low electronic conductivity and inadequate energy density.Herein,a high-entropy modification strategy is rea...Na_(3)V_(2)(PO_(4))_(3)(NVP)is gifted with fast Na^(+)conductive NASICON structure.But it still suffers from low electronic conductivity and inadequate energy density.Herein,a high-entropy modification strategy is realized by doping V^(3+)site with Ga^(3+)/Cr^(3+)/Al^(3+)/Fe^(3+)/In^(3+)simultaneously(i.e.Na_(3)V_(2-x)(GaCrAlFeIn)_x(PO_(4))_(3);x=0,0.04,0.06,and 0.08)to stimulate the V^(5+)■V^(2+)reversible multi-electron redox.Such configuration high-entropy can effectively suppress the structural collapse,enhance the redox reversibility in high working voltage(4.0 V),and optimize the electronic induced effect.The in-situ X-ray powder diffraction and in-situ electrochemical impedance spectroscopy tests efficaciously confirm the robust structu ral recovery and far lower polarization throughout an entire charge-discharge cycle during 1.6-4.3 V,respectively.Moreover,the density functional theory calculations clarify the stronger metallicity of high-entropy electrode than the bare that is derived from the more mobile free electrons surrounding the vicinity of Fermi level.By grace of high-entropy design and multi-electron transfer reactions,the optimal Na_(3)V_(1.7)(GaCrAlFeIn)_(0.06)(PO_(4))_(3)can exhibit perfect cycling/rate performances(90.97%@5000 cycles@30 C;112 mA h g^(-1)@10 C and 109 mA h g^(-1)@30 C,2.0-4.3 V).Furthermore,it can supply ultra-high185 mA h g^(-1)capacity with fa ntastic energy density(522 W h kg^(-1))in half-cells(1.4-4.3 V),and competitive capacity(121 mA h g^(-1))as well as energy density(402 W h kg^(-1))in full-cells(1.6-4.1 V),demonstrating enormous application potential for sodium-ion batteries.展开更多
A novel bismuth–carbon composite, in which bismuth nanoparticles were anchored in a nitrogen-doped carbon matrix(Bi@NC), is proposed as anode for high volumetric energy density lithium ion batteries(LIBs).Bi@NC compo...A novel bismuth–carbon composite, in which bismuth nanoparticles were anchored in a nitrogen-doped carbon matrix(Bi@NC), is proposed as anode for high volumetric energy density lithium ion batteries(LIBs).Bi@NC composite was synthesized via carbonization of Zn-containing zeolitic imidazolate(ZIF-8) and replacement of Zn with Bi, resulting in the N-doped carbon that was hierarchically porous and anchored with Bi nanoparticles. The matrix provides a highly electronic conductive network that facilitates the lithiation/delithiation of Bi.Additionally, it restrains aggregation of Bi nanoparticles and serves as a buffer layer to alleviate the mechanical strain of Bi nanoparticles upon Li insertion/extraction.With these contributions, Bi@NC exhibits excellent cycling stability and rate capacity compared to bare Bi nanoparticles or their simple composites with carbon. This study provides a new approach for fabricating high volumetric energy density LIBs.展开更多
Electrode material based on a novel core–shell structure consisting of NiCoS（NCS） solid fiber core and Mn S（MS） sheet shell（NCS@MS） in situ grown on carbon cloth（CC） has been successfully prepared by a simple...Electrode material based on a novel core–shell structure consisting of NiCoS（NCS） solid fiber core and Mn S（MS） sheet shell（NCS@MS） in situ grown on carbon cloth（CC） has been successfully prepared by a simple sulfurization-assisted hydrothermal method for high performance supercapacitor. The synthesized NiCoS@Mn S/CC electrode shows high capacitance of 1908.3 F gat a current density of 0.5 A gwhich is higher than those of NiCoSand Mn S at the same current density. A flexible all-solid-state asymmetric supercapacitor（ASC） is constructed by using NiCoS@Mn S/CC as positive electrode, active carbon/CC as negative electrode and KOH/poly（vinyl alcohol）(PVA) as electrolyte. The optimized ASC shows a maximum energy density of 23.3 Wh kgat 1 A g, a maximum power density of about7.5 kw kgat 10 A gand remarkable cycling stability. After 9000 cycles, the ASC still exhibited67.8% retention rate and largely unchanged charge/discharge curves. The excellent electrochemical properties are resulted from the novel core–shell structure of the NiCoS@Mn S/CC electrode, which possesses both high surface area for Faraday redox reaction and superior kinetics of charge transport. The NiCoS@Mn S/CC electrode shows a promising potential for energy storage applications in the future.展开更多
Ultrafast imaging tools are of great importance for determining the dynamic density distribution in high energy density(HED)matter.In this work,we designed a high energy electron radiography(HEER)system based on a lin...Ultrafast imaging tools are of great importance for determining the dynamic density distribution in high energy density(HED)matter.In this work,we designed a high energy electron radiography(HEER)system based on a linear electron accelerator to evaluate its capability for imaging HED matter.40 MeV electron beams were used to image an aluminum target to study the density resolution and spatial resolution of HEER.The results demonstrate a spatial resolution of tens of micrometers.The interaction of the beams with the target and the beam transport of the transmitted electrons are further simulated with EGS5 and PARMELA codes,with the results showing good agreement with the experimental resolution.Furthermore,the experiment can be improved by adding an aperture at the Fourier plane.展开更多
Hydrogen storage and delivery technology is still a bottleneck in the hydrogen industry chain.Among all kinds of hydrogen storage methods,light-weight solid-state hydrogen storage(LSHS)materials could become promising...Hydrogen storage and delivery technology is still a bottleneck in the hydrogen industry chain.Among all kinds of hydrogen storage methods,light-weight solid-state hydrogen storage(LSHS)materials could become promising due to its intrinsic high hydrogen capacity.Hydrolysis reaction of LSHS materials occurs at moderate conditions,indicating the potential for portable applications.At present,most of review work focuses on the improvement of material performance,especially the catalysts design.This part is important,but the others,such as operation modes,are also vital to to make full use of material potential in the practical applications.Different operation modes of hydrolysis reaction have an impact on hydrogen capacity to various degrees.For example,hydrolysis in solution would decrease the hydrogen capacity of hydrogen generator to a low value due to the excessive water participating in the reaction.Therefore,application-oriented operation modes could become a key problem for hydrolysis reaction of LSHS materials.In this paper,the operation modes of hydrolysis reaction and their practical applications are mainly reviewed.The implements of each operation mode are discussed and compared in detail to determine the suitable one for practical applications with the requirement of high energy density.The current challenges and future directions are also discussed.展开更多
Electronic textiles hold the merits of high conformability with the human body and natural surrounding,possessing large market demand and wide application foreground in smart wearable and portable devices.However,thei...Electronic textiles hold the merits of high conformability with the human body and natural surrounding,possessing large market demand and wide application foreground in smart wearable and portable devices.However,their further application is largely hindered by the shortage of flexible and stable power sources with multifunctional designability.Herein,a free-standing ZnHCF@CF electrode(ZnHCF grown on carbon nanotube fiber)with good mechanical deformability and high electrochemical performance for aqueous fiber-shaped calcium ion battery(FCIB)is reported.Benefiting from the unique Ca^(2+)/H^(+)co-insertion mechanism,the ZnHCF@CF cathode can exhibit great ion storage capability within a broadened voltage window.By pairing with a polyaniline(PANI)@CF anode,a ZnHCF@CF//PANI@CF FCIB is successfully fabricated,which exhibits a desirable volumetric energy density of 43.2mWh cm^(-3)and maintains superior electrochemical properties under different deformations.Moreover,the high-energy FCIB can be harmoniously integrated with a fiber-shaped strain sensor(FSS)to achieve real-time physiological monitoring on knees during long-running,exhibiting great promise for the practical application of electronic textiles.展开更多
Rechargeable lithium batteries with high-capacity cathodes/anodes promise high energy densities for nextgeneration electrochemical energy storage.However,the associated limitations at various scales greatly hinder the...Rechargeable lithium batteries with high-capacity cathodes/anodes promise high energy densities for nextgeneration electrochemical energy storage.However,the associated limitations at various scales greatly hinder their practical applications.Functional gradient material(FGM)design endows the electrode materials with property gradient,thus providing great opportunities to address the kinetics and stability obstacles.To date,still no review or perspective has covered recent advancements in gradient design at multiple scales for boosting lithium battery performances.To fill this void,this work provides a timely and comprehensive overview of this exciting and sustainable research field.We begin by overviewing the fundamental features of FGM and the rationales of gradient design for improved electrochemical performance.Then,we comprehensively review FGM design for rechargeable lithium batteries at various scales,including natural or artificial solid electrolyte interphase(SEI)at the nanoscale,micrometer-scale electrode particles,and macroscale electrode films.The link between gradient structure design and improved electrochemical performance is particularly highlighted.The most recent research into constructing novel functional gradients,such as valence and temperature gradients,has also been explored.Finally,we discussed the current constraints and future scope of FGM in rechargeable lithium batteries,aiming to inspire the development of novel FGM for next-generation high-performance lithium batteries.展开更多
Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3...Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3 D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti_3 C_2 T_x flakes on sulfur-impregnated carbon cloth(Ti_3 C_2 T_x@S/CC) to achieve high loading and high energy density Li-S batteries,in which,the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer,while the outer-coated Ti_3 C_2 T_x can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode,achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion.Due to these advantages,at a sulfur loading of 4 mg cm^(-2),Li-S cells with Ti_3 C_2 T_x@S/CC cathodes can deliver outstanding cycling stability(746.1 mAh g^(-1) after 200 cycles at1 C),superb rate performance(866.8 mAh g^(-1) up to 2 C) and a high specific energy density(564.2 Wh kg^(-1) after 100 cycles at 0.5 C).More significantly,they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm^(-2) at the increased loading of 8 mg cm^(-2).展开更多
Fluorinated carbons(CFx)have been widely applied as lithium primary batteries due to their ultra-high energy density.It will be a great promise if CFx can be rechargeable.In this study,we rationally tune the C-F bond ...Fluorinated carbons(CFx)have been widely applied as lithium primary batteries due to their ultra-high energy density.It will be a great promise if CFx can be rechargeable.In this study,we rationally tune the C-F bond strength for the alkaline intercalated CFx via importing an electronegative weaker element K instead of Li.It forms a ternary phase K_(x)FC instead of two phases(LiF+C)in lithium-ion batteries.Meanwhile,we choose a large layer distance and more defects CFx,namely fluorinated soft carbon,to accommodate K.Thus,we enable CFx rechargeable as a potassium-ion battery cathode.In detail fluorinated soft carbon CF_(1.01) presents a reversible specific capacity of 339 mA h g^(-1)(797 Wh kg^(-1))in the 2nd cycle and maintains 330 mA h g^(-1)(726 Wh kg^(-1))in the 15th cycle.This study reveals the importance of tuning chemical bond stability using different alkaline ions to endow batteries with rechargeability.This work provides good references for focusing on developing reversible electrode materials from popular primary cell configurations.展开更多
Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulo...Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulombic efficiency(ICE),large interfacial resistance,and severe embrittlement,as the large specific surface area often results in severe interfacial decomposition of the electrolyte and the formation of thick and fluffy solid electrolyte interphase(SEI)during cycling of LIBs.Herein,we demonstrate that when the CNT-based current collector and Na foil(which are being stacked intimately upon each other)are being placed in Na+-based organic electrolyte,local redox reaction between the Na foil and the electrolyte would occur spontaneously,generating a thin and homogeneous NaF-based passivating layer on the CNTs.More importantly,we found that owing to the weak solvation behaviors of Na+in the organic electrolyte,the resulting passivation layer,which is rich in NaF,is thin and dense;when used as the anode current collector in LIBs,the pre-existing passivating layer can function effectively in isolating the anode from the solvated Li+,thus suppressing the formation of bulky SEI and the destructive intercalation of solvated Li+.The relevant half-cell(graphite as anode)exhibits a high ICE of 92.1%;the relevant pouch cell with thus passivated CNT film as current collectors for both electrodes(LiCoO_(2)as cathode,graphite as anode)displays a high energy density of 255 Wh kg^(-1),spelling an increase of 50%compared with that using the conventional metal current collectors.展开更多
The mass fraction of electrolytes is the crucial factor affecting the energy density of lithium-sulfur(Li-S)batteries. Due to the high porosity within the C/S cathode, high concentration of polysulfides, and side reac...The mass fraction of electrolytes is the crucial factor affecting the energy density of lithium-sulfur(Li-S)batteries. Due to the high porosity within the C/S cathode, high concentration of polysulfides, and side reaction in lithiun metal anode under lean electrolyte, it is extremely challenging to improve performance while reducing the electrolyte volume. Here, we report a novel electrolyte with relatively low density(1.16 g cm^(-2)), low viscosity(1.84 m Pa s), and high ionic conductivity, which significantly promotes energy density and cyclability of Li-S batteries under practical conditions. Moreover, such electrolyte enables a hybrid cathode electrolyte interphase(CEI) and solid electrolyte interface(SEI) layer with plentiful Li F, which leads to fast kinetics of ions transport and stable cyclability even under low temperatures.Compared to Li-S batteries in electrolyte employing 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether(TTE) diluent, the ultra-thick cathode(20 mg cm^(-2)) shows a high capacity of 9.48 m Ah cm^(-2)and excellent capacity retention of 80.3% over 191 cycles at a low electrolyte-to-sulfur ratio(E/S = 2) and negative-to-positive capacity ratio(N/P = 2.5), realizing a 19.2% improvement in energy density in coin cells(from 370 to 441 Wh kg^(-1)) and a high energy density up to 467 Wh kg^(-1) in pouch cells. This study not only provides guidance for the electrolyte design but also paves the way for the development of high performance Li-S batteries under practical conditions.展开更多
By using a two-dimensional particle-in-cell simulation,we demonstrate a scheme for highenergy-density electron beam generation by irradiating an ultra intense laser pulse onto an aluminum（Al） target.With the laser h...By using a two-dimensional particle-in-cell simulation,we demonstrate a scheme for highenergy-density electron beam generation by irradiating an ultra intense laser pulse onto an aluminum（Al） target.With the laser having a peak intensity of 4×10^23W cm^-2,a high quality electron beam with a maximum density of 117 nc and a kinetic energy density up to8.79×10^18J m^-3 is generated.The temperature of the electron beam can be 416 Me V,and the beam divergence is only 7.25°.As the laser peak intensity increases（e.g.,1024 W cm^-2）,both the beam energy density（3.56×10^19J m^-3） and the temperature（545 Me V） are increased,and the beam collimation is well controlled.The maximum density of the electron beam can even reach 180 nc.Such beams should have potential applications in the areas of antiparticle generation,laboratory astrophysics,etc.展开更多
Molecular crystals are complex systems exhibiting various crystal structures,and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure.Here,we perform a...Molecular crystals are complex systems exhibiting various crystal structures,and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure.Here,we perform an extensive structure search of ternary carbon-nitrogen-oxygen(CNO)compound under high pressure with the CALYPSO method and first principles calculations,and successfully identify three polymeric CNO compounds with Pbam,C2/m and I4m2symmetries under 100 GPa.More interestingly,these structures are also dynamically stable at ambient pressure,and are potential high energy density materials(HEDMs).The energy densities of Pbam,C2/m and I4m2 phases of CNO are about2.30 kJ/g,1.37 kJ/g and 2.70 kJ/g,respectively,with the decompositions of graphitic carbon and molecular carbon dioxide andα-N(molecular N_(2))at ambient pressure.The present results provide in-depth insights into the structural evolution and physical properties of CNO compounds under high pressures,which offer crucial insights for designs and syntheses of novel HEDMs.展开更多
The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batterie...The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^(-2) delivers a stable area capacity of 6.6 mAh cm^(-2) over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^(-2) over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.展开更多
Rechargeable batteries of high energy density and overall performance are becoming a critically important technology in the rapidly changing society of the twenty-first century.While lithium-ion batteries have so far ...Rechargeable batteries of high energy density and overall performance are becoming a critically important technology in the rapidly changing society of the twenty-first century.While lithium-ion batteries have so far been the dominant choice,numerous emerging applications call for higher capacity,better safety and lower costs while maintaining sufficient cyclability.The design space for potentially better alternatives is extremely large,with numerous new chemistries and architectures being simultaneously explored.These include other insertion ions(e.g.sodium and numerous multivalent ions),conversion electrode materials(e.g.silicon,metallic anodes,halides and chalcogens)and aqueous and solid electrolytes.However,each of these potential“beyond lithium-ion”alternatives faces numerous challenges that often lead to very poor cyclability,especially at the commercial cell level,while lithium-ion batteries continue to improve in performance and decrease in cost.This review examines fundamental principles to rationalise these numerous developments,and in each case,a brief overview is given on the advantages,advances,remaining challenges preventing cell-level implementation and the state-of-the-art of the solutions to these challenges.Finally,research and development results obtained in academia are compared to emerging commercial examples,as a commentary on the current and near-future viability of these“beyond lithium-ion”alternatives.展开更多
Flexible supercapacitor electrodes with high mass loading are crucial for obtaining favorable electrochemical performance but still challenging due to sluggish electron and ion transport.Herein,rationally designed CNT...Flexible supercapacitor electrodes with high mass loading are crucial for obtaining favorable electrochemical performance but still challenging due to sluggish electron and ion transport.Herein,rationally designed CNT/MnO2/graphene-grafted carbon cloth electrodes are prepared by a“graft-deposit-coat”strategy.Due to the large surface area and good conductivity,graphene grafted on carbon cloth offers additional surface areas for the uniform deposition of MnO2(9.1 mg cm?2)and facilitates charge transfer.Meanwhile,the nanostructured MnO2 provides abundant electroactive sites and short ion transport distance,and CNT coated on MnO2 acts as interconnected conductive“highways”to accelerate the electron transport,significantly improving redox reaction kinetics.Benefiting from high mass loading of electroactive materials,favorable conductivity,and a porous structure,the electrode achieves large areal capacitances without compromising rate capability.The assembled asymmetric supercapacitor demonstrates a wide working voltage(2.2 V)and high energy density of 10.18 mWh cm?3.展开更多
Development of cost-effective and environmental friendly energy storage devices(ESDs) has attracted widespread attention in recent scenario of energy research.Recently,the environmentally viable "water-in-salt&qu...Development of cost-effective and environmental friendly energy storage devices(ESDs) has attracted widespread attention in recent scenario of energy research.Recently,the environmentally viable "water-in-salt"(WiS) electrolytes has received significant interest for the development of advanced high performance ESDs.The WiS electrolyte exhibits wide electrochemical stability window(ESW),highsafety,non-flammability and superior electrochemical performance compared to the conventional "salt-in-water" electrolytes.This review aims to provide a comprehensive discussion on WiS electrolyte based on theoretical,electrochemical and physicochemical characteristics.A strategic way for the usage of WiS electrolyte in rechargeable metal-ion batteries and supercapacitors with potentially improved electrochemical performance has been reviewed systematically.This review also discussed the unique advantages of WiS electrolytes as well as the future scope and challenges.展开更多
基金National Natural Science Foundation of China(22322903,52072061)Natural Science Foundation of Sichuan,China(2023NSFSC1914)Beijing National Laboratory for Condensed Matter Physics(2023BNLCMPKF015)。
文摘Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and sustainability.Despite the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing costs.This review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes(SSEs),as well as state-of-the-art progress in various promising cathodes(e.g.,FeS_(2),CuS,FeF_(3),FeF_(2),and S)in SSLBs.Furthermore,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical application.Significantly,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type cathodes.Finally,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.
基金supported by the National Key Research and Development Program of China,China(2019YFA0705102)the National Natural Science Foundation of China,China(22179144,22005332)。
文摘Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated using the conventional slurry casting approach frequently exhibit an exacerbated accumulation of carbon additives and binders on their surfaces,invariably leading to compromised electrochemical properties.In this study,we introduce a designed conductive agent/binder composite synthesized from carbon nanotube and polytetrafluoroethylene.This agent/binder composite facilitates production of dry-process-prepared ultra-thick electrodes endowed with a three-dimensional and uniformly distributed percolative architecture,ensuring superior electronic conductivity and remarkable mechanical resilience.Using this approach,ultra-thick LiCoO_(2)(LCO) electrodes demonstrated superior cycling performance and rate capabilities,registering an impressive loading capacity of up to 101.4 mg/cm^(2),signifying a 242% increase in battery energy density.In another analytical endeavor,time-of-flight secondary ion mass spectroscopy was used to clarify the distribution of cathode electrolyte interphase(CEI) in cycled LCO electrodes.The results provide unprecedented evidence explaining the intricate correlation between CEI generation and carbon distribution,highlighting the intrinsic advantages of the proposed dry-process approach in fine-tu ning the CEI,with excellent cycling performance in batteries equipped with ultra-thick electrodes.
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.52373047,No.52302106)the Sichuan Youth Science and Technology Innovation Research Team Project(No.2022JDTD0012)+2 种基金the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(No.2020SCUNG203)the Natural Science Foundation of Sichuan Province(No.2023NSFSC0418)the Program for State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-3-10)。
文摘The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.
基金financially supported by the National Key Research and Development Program of China (2022YFA1505700,2019YFA0210403)the National Natural Science Foundation of China (52102216)+1 种基金the Natural Science Foundation of Fujian Province (2022J01625,2022-S-002)the Innovation Training Program for College Students (202310394020,cxxl-2023097,cxxl-2024131,cxxl-2024136)。
文摘Na_(3)V_(2)(PO_(4))_(3)(NVP)is gifted with fast Na^(+)conductive NASICON structure.But it still suffers from low electronic conductivity and inadequate energy density.Herein,a high-entropy modification strategy is realized by doping V^(3+)site with Ga^(3+)/Cr^(3+)/Al^(3+)/Fe^(3+)/In^(3+)simultaneously(i.e.Na_(3)V_(2-x)(GaCrAlFeIn)_x(PO_(4))_(3);x=0,0.04,0.06,and 0.08)to stimulate the V^(5+)■V^(2+)reversible multi-electron redox.Such configuration high-entropy can effectively suppress the structural collapse,enhance the redox reversibility in high working voltage(4.0 V),and optimize the electronic induced effect.The in-situ X-ray powder diffraction and in-situ electrochemical impedance spectroscopy tests efficaciously confirm the robust structu ral recovery and far lower polarization throughout an entire charge-discharge cycle during 1.6-4.3 V,respectively.Moreover,the density functional theory calculations clarify the stronger metallicity of high-entropy electrode than the bare that is derived from the more mobile free electrons surrounding the vicinity of Fermi level.By grace of high-entropy design and multi-electron transfer reactions,the optimal Na_(3)V_(1.7)(GaCrAlFeIn)_(0.06)(PO_(4))_(3)can exhibit perfect cycling/rate performances(90.97%@5000 cycles@30 C;112 mA h g^(-1)@10 C and 109 mA h g^(-1)@30 C,2.0-4.3 V).Furthermore,it can supply ultra-high185 mA h g^(-1)capacity with fa ntastic energy density(522 W h kg^(-1))in half-cells(1.4-4.3 V),and competitive capacity(121 mA h g^(-1))as well as energy density(402 W h kg^(-1))in full-cells(1.6-4.1 V),demonstrating enormous application potential for sodium-ion batteries.
基金supported by the Natural Science Foundation of Guangdong Province (Grant No.2017B030306013)the key project of Science and Technology in Guangdong Province (Grant No.2017A010106006)
文摘A novel bismuth–carbon composite, in which bismuth nanoparticles were anchored in a nitrogen-doped carbon matrix(Bi@NC), is proposed as anode for high volumetric energy density lithium ion batteries(LIBs).Bi@NC composite was synthesized via carbonization of Zn-containing zeolitic imidazolate(ZIF-8) and replacement of Zn with Bi, resulting in the N-doped carbon that was hierarchically porous and anchored with Bi nanoparticles. The matrix provides a highly electronic conductive network that facilitates the lithiation/delithiation of Bi.Additionally, it restrains aggregation of Bi nanoparticles and serves as a buffer layer to alleviate the mechanical strain of Bi nanoparticles upon Li insertion/extraction.With these contributions, Bi@NC exhibits excellent cycling stability and rate capacity compared to bare Bi nanoparticles or their simple composites with carbon. This study provides a new approach for fabricating high volumetric energy density LIBs.
基金supported by the Grant-in-Aid for Scientific Research (KAKENHI) program, Japan (C, Grant Number 15K05597)Takahashi Industrial and Economic Research Foundation (Takahashi Grant Number 06-003-154)
文摘Electrode material based on a novel core–shell structure consisting of NiCoS（NCS） solid fiber core and Mn S（MS） sheet shell（NCS@MS） in situ grown on carbon cloth（CC） has been successfully prepared by a simple sulfurization-assisted hydrothermal method for high performance supercapacitor. The synthesized NiCoS@Mn S/CC electrode shows high capacitance of 1908.3 F gat a current density of 0.5 A gwhich is higher than those of NiCoSand Mn S at the same current density. A flexible all-solid-state asymmetric supercapacitor（ASC） is constructed by using NiCoS@Mn S/CC as positive electrode, active carbon/CC as negative electrode and KOH/poly（vinyl alcohol）(PVA) as electrolyte. The optimized ASC shows a maximum energy density of 23.3 Wh kgat 1 A g, a maximum power density of about7.5 kw kgat 10 A gand remarkable cycling stability. After 9000 cycles, the ASC still exhibited67.8% retention rate and largely unchanged charge/discharge curves. The excellent electrochemical properties are resulted from the novel core–shell structure of the NiCoS@Mn S/CC electrode, which possesses both high surface area for Faraday redox reaction and superior kinetics of charge transport. The NiCoS@Mn S/CC electrode shows a promising potential for energy storage applications in the future.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11435015 and 11505251)the Ministry of Science and Technology of China(Grant No.2016YFE0104900)the Chinese Academy of Sciences(Grant Nos.28Y740010 and 113462KYSB20160036)
文摘Ultrafast imaging tools are of great importance for determining the dynamic density distribution in high energy density(HED)matter.In this work,we designed a high energy electron radiography(HEER)system based on a linear electron accelerator to evaluate its capability for imaging HED matter.40 MeV electron beams were used to image an aluminum target to study the density resolution and spatial resolution of HEER.The results demonstrate a spatial resolution of tens of micrometers.The interaction of the beams with the target and the beam transport of the transmitted electrons are further simulated with EGS5 and PARMELA codes,with the results showing good agreement with the experimental resolution.Furthermore,the experiment can be improved by adding an aperture at the Fourier plane.
基金financially supported by the National Key R&D Program of China(2022YFE0101300)the National Natural Science Foundation of China(52176203 and 52050027)the China Education Association for International Exchange(202006)。
文摘Hydrogen storage and delivery technology is still a bottleneck in the hydrogen industry chain.Among all kinds of hydrogen storage methods,light-weight solid-state hydrogen storage(LSHS)materials could become promising due to its intrinsic high hydrogen capacity.Hydrolysis reaction of LSHS materials occurs at moderate conditions,indicating the potential for portable applications.At present,most of review work focuses on the improvement of material performance,especially the catalysts design.This part is important,but the others,such as operation modes,are also vital to to make full use of material potential in the practical applications.Different operation modes of hydrolysis reaction have an impact on hydrogen capacity to various degrees.For example,hydrolysis in solution would decrease the hydrogen capacity of hydrogen generator to a low value due to the excessive water participating in the reaction.Therefore,application-oriented operation modes could become a key problem for hydrolysis reaction of LSHS materials.In this paper,the operation modes of hydrolysis reaction and their practical applications are mainly reviewed.The implements of each operation mode are discussed and compared in detail to determine the suitable one for practical applications with the requirement of high energy density.The current challenges and future directions are also discussed.
基金partially supported by the Natural Science Foundation of Liaoning Province(2023-MS-115)the Large Instrument and Equipment Open Foundation of Dalian University of Technology+1 种基金the National Natural Science Foundation of China(22308261)funding from the Fundamental Research Funds for the Central Universities,conducted at Tongji University。
文摘Electronic textiles hold the merits of high conformability with the human body and natural surrounding,possessing large market demand and wide application foreground in smart wearable and portable devices.However,their further application is largely hindered by the shortage of flexible and stable power sources with multifunctional designability.Herein,a free-standing ZnHCF@CF electrode(ZnHCF grown on carbon nanotube fiber)with good mechanical deformability and high electrochemical performance for aqueous fiber-shaped calcium ion battery(FCIB)is reported.Benefiting from the unique Ca^(2+)/H^(+)co-insertion mechanism,the ZnHCF@CF cathode can exhibit great ion storage capability within a broadened voltage window.By pairing with a polyaniline(PANI)@CF anode,a ZnHCF@CF//PANI@CF FCIB is successfully fabricated,which exhibits a desirable volumetric energy density of 43.2mWh cm^(-3)and maintains superior electrochemical properties under different deformations.Moreover,the high-energy FCIB can be harmoniously integrated with a fiber-shaped strain sensor(FSS)to achieve real-time physiological monitoring on knees during long-running,exhibiting great promise for the practical application of electronic textiles.
基金financial support from the National Natural Science Foundation of China(Nos.52261160384 and 52072208)the Project of Department of Education of Guangdong Province(No.2022ZDZX3018)+2 种基金the Natural Science Foundation of Guangdong(No.2023A1515010020)the Innovation and Technology Fund(No.ITS-325-22FP)the Shenzhen Science and Technology Program(No.KJZD20230923114107014)。
文摘Rechargeable lithium batteries with high-capacity cathodes/anodes promise high energy densities for nextgeneration electrochemical energy storage.However,the associated limitations at various scales greatly hinder their practical applications.Functional gradient material(FGM)design endows the electrode materials with property gradient,thus providing great opportunities to address the kinetics and stability obstacles.To date,still no review or perspective has covered recent advancements in gradient design at multiple scales for boosting lithium battery performances.To fill this void,this work provides a timely and comprehensive overview of this exciting and sustainable research field.We begin by overviewing the fundamental features of FGM and the rationales of gradient design for improved electrochemical performance.Then,we comprehensively review FGM design for rechargeable lithium batteries at various scales,including natural or artificial solid electrolyte interphase(SEI)at the nanoscale,micrometer-scale electrode particles,and macroscale electrode films.The link between gradient structure design and improved electrochemical performance is particularly highlighted.The most recent research into constructing novel functional gradients,such as valence and temperature gradients,has also been explored.Finally,we discussed the current constraints and future scope of FGM in rechargeable lithium batteries,aiming to inspire the development of novel FGM for next-generation high-performance lithium batteries.
基金supported by the National Natural Science Foundation of China (51772069)。
文摘Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3 D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti_3 C_2 T_x flakes on sulfur-impregnated carbon cloth(Ti_3 C_2 T_x@S/CC) to achieve high loading and high energy density Li-S batteries,in which,the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer,while the outer-coated Ti_3 C_2 T_x can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode,achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion.Due to these advantages,at a sulfur loading of 4 mg cm^(-2),Li-S cells with Ti_3 C_2 T_x@S/CC cathodes can deliver outstanding cycling stability(746.1 mAh g^(-1) after 200 cycles at1 C),superb rate performance(866.8 mAh g^(-1) up to 2 C) and a high specific energy density(564.2 Wh kg^(-1) after 100 cycles at 0.5 C).More significantly,they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm^(-2) at the increased loading of 8 mg cm^(-2).
基金supported by the National Natural Science Foundation of China(52072061)21C Innovation Laboratory,Contemporary Amperex Technology Ltd.by project No.21C–OP–202103。
文摘Fluorinated carbons(CFx)have been widely applied as lithium primary batteries due to their ultra-high energy density.It will be a great promise if CFx can be rechargeable.In this study,we rationally tune the C-F bond strength for the alkaline intercalated CFx via importing an electronegative weaker element K instead of Li.It forms a ternary phase K_(x)FC instead of two phases(LiF+C)in lithium-ion batteries.Meanwhile,we choose a large layer distance and more defects CFx,namely fluorinated soft carbon,to accommodate K.Thus,we enable CFx rechargeable as a potassium-ion battery cathode.In detail fluorinated soft carbon CF_(1.01) presents a reversible specific capacity of 339 mA h g^(-1)(797 Wh kg^(-1))in the 2nd cycle and maintains 330 mA h g^(-1)(726 Wh kg^(-1))in the 15th cycle.This study reveals the importance of tuning chemical bond stability using different alkaline ions to endow batteries with rechargeability.This work provides good references for focusing on developing reversible electrode materials from popular primary cell configurations.
基金financially supported by the National Key Research and Development Program of China(2022YFB4002103)the National Natural Science Foundation of China(22279107)。
文摘Extensive usage of highly conductive carbon materials with large specific surface area(e.g.,carbon nanotubes,CNTs)in lithium ion batteries(LIBs),especially as current collector of anodes,suffers from low initial coulombic efficiency(ICE),large interfacial resistance,and severe embrittlement,as the large specific surface area often results in severe interfacial decomposition of the electrolyte and the formation of thick and fluffy solid electrolyte interphase(SEI)during cycling of LIBs.Herein,we demonstrate that when the CNT-based current collector and Na foil(which are being stacked intimately upon each other)are being placed in Na+-based organic electrolyte,local redox reaction between the Na foil and the electrolyte would occur spontaneously,generating a thin and homogeneous NaF-based passivating layer on the CNTs.More importantly,we found that owing to the weak solvation behaviors of Na+in the organic electrolyte,the resulting passivation layer,which is rich in NaF,is thin and dense;when used as the anode current collector in LIBs,the pre-existing passivating layer can function effectively in isolating the anode from the solvated Li+,thus suppressing the formation of bulky SEI and the destructive intercalation of solvated Li+.The relevant half-cell(graphite as anode)exhibits a high ICE of 92.1%;the relevant pouch cell with thus passivated CNT film as current collectors for both electrodes(LiCoO_(2)as cathode,graphite as anode)displays a high energy density of 255 Wh kg^(-1),spelling an increase of 50%compared with that using the conventional metal current collectors.
基金supported by the National Natural Science Foundation of China (21975087, U1966214, 22008082)the Certificate of China Postdoctoral Science Foundation Grant (2019M652634,2020M672337)。
文摘The mass fraction of electrolytes is the crucial factor affecting the energy density of lithium-sulfur(Li-S)batteries. Due to the high porosity within the C/S cathode, high concentration of polysulfides, and side reaction in lithiun metal anode under lean electrolyte, it is extremely challenging to improve performance while reducing the electrolyte volume. Here, we report a novel electrolyte with relatively low density(1.16 g cm^(-2)), low viscosity(1.84 m Pa s), and high ionic conductivity, which significantly promotes energy density and cyclability of Li-S batteries under practical conditions. Moreover, such electrolyte enables a hybrid cathode electrolyte interphase(CEI) and solid electrolyte interface(SEI) layer with plentiful Li F, which leads to fast kinetics of ions transport and stable cyclability even under low temperatures.Compared to Li-S batteries in electrolyte employing 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether(TTE) diluent, the ultra-thick cathode(20 mg cm^(-2)) shows a high capacity of 9.48 m Ah cm^(-2)and excellent capacity retention of 80.3% over 191 cycles at a low electrolyte-to-sulfur ratio(E/S = 2) and negative-to-positive capacity ratio(N/P = 2.5), realizing a 19.2% improvement in energy density in coin cells(from 370 to 441 Wh kg^(-1)) and a high energy density up to 467 Wh kg^(-1) in pouch cells. This study not only provides guidance for the electrolyte design but also paves the way for the development of high performance Li-S batteries under practical conditions.
基金financially supported by the National Natural Science Foundation of China(Nos.11475260,11305264,11622547,91230205,and 11474360)the National Basic Research Program of China(No.2013CBA01504)the Research Project of NUDT(No.JC14-02-02)
文摘By using a two-dimensional particle-in-cell simulation,we demonstrate a scheme for highenergy-density electron beam generation by irradiating an ultra intense laser pulse onto an aluminum（Al） target.With the laser having a peak intensity of 4×10^23W cm^-2,a high quality electron beam with a maximum density of 117 nc and a kinetic energy density up to8.79×10^18J m^-3 is generated.The temperature of the electron beam can be 416 Me V,and the beam divergence is only 7.25°.As the laser peak intensity increases（e.g.,1024 W cm^-2）,both the beam energy density（3.56×10^19J m^-3） and the temperature（545 Me V） are increased,and the beam collimation is well controlled.The maximum density of the electron beam can even reach 180 nc.Such beams should have potential applications in the areas of antiparticle generation,laboratory astrophysics,etc.
基金the National Natural Science Foundation of China(Grant Nos.12174352 and 12111530103)the Fundamental Research Funds for the Central UniversitiesChina University of Geosciences(Wuhan)(Grant No.G1323523065)。
文摘Molecular crystals are complex systems exhibiting various crystal structures,and accurately modeling the crystal structures is essential for understanding their physical behaviors under high pressure.Here,we perform an extensive structure search of ternary carbon-nitrogen-oxygen(CNO)compound under high pressure with the CALYPSO method and first principles calculations,and successfully identify three polymeric CNO compounds with Pbam,C2/m and I4m2symmetries under 100 GPa.More interestingly,these structures are also dynamically stable at ambient pressure,and are potential high energy density materials(HEDMs).The energy densities of Pbam,C2/m and I4m2 phases of CNO are about2.30 kJ/g,1.37 kJ/g and 2.70 kJ/g,respectively,with the decompositions of graphitic carbon and molecular carbon dioxide andα-N(molecular N_(2))at ambient pressure.The present results provide in-depth insights into the structural evolution and physical properties of CNO compounds under high pressures,which offer crucial insights for designs and syntheses of novel HEDMs.
基金supported by the Double First-Class Construction Funds of Sichuan University and National Natural Science Foundation of China(NNSFC)financial support from the National Science Foundation of China(51873126,51422305,51721091)。
文摘The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^(-2) delivers a stable area capacity of 6.6 mAh cm^(-2) over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^(-2) over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.
基金J.Wang acknowledges the support by MOE,Singapore Ministry of Education(MOE2018-T2-2-095)for research work conducted at the National University of Singapore.Z.L.Liu acknowledges the A*STAR’s Central Research Funds(CRF)Award(Project:SC25/21-111312)+1 种基金Y.Gao acknowledges financial support by ST Engineering Advanced Material Engineering Pte.Ltd.and Singapore Economic Development BoardOpen access funding provided by Shanghai Jiao Tong University
文摘Rechargeable batteries of high energy density and overall performance are becoming a critically important technology in the rapidly changing society of the twenty-first century.While lithium-ion batteries have so far been the dominant choice,numerous emerging applications call for higher capacity,better safety and lower costs while maintaining sufficient cyclability.The design space for potentially better alternatives is extremely large,with numerous new chemistries and architectures being simultaneously explored.These include other insertion ions(e.g.sodium and numerous multivalent ions),conversion electrode materials(e.g.silicon,metallic anodes,halides and chalcogens)and aqueous and solid electrolytes.However,each of these potential“beyond lithium-ion”alternatives faces numerous challenges that often lead to very poor cyclability,especially at the commercial cell level,while lithium-ion batteries continue to improve in performance and decrease in cost.This review examines fundamental principles to rationalise these numerous developments,and in each case,a brief overview is given on the advantages,advances,remaining challenges preventing cell-level implementation and the state-of-the-art of the solutions to these challenges.Finally,research and development results obtained in academia are compared to emerging commercial examples,as a commentary on the current and near-future viability of these“beyond lithium-ion”alternatives.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF2018R1D1A1B07051249)Nano Material Technology Development Program(NRF-2015M3A7B6027970)of MSIP/NRF and Center for Integrated Smart Sensors funded by the Ministry of Science,ICTFuture Planning,Republic of Korea,as Global Frontier Project(CISS-2012M3A6A6054186).
文摘Flexible supercapacitor electrodes with high mass loading are crucial for obtaining favorable electrochemical performance but still challenging due to sluggish electron and ion transport.Herein,rationally designed CNT/MnO2/graphene-grafted carbon cloth electrodes are prepared by a“graft-deposit-coat”strategy.Due to the large surface area and good conductivity,graphene grafted on carbon cloth offers additional surface areas for the uniform deposition of MnO2(9.1 mg cm?2)and facilitates charge transfer.Meanwhile,the nanostructured MnO2 provides abundant electroactive sites and short ion transport distance,and CNT coated on MnO2 acts as interconnected conductive“highways”to accelerate the electron transport,significantly improving redox reaction kinetics.Benefiting from high mass loading of electroactive materials,favorable conductivity,and a porous structure,the electrode achieves large areal capacitances without compromising rate capability.The assembled asymmetric supercapacitor demonstrates a wide working voltage(2.2 V)and high energy density of 10.18 mWh cm?3.
基金the Council of Scientific & Industrial Research(CSIR) for the financial support through the HCP-44/02/1 projectthe DST-INSPIRE Faculty Scheme,Department of Science and Technology,New Delhi,Govt.of India(IFA20-MS-168) for the financial supports。
文摘Development of cost-effective and environmental friendly energy storage devices(ESDs) has attracted widespread attention in recent scenario of energy research.Recently,the environmentally viable "water-in-salt"(WiS) electrolytes has received significant interest for the development of advanced high performance ESDs.The WiS electrolyte exhibits wide electrochemical stability window(ESW),highsafety,non-flammability and superior electrochemical performance compared to the conventional "salt-in-water" electrolytes.This review aims to provide a comprehensive discussion on WiS electrolyte based on theoretical,electrochemical and physicochemical characteristics.A strategic way for the usage of WiS electrolyte in rechargeable metal-ion batteries and supercapacitors with potentially improved electrochemical performance has been reviewed systematically.This review also discussed the unique advantages of WiS electrolytes as well as the future scope and challenges.
