An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium brom...An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic surfactant,is adopted to draw more anions into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO_(3)^(−)/FSI−anions in the EDL region due to the positively charged CTA^(+).In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li^(+)transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li||Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm^(-2) with a capacity of 1 mAh cm^(-2).Moreover,Li||LiFePO_(4) and Li||LiCoO_(2) with a high cathode mass loading of>10 mg cm^(-2) can be stably cycled over 180 cycles.展开更多
The absence of control over carriers transport during electrochemical cycling,accompanied by the deterioration of the solid electrolyte interphase(SEI)and the growth of lithium dendrites,has hindered the development o...The absence of control over carriers transport during electrochemical cycling,accompanied by the deterioration of the solid electrolyte interphase(SEI)and the growth of lithium dendrites,has hindered the development of lithium metal batteries.Herein,a separator complexion consisting of polyacrylonitrile(PAN)nanofiber and MIL-101(Cr)particles prepared by electrospinning is proposed to bind the anions from the electrolyte utilizing abundant effective open metal sites in the MIL-101(Cr)particles to modulate the transport of non-effective carriers.The binding effect of the PANM separator promotes uniform lithium metal deposition and enhances the stability of the SEI layer and long cycling stability of ultra-high nickel layered oxide cathodes.Taking PANM as the Li||NCM96 separator enables high-voltage cycling stability,maintaining 72%capacity retention after 800 cycles at a charging and discharging rate of 0.2 C at a cut-off voltage of 4.5 V and 0°C.Meanwhile,the excellent high-rate performance delivers a specific capacity of 156.3 mA h g^(-1) at 10 C.In addition,outstanding cycling performance is realized from−20 to 60°C.The separator engineering facilitates the electrochemical performance of lithium metal batteries and enlightens a facile and promising strategy to develop fast charge/discharge over a wide range of temperatures.展开更多
Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand applications.However,their commercial applicability is hampered by hysteretic electrode reactio...Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand applications.However,their commercial applicability is hampered by hysteretic electrode reaction kinetics and the shuttle effect of lithium polysulfides(LiPSs).In this work,an interlayer consisting of high-entropy metal oxide(Cu_(0.7)Fe_(0.6)Mn_(0.4)Ni_(0.6)Sn_(0.5))O_(4) grown on carbon nanofibers(HEO/CNFs)is designed for LSBs.The CNFs with highly porous networks provide transport pathways for Li^(+) and e^(-),as well as a physical sieve effect to limit LiPSs crossover.In particular,the grapevine-like HEO nanoparticles generate metal-sulfur bonds with LiPSs,efficiently anchoring active materials.The unique structure and function of the interlayer enable the LSBs with superior electrochemical performance,i.e.,the high specific capacity of 1381 mAh g^(-1) at 0.1 C and 561 mAh g^(-1) at 6 C.This work presents a facile strategy for exploiting high-performance LSBs.展开更多
The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuni...The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.展开更多
In this review,we discuss the electrochemical properties of Prussian blue(PB)for Na^(+)storage by combining structural engineering and electrolyte modifications.We integrated experimental data and density functional t...In this review,we discuss the electrochemical properties of Prussian blue(PB)for Na^(+)storage by combining structural engineering and electrolyte modifications.We integrated experimental data and density functional theory(DFT)in sodium-ion battery(SIB)research to refine the atomic arrangements and crystal lattices and introduce substitutions and dopants.These changes affect the lattice stability,intercalation,electronic and ionic conductivities,and electrochemical performance.We unraveled the intricate structure-electrochemical behavior relationship by combining experimental data with computational models,including first-principles calculations.This holistic approach identified techniques for optimizing PB and Prussian blue analog(PBA)structu ral properties for SIBs.We also discuss the tuning of electrolytes by systematically adjusting their composition,concentration,and additives using a combination of molecular dynamics(MD)simulations and DFT computations.Our review offers a comprehensive assessment of strategies for enhancing the electrochemical properties of PB and PBAs through structural engineering and electrolyte modifications,combining experimental insights with advanced computational simulations,and paving the way for next-generation energy storage systems.展开更多
Lithium sulfur batteries(LSBs)are recognized as promising devices for developing next-generation energy storage systems.In addition,they are attractive rechargeable battery systems for replacing lithium-ion batteries(...Lithium sulfur batteries(LSBs)are recognized as promising devices for developing next-generation energy storage systems.In addition,they are attractive rechargeable battery systems for replacing lithium-ion batteries(LIBs)for commercial use owing to their higher theoretical energy density and lower cost compared to those of LIBs.However,LSBs are still beset with some persistent issues that prevent them from being used industrially,such as the unavoidable dissolution of lithium polysulfide intermediates during electrochemical reactions and large volume expansion(up to 80%)upon the formation of Li_(2)S,resulting in serious battery life and safety limitations.In the process of solving these problems,it is necessary to maintain a high sulfur content in the cathode materials to ensure that the LSBs have high energy densities and excellent cycle performance.In this review,the novel preparation methods and cathode materials used for preparing LSBs in recent years are reviewed considering the sulfur content and cycle performance.In addition,the problems and difficulties in practically applying cathode materials are described,and the development trend is discussed.展开更多
Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in seconda...Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.展开更多
Composite solid electrolytes(CSEs)with poly(ethylene oxide)(PEO)have become fairly prevalent for fabricating high-performance solid-state lithium metal batteries due to their high Li~+solvating capability,flexible pro...Composite solid electrolytes(CSEs)with poly(ethylene oxide)(PEO)have become fairly prevalent for fabricating high-performance solid-state lithium metal batteries due to their high Li~+solvating capability,flexible processability and low cost.However,unsatisfactory room-temperature ionic conductivity,weak interfacial compatibility and uncontrollable Li dendrite growth seriously hinder their progress.Enormous efforts have been devoted to combining PEO with ceramics either as fillers or major matrix with the rational design of two-phase architecture,spatial distribution and content,which is anticipated to hold the key to increasing ionic conductivity and resolving interfacial compatibility within CSEs and between CSEs/electrodes.Unfortunately,a comprehensive review exclusively discussing the design,preparation and application of PEO/ceramic-based CSEs is largely lacking,in spite of tremendous reviews dealing with a broad spectrum of polymers and ceramics.Consequently,this review targets recent advances in PEO/ceramicbased CSEs,starting with a brief introduction,followed by their ionic conduction mechanism,preparation methods,and then an emphasis on resolving ionic conductivity and interfacial compatibility.Afterward,their applications in solid-state lithium metal batteries with transition metal oxides and sulfur cathodes are summarized.Finally,a summary and outlook on existing challenges and future research directions are proposed.展开更多
Rechargeable aqueous zinc-ion batteries are promising candidate for gridscale energy storage.However,the development of zinc-ion batteries has been plagued by the lack of cathode materials with high specific capacity ...Rechargeable aqueous zinc-ion batteries are promising candidate for gridscale energy storage.However,the development of zinc-ion batteries has been plagued by the lack of cathode materials with high specific capacity and superior lifespan.Herein,hexagonal Cs_(0.3)V_(2)O_(5)cathode is fabricated and investigated in zinc-ion batteries.Compared with the traditional vanadium oxides,the introduction of Cs changes the periodic atomic arrangements,which not only stabilizes the open framework structure but also facilitates the Zn^(2+)diffusion with a lower migration energy barrier.Consequently,high specific capacity of 543.8 mA h g^(-1)at 0.1 A g^(-1)is achieved,which surpasses most of reported cathode materials in zinc-ion batteries.The excellent cycle life is achieved over 1000 cycles with about 87.8%capacity retention at 2 A g^(-1).Furthermore,the morphological evolution and energy storage mechanisms are also revealed via a series of techniques.This work opens up a phase engineering strategy to fabricate the hexagonal vanadium oxide and elucidate the application of phase-dependent cathodes in zinc-ion batteries.展开更多
This study explored the complex effect of graphite tortuosity on the electrochemical performance of Ni-rich NCA90 Li-ion batteries(LIBs).Different levels of graphite anode tortuosity were analyzed,revealing that low-t...This study explored the complex effect of graphite tortuosity on the electrochemical performance of Ni-rich NCA90 Li-ion batteries(LIBs).Different levels of graphite anode tortuosity were analyzed,revealing that low-tortuosity electrodes had better graphite utilization.The in-plane tortuosities of the graphite anode electrodes examined were 1.70,1.94,2.05,and 2.18,while their corresponding through-plane tortuosities were 4.74,6.94,8.19,and 9.80.In-operando X-ray diffraction and differential electrochemical mass spectrometry were employed to investigate the charge storage mechanism and gas evolution.The study revealed that while graphite electrode tortuosity impacted the amount of Li present in the lithiated graphite phase due to diffusion constraints,it did not affect gas generation.The Li-ion utilization in low-tortuosity electrodes was higher than that in high-tortuosity electrodes because of solid-diffusion limitations.Additionally,the galvanostatic intermittent titration technique(GITT) was employed to investigate a lithium-ion diffusion coefficient.Our results indicate that the lithium-ion diffusion coefficient exhibits a significant difference only during LiC_(6) phase transition.We also observed that the use of a lower tortuosity electrode leads to improved lithium-ion insertion.Consequently,graphite utilization is influenced by the porous electrode design.Safety tests adhering to UN38.3 guidelines verified battery safety.The study demonstrated the practical application of optimized NCA90 LIB cells with diverse graphite electrode tortuosities in a high-performance Lamborghini GoKart,paving the way for further advancements in Ni-rich LIB technology.展开更多
Because of their large volume variation and inferior electrical conductivity,Mn_(3)O_(4)-based oxide anode materials have short cyclic lives and poor rate capability,which obstructs their development.In this study,we ...Because of their large volume variation and inferior electrical conductivity,Mn_(3)O_(4)-based oxide anode materials have short cyclic lives and poor rate capability,which obstructs their development.In this study,we successfully prepared a Mn_(3)O_(4)/N-doped honeycomb carbon composite using a smart and facile synthetic method.The Mn_(3)O_(4)nanopolyhedra are grown on N-doped honeycomb carbon,which evidently mitigates the volume change in the charging and discharging processes but also improves the electrochemical reaction kinetics.More importantly,the Mn-O-C bond in the Mn_(3)O_(4)/N-doped honeycomb carbon composite benefits electrochemical reversibility.These features of the Mn_(3)O_(4)/N-doped honeycomb carbon(NHC)composite are responsible for its superior electrochemical performance.When used for Li-ion batteries,the Mn_(3)O_(4)/N-doped honeycomb carbon anode exhibits a high reversible capacity of 598 mAh·g^(−1)after 350 cycles at 1 A·g^(−1).Even at 2 A·g^(−1),the Mn_(3)O_(4)/NHC anode still delivers a high capacity of 472 mAh·g^(−1).This work provides a new prospect for synthesizing and developing manganese-based oxide materials for energy storage.展开更多
All solid-state electrolytes have the advantages of good mechanical and thermal properties for safer energy storage,but their energy density has been limited by low ionic conductivity and large interfacial resistance ...All solid-state electrolytes have the advantages of good mechanical and thermal properties for safer energy storage,but their energy density has been limited by low ionic conductivity and large interfacial resistance caused by the poor Li~+transport kinetics due to the solid-solid contacts between the electrodes and the solid-state electrolytes.Herein,a novel gel polymer electrolyte(UPP-5)composed of ionic liquid incorporated metal-organic frameworks nanoparticles(IL@MOFs)is designed,it exhibits satisfying electrochemical performances,consisting of an excellent electrochemical stability window(5.5 V)and an improved Li^(+)transference number of 0.52.Moreover,the Li/UPP-5/LiFePO_(4) full cells present an ultra-stable cycling performance at 0.2C for over 100 cycles almost without any decay in capacities.This study might provide new insight to create an effective Li^(+)conductive network for the development of all-solid-state lithium-ion batteries.展开更多
The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,...The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton(3DIO FCSe-QDs@NC)is elaborately designed for both sulfur cathode and Li metal anode.The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble Li PSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors.Simultaneously,the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites.Taking advantage of these merits,the assembled Li-S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability(a low decay rate of 0.014%over 2,000 cycles at 2C).Remarkably,a promising areal capacity of 8.41 mAh cm^(-2)can be achieved at the sulfur loading up to 8.50 mg cm^(-2)with an ultra-low electrolyte/sulfur ratio of 4.1μL mg^(-1).This work paves the bi-serve host design from systematic experimental and theoretical analysis,which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li-S full batteries.展开更多
Realizing a lithium sulfide(Li_(2)S)cathode with both high energy density and a long lifespan requires an innovative cathode design that maximizes electrochemical performance and resists electrode deterioration.Herein...Realizing a lithium sulfide(Li_(2)S)cathode with both high energy density and a long lifespan requires an innovative cathode design that maximizes electrochemical performance and resists electrode deterioration.Herein,a high-loading Li_(2)S-based cathode with micrometric Li_(2)S particles composed of two-dimensional graphene(Gr)and one-dimensional carbon nanotubes(CNTs)in a compact geometry is developed,and the role of CNTs in stable cycling of high-capacity Li–S batteries is emphasized.In a dimensionally combined carbon matrix,CNTs embedded within the Gr sheets create robust and sustainable electron diffusion pathways while suppressing the passivation of the active carbon surface.As a unique point,during the first charging process,the proposed cathode is fully activated through the direct conversion of Li_(2)S into S_(8) without inducing lithium polysulfide formation.The direct conversion of Li_(2)S into S_(8) in the composite cathode is ubiquitously investigated using the combined study of in situ Raman spectroscopy,in situ optical microscopy,and cryogenic transmission electron microscopy.The composite cathode demonstrates unprecedented electrochemical properties even with a high Li_(2)S loading of 10 mg cm^(–2);in particular,the practical and safe Li–S full cell coupled with a graphite anode shows ultra-long-term cycling stability over 800 cycles.展开更多
The electrolyte integrated with lithium metal anodes is subjected to the issues of interfacial compatibility and stability,which strongly influence the performances of high-energy lithium metal batteries.Here,we repor...The electrolyte integrated with lithium metal anodes is subjected to the issues of interfacial compatibility and stability,which strongly influence the performances of high-energy lithium metal batteries.Here,we report a new electrolyte recipe viz.a moderately concentrated electrolyte comprising of 2.4 M lithium bis(fluorosulfonyl)imide(LiFSI)in a cosolvent mixture of fluorinated ethylene carbonate(FEC)and dimethyl carbonate(DMC)with relatively high ion conductivity.Owing to the preferential decomposition of LiFSI and FEC,an inorganic-rich interphase with abundant Li_(2)O and LiF nanocrystals is formed on lithium metal with improved robustness and ion transfer kinetics,enabling lithium plating/stripping with an extremely low overpotential of~8 mV and the average CE of 97%.When tested in Li||LiFePO_(4) cell,this electrolyte provides long-term cycling with a capacity retention of 98.3%after 1000 cycles at 1 C and an excellent rate performance of 20 C,as well as an areal capacity of 1.35 mA h cm^(-2)at the cathode areal loading of 9 mg cm^(-2).Moreover,the Li||LiFePO_(4) cell exhibits excellent wide-temperature performances(-40~60℃),including long-term cycling stability over 2600 cycles without visible capacity fading at 0℃,as well as extremely high average CEs of 99.6%and 99.8% over 400 cycles under-20℃ and 45℃.展开更多
To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a st...To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a strategy to effectively capture soluble lithium polysulfide intermediates and promote their conversion reaction by integrating highly polar metal oxides with catalytically active metals sulfides.However,to fully exploit the outstanding properties of heterostructure-based composites,their detailed structure and interfacial contacts should be designed rationally.Herein,optimally arranged TiO_(2)and MoS_(2)-based heterostructures(TiO_(2)@MoS_(2)) are fabricated on carbon cloth as a multifunctional interlayer to efficiently trap polysulfide intermediates and accelerate their redox kinetics.Owing to the synergistic effects between TiO_(2)and MoS_(2)and the uniform heterointerface distribution that induces the ideally oriented built-in electric field,Li-S batteries with TiO_(2)@MoS_(2)interlayers exhibit high rate capability(601 mA h g^(-1)at 5 C),good cycling stability(capacity-fade rate of 0.067% per cycle over 500 cycles at2 C),and satisfactory areal capacity(5.2 mA h cm^(-2)) under an increased sulfur loading of 5.2 mg cm^(-2).Moreover,by comparing with a MoS_(2)@TiO_(2)interlayer composed of reversely arranged heterostructures,the effect of the built-in electric field’s direction on the electrocatalytic reactions of polysulfide intermediates is thoroughly investigated for the first time.The superior electrocatalytic activities of the rationally arranged TiO_(2)@MoS_(2)interlayer demonstrate the importance of optimizing the built-in electric field of heterostructures for producing high-performance Li-S batteries.展开更多
The use of carbonized wood in various functional devices is attracting considerable attention due to its low cost,vertical channels,and high electrical conduction.However,the conventional carbonization method requires...The use of carbonized wood in various functional devices is attracting considerable attention due to its low cost,vertical channels,and high electrical conduction.However,the conventional carbonization method requires a long processing time and an inert atmosphere.Here,a microwave-assisted ultrafast carbonization technique was developed that carbonizes natural wood in seconds without the need for an inert atmosphere,and the obtained aligned-porous carbonized wood provided an excellent electrochemical performance as an anode material for lithium-ion batteries.This ultrafast carbonization technique simultaneously produced ZnO nanoparticles during the carbonization process that were uniformly distributed on the alignedporous carbon.The hierarchical structure of carbonized wood functionalized with ZnO nanoparticles was used as a host for achieving high-performance lithium-sulfur batteries:the highly conductive carbonized wood framework with vertical channels provided good electron transport pathways,and the homogeneously dispersed ZnO nanoparticles effectively adsorbed lithium polysulfide and catalyzed its conversion reactions.In summary,a new method was developed to realize the ultrafast carbonization of biomass materials with decorated metal oxide nanoparticles.展开更多
Lithium-sulfur(Li-S)batteries with high energy density are considered promising energy storage devices for the next generation.Nevertheless,the shuttle effect and the passive layer between the separator and the electr...Lithium-sulfur(Li-S)batteries with high energy density are considered promising energy storage devices for the next generation.Nevertheless,the shuttle effect and the passive layer between the separator and the electrodes still seriously affect the cycle stability and life.Herein,a bimetallic Ni-Co metal-organic framework(MOF)with adsorption and catalytic synergism for polysulfides was successfully synthesized as an electrospinning separator sandwich for Li-S batteries.Introducing porous Ni-Co MOF coatings into the separator provides more adsorption catalytic sites for polysulfides,prevents their diffusion to the anode,and enhances sulfur utilization.Consequently,the improved Li-S batteries with a Ni-Co MOF@PAN(NCMP)electrospun separator delivered excellent rate performance and outstanding cycle stability,yielding an ultra-high initial capacity of 1560 mA h g^(-1)at 0.1 C.Notably,remarkable Li-S battery performance with a discharge capacity of 794 mA h g^(-1)(84.1%capacity retention)was obtained after500 cycles,while delivering a low capacity decay rate of 0.032%during long-term cycling(up to 500cycles)at 1 C.Surprisingly,even at the current density of 2 C,the capacity attenuation rate of 2000 cycles is only 0.034%per cycle.In addition,compared with the Celgard separator,the NCMP separator also had high thermal stability(keeping the separator outline at 200℃)that ensured battery safety and excellent electrolyte wettability(73%porosity and 535%electrolyte absorption)and significantly enhanced the ionic conductivity and Li^(+) transfer number,and protected the surface integrity of the anode.展开更多
Na_(3)V_(2)(PO_(4))_(2)O_(2)F(NVPOF)has received considerable interest as a promising cathode material for sodium-ion batteries because of its high working voltage and good structural/thermal stability.However,the slu...Na_(3)V_(2)(PO_(4))_(2)O_(2)F(NVPOF)has received considerable interest as a promising cathode material for sodium-ion batteries because of its high working voltage and good structural/thermal stability.However,the sluggish electrode reaction resulting from its low intrinsic electronic conductivity significantly restricts its electrochemical performance and thus its practical application.Herein,Nb-doped Na_(3)V_(2-x)Nb_(x)(PO_(4))_(2)O_(2)F/graphene(rGO)composites(x=0,0.05,0.1)were prepared using a solvothermal method followed by calcination.Compared to the un-doped NVPOF/r GO,doping V-site with high-valence Nb element(Nb^(5+))(Na_(3)V_(1.95)Nb_(0.05)(PO_(4))_(2)O_(2)F/r GO(NVN05POF/rGO))can result in the generated V4^(+)/V3^(+)mixed-valence,ensuring the lower bandgap and thus the increased intrinsic electronic conductivity.Besides,the expanded lattice space favors the Na^(+)migration.With the structure feature where NVN05POF particles are attached to the rGO sheets,the electrode reaction kinetics is further accelerated owing to the well-constructed electron conductive network.As a consequence,the as-prepared NVN05POF/r GO sample exhibits a high specific capacity of~72 m Ah·g^(-1)at 10C(capacity retention of 65.2%(vs.0.5C))and excellent long-term cycling stability with the capacity fading rate of~0.099%per cycle in 500 cycles at 5C.展开更多
Natural minerals-based energy materials have attracted enormous attention because of the advantages of good materials consistency,high production,environmental friendliness,and low cost.The uniform distribution of gra...Natural minerals-based energy materials have attracted enormous attention because of the advantages of good materials consistency,high production,environmental friendliness,and low cost.The uniform distribution of grains can effectively inhibit the aggregation of active materials,improving lithium storage performance.In this work,natural graphite is modified by polyvinylpyrrolidone to obtain modified graphite with reduced size and better dispersion.Natural pyrite composite polyvinylpyrrolidone-modified graphite(pyrite/PG)material with uniform particle distribution is obtained by the ball milling process.The subsequent calcination process converts pyrite/PG into Fe_(1-x)Scompounded with polyvinylpyrrolidone-modified graphite(Fe_(1-x)S/PG).The homogeneous grain distributions of active material can facilitate the faster transfer of electrons and promote the efficient utilization of active materials.The as-prepared Fe_(1-x)S/PG electrode exhibits a remarkably reversible specific capacity of 613.0 mAh·g^(-1)at 0.2 A·g^(-1)after 80 cycles and an excellent rate capability of 523.0 mAh·g^(-1)at 5 A·g^(-1).Even at a higher current density of 10 A·g^(-1),it can deliver a specific capacity of 348.0 mAh·g^(-1).Moreover,the dominant pseudocapacitance in redox reactions accounts for the impressive rate and cycling stability.This work provides a low-cost and facile method to fabricate natural mineral-based anode materials and apprise readers about the impact of uniform particle distribution on lithium storage performance.展开更多
基金financial support from Singapore Ministry of Education under its AcRF Tier 2 Grant No MOE-T2EP10123-0001Singapore National Research Foundation Investigatorship under Grant No NRF-NRFI08-2022-0009Academic Excellence Foundation of BUAA for PhD Students(applicant:Hongfei Xu).
文摘An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic surfactant,is adopted to draw more anions into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO_(3)^(−)/FSI−anions in the EDL region due to the positively charged CTA^(+).In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li^(+)transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li||Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm^(-2) with a capacity of 1 mAh cm^(-2).Moreover,Li||LiFePO_(4) and Li||LiCoO_(2) with a high cathode mass loading of>10 mg cm^(-2) can be stably cycled over 180 cycles.
基金financially supported by the National Key Research and Development Program of China(No.2021YFB2400300)the IPE Talent Start-up Program of Institute of Process Engineering of Chinese Academy of Sciences(Grant No.E0293507)。
文摘The absence of control over carriers transport during electrochemical cycling,accompanied by the deterioration of the solid electrolyte interphase(SEI)and the growth of lithium dendrites,has hindered the development of lithium metal batteries.Herein,a separator complexion consisting of polyacrylonitrile(PAN)nanofiber and MIL-101(Cr)particles prepared by electrospinning is proposed to bind the anions from the electrolyte utilizing abundant effective open metal sites in the MIL-101(Cr)particles to modulate the transport of non-effective carriers.The binding effect of the PANM separator promotes uniform lithium metal deposition and enhances the stability of the SEI layer and long cycling stability of ultra-high nickel layered oxide cathodes.Taking PANM as the Li||NCM96 separator enables high-voltage cycling stability,maintaining 72%capacity retention after 800 cycles at a charging and discharging rate of 0.2 C at a cut-off voltage of 4.5 V and 0°C.Meanwhile,the excellent high-rate performance delivers a specific capacity of 156.3 mA h g^(-1) at 10 C.In addition,outstanding cycling performance is realized from−20 to 60°C.The separator engineering facilitates the electrochemical performance of lithium metal batteries and enlightens a facile and promising strategy to develop fast charge/discharge over a wide range of temperatures.
基金financially supported by the Certificate of postdoctoral research grant in Henan province,the Natural Science Foundation of Henan province(Grant No.212300410281)the National Natural Science Foundation of China(Grant No.21975225).
文摘Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand applications.However,their commercial applicability is hampered by hysteretic electrode reaction kinetics and the shuttle effect of lithium polysulfides(LiPSs).In this work,an interlayer consisting of high-entropy metal oxide(Cu_(0.7)Fe_(0.6)Mn_(0.4)Ni_(0.6)Sn_(0.5))O_(4) grown on carbon nanofibers(HEO/CNFs)is designed for LSBs.The CNFs with highly porous networks provide transport pathways for Li^(+) and e^(-),as well as a physical sieve effect to limit LiPSs crossover.In particular,the grapevine-like HEO nanoparticles generate metal-sulfur bonds with LiPSs,efficiently anchoring active materials.The unique structure and function of the interlayer enable the LSBs with superior electrochemical performance,i.e.,the high specific capacity of 1381 mAh g^(-1) at 0.1 C and 561 mAh g^(-1) at 6 C.This work presents a facile strategy for exploiting high-performance LSBs.
基金supported by the National Natural Science Foundation of China (52173286, 52207249)Major basic research project of Natural Science Foundation of Shandong Province (ZR2023ZD12)+1 种基金the State Key Laboratory of Marine Resource Utilization in South China Sea (Hainan University) (MRUKF2023013)Open Program of Guangxi Key Laboratory of Information Materials (221024-K)。
文摘The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(NRF-2022R1C1C1011058)。
文摘In this review,we discuss the electrochemical properties of Prussian blue(PB)for Na^(+)storage by combining structural engineering and electrolyte modifications.We integrated experimental data and density functional theory(DFT)in sodium-ion battery(SIB)research to refine the atomic arrangements and crystal lattices and introduce substitutions and dopants.These changes affect the lattice stability,intercalation,electronic and ionic conductivities,and electrochemical performance.We unraveled the intricate structure-electrochemical behavior relationship by combining experimental data with computational models,including first-principles calculations.This holistic approach identified techniques for optimizing PB and Prussian blue analog(PBA)structu ral properties for SIBs.We also discuss the tuning of electrolytes by systematically adjusting their composition,concentration,and additives using a combination of molecular dynamics(MD)simulations and DFT computations.Our review offers a comprehensive assessment of strategies for enhancing the electrochemical properties of PB and PBAs through structural engineering and electrolyte modifications,combining experimental insights with advanced computational simulations,and paving the way for next-generation energy storage systems.
基金the National Natural Science Foundation of China(52103093)the Young Elite Scientists Sponsorship Program by China Association for Science and Technology(2021QNRC001)+2 种基金the Jiangxi Provincial Natural Science Foundation(20212BAB214048)Science and Technology Support Project of Shangrao(2020L009,2021J006)Science and Technological Project of Education Department of Jiangxi(GJJ211704)for funding their contributions to this paper。
文摘Lithium sulfur batteries(LSBs)are recognized as promising devices for developing next-generation energy storage systems.In addition,they are attractive rechargeable battery systems for replacing lithium-ion batteries(LIBs)for commercial use owing to their higher theoretical energy density and lower cost compared to those of LIBs.However,LSBs are still beset with some persistent issues that prevent them from being used industrially,such as the unavoidable dissolution of lithium polysulfide intermediates during electrochemical reactions and large volume expansion(up to 80%)upon the formation of Li_(2)S,resulting in serious battery life and safety limitations.In the process of solving these problems,it is necessary to maintain a high sulfur content in the cathode materials to ensure that the LSBs have high energy densities and excellent cycle performance.In this review,the novel preparation methods and cathode materials used for preparing LSBs in recent years are reviewed considering the sulfur content and cycle performance.In addition,the problems and difficulties in practically applying cathode materials are described,and the development trend is discussed.
基金financially supported by the Shenzhen Science and Technology Program(JCYJ20220530141012028),ChinaThe National Natural Science Foundation of China(22005178),China+2 种基金The Key Research and Development Program of Shandong Province(2021ZLGX01),ChianThe fellowship of China Postdoctoral Science Foundation(2022M722333),Chianthe Jiangsu Funding Program for Excellent Postdoctoral Talent,Chian。
文摘Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.
基金financially supported by National Key R&D Program for International Cooperation(No.2021YFE0115100)the project of the National Natural Science Foundation of China(Nos.51872240,51972270 and 52172101)+4 种基金Key Research and Development Program of Shaanxi Province(No.2021ZDLGY14-08 and 2022KWZ-04)Natural Science Foundation of Shaanxi Province(2020JZ-07)the Research Fund of the State Key Laboratory of Solidification Processing(NPU),China(2021-TS-03)the Fundamental Research Funds for the Central Universities(No.3102019JC005 and G2022KY0604)the Research Fund of the State Key Laboratory of Solid Lubrication(CAS),China(LSL-2007)。
文摘Composite solid electrolytes(CSEs)with poly(ethylene oxide)(PEO)have become fairly prevalent for fabricating high-performance solid-state lithium metal batteries due to their high Li~+solvating capability,flexible processability and low cost.However,unsatisfactory room-temperature ionic conductivity,weak interfacial compatibility and uncontrollable Li dendrite growth seriously hinder their progress.Enormous efforts have been devoted to combining PEO with ceramics either as fillers or major matrix with the rational design of two-phase architecture,spatial distribution and content,which is anticipated to hold the key to increasing ionic conductivity and resolving interfacial compatibility within CSEs and between CSEs/electrodes.Unfortunately,a comprehensive review exclusively discussing the design,preparation and application of PEO/ceramic-based CSEs is largely lacking,in spite of tremendous reviews dealing with a broad spectrum of polymers and ceramics.Consequently,this review targets recent advances in PEO/ceramicbased CSEs,starting with a brief introduction,followed by their ionic conduction mechanism,preparation methods,and then an emphasis on resolving ionic conductivity and interfacial compatibility.Afterward,their applications in solid-state lithium metal batteries with transition metal oxides and sulfur cathodes are summarized.Finally,a summary and outlook on existing challenges and future research directions are proposed.
基金financialy supported by the National Natural Science Foundation of China(Nos.22109140,21875221,and 22075223)Distinguished Young Scholars Innovation Team of Zhengzhou University(No.32320275)the Youth Talent Support Program of High-Level Talents Special Support Plan in Henan Province(ZYQR201810148)
文摘Rechargeable aqueous zinc-ion batteries are promising candidate for gridscale energy storage.However,the development of zinc-ion batteries has been plagued by the lack of cathode materials with high specific capacity and superior lifespan.Herein,hexagonal Cs_(0.3)V_(2)O_(5)cathode is fabricated and investigated in zinc-ion batteries.Compared with the traditional vanadium oxides,the introduction of Cs changes the periodic atomic arrangements,which not only stabilizes the open framework structure but also facilitates the Zn^(2+)diffusion with a lower migration energy barrier.Consequently,high specific capacity of 543.8 mA h g^(-1)at 0.1 A g^(-1)is achieved,which surpasses most of reported cathode materials in zinc-ion batteries.The excellent cycle life is achieved over 1000 cycles with about 87.8%capacity retention at 2 A g^(-1).Furthermore,the morphological evolution and energy storage mechanisms are also revealed via a series of techniques.This work opens up a phase engineering strategy to fabricate the hexagonal vanadium oxide and elucidate the application of phase-dependent cathodes in zinc-ion batteries.
基金financially supported under the Program Management Unit for National Competitiveness Enhancement (PMUC) by the Office of the National Higher Education Science Research and Innovation Policy Council (NXPO) PTT Public Company LimitedIRPC Public Company Limited, Thailand Science Research and Innovation (TSRI) under the Fundamental Fund by TSRI (FRB660004/0457)+2 种基金Vidyasirimedhi Institute of Science and Technology (VISTEC)Energy Policy and Planning Office (EPPO), Ministry of Energy, Thailandthe Frontier Research Centre (FRC) supported this work, VISTEC。
文摘This study explored the complex effect of graphite tortuosity on the electrochemical performance of Ni-rich NCA90 Li-ion batteries(LIBs).Different levels of graphite anode tortuosity were analyzed,revealing that low-tortuosity electrodes had better graphite utilization.The in-plane tortuosities of the graphite anode electrodes examined were 1.70,1.94,2.05,and 2.18,while their corresponding through-plane tortuosities were 4.74,6.94,8.19,and 9.80.In-operando X-ray diffraction and differential electrochemical mass spectrometry were employed to investigate the charge storage mechanism and gas evolution.The study revealed that while graphite electrode tortuosity impacted the amount of Li present in the lithiated graphite phase due to diffusion constraints,it did not affect gas generation.The Li-ion utilization in low-tortuosity electrodes was higher than that in high-tortuosity electrodes because of solid-diffusion limitations.Additionally,the galvanostatic intermittent titration technique(GITT) was employed to investigate a lithium-ion diffusion coefficient.Our results indicate that the lithium-ion diffusion coefficient exhibits a significant difference only during LiC_(6) phase transition.We also observed that the use of a lower tortuosity electrode leads to improved lithium-ion insertion.Consequently,graphite utilization is influenced by the porous electrode design.Safety tests adhering to UN38.3 guidelines verified battery safety.The study demonstrated the practical application of optimized NCA90 LIB cells with diverse graphite electrode tortuosities in a high-performance Lamborghini GoKart,paving the way for further advancements in Ni-rich LIB technology.
基金financially supported by the Natural Science Foundation of Henan Province of China(No.222300420252)Nanyang Normal University(Nos.2020ZX013 and 2020ZX014).
文摘Because of their large volume variation and inferior electrical conductivity,Mn_(3)O_(4)-based oxide anode materials have short cyclic lives and poor rate capability,which obstructs their development.In this study,we successfully prepared a Mn_(3)O_(4)/N-doped honeycomb carbon composite using a smart and facile synthetic method.The Mn_(3)O_(4)nanopolyhedra are grown on N-doped honeycomb carbon,which evidently mitigates the volume change in the charging and discharging processes but also improves the electrochemical reaction kinetics.More importantly,the Mn-O-C bond in the Mn_(3)O_(4)/N-doped honeycomb carbon composite benefits electrochemical reversibility.These features of the Mn_(3)O_(4)/N-doped honeycomb carbon(NHC)composite are responsible for its superior electrochemical performance.When used for Li-ion batteries,the Mn_(3)O_(4)/N-doped honeycomb carbon anode exhibits a high reversible capacity of 598 mAh·g^(−1)after 350 cycles at 1 A·g^(−1).Even at 2 A·g^(−1),the Mn_(3)O_(4)/NHC anode still delivers a high capacity of 472 mAh·g^(−1).This work provides a new prospect for synthesizing and developing manganese-based oxide materials for energy storage.
基金financially supported by National Natural Science Foundation of China (No.21701083)。
文摘All solid-state electrolytes have the advantages of good mechanical and thermal properties for safer energy storage,but their energy density has been limited by low ionic conductivity and large interfacial resistance caused by the poor Li~+transport kinetics due to the solid-solid contacts between the electrodes and the solid-state electrolytes.Herein,a novel gel polymer electrolyte(UPP-5)composed of ionic liquid incorporated metal-organic frameworks nanoparticles(IL@MOFs)is designed,it exhibits satisfying electrochemical performances,consisting of an excellent electrochemical stability window(5.5 V)and an improved Li^(+)transference number of 0.52.Moreover,the Li/UPP-5/LiFePO_(4) full cells present an ultra-stable cycling performance at 0.2C for over 100 cycles almost without any decay in capacities.This study might provide new insight to create an effective Li^(+)conductive network for the development of all-solid-state lithium-ion batteries.
基金financial support from the National Natural Science Foundation of China(Grant Nos.51871188 and 51931006)the Fundamental Research Funds for the Central Universities of China(Xiamen University:Nos.20720200068,20720190007 and 20720220074)+2 种基金Guangdong Basic and Applied Basic Research Foundation(No.2021A1515010139)Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(HRTP-[2022]-22)the“Double-First Class”Foundation of Materials Intelligent Manufacturing Discipline of Xiamen University。
文摘The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton(3DIO FCSe-QDs@NC)is elaborately designed for both sulfur cathode and Li metal anode.The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble Li PSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors.Simultaneously,the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites.Taking advantage of these merits,the assembled Li-S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability(a low decay rate of 0.014%over 2,000 cycles at 2C).Remarkably,a promising areal capacity of 8.41 mAh cm^(-2)can be achieved at the sulfur loading up to 8.50 mg cm^(-2)with an ultra-low electrolyte/sulfur ratio of 4.1μL mg^(-1).This work paves the bi-serve host design from systematic experimental and theoretical analysis,which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li-S full batteries.
基金Korea Institute of Energy Technology Evaluation and Planning,Grant/Award Number:20214000000320Samsung Research Funding&Incubation Center of Samsung Electronics,Grant/Award Number:SRFC-MA1901-06。
文摘Realizing a lithium sulfide(Li_(2)S)cathode with both high energy density and a long lifespan requires an innovative cathode design that maximizes electrochemical performance and resists electrode deterioration.Herein,a high-loading Li_(2)S-based cathode with micrometric Li_(2)S particles composed of two-dimensional graphene(Gr)and one-dimensional carbon nanotubes(CNTs)in a compact geometry is developed,and the role of CNTs in stable cycling of high-capacity Li–S batteries is emphasized.In a dimensionally combined carbon matrix,CNTs embedded within the Gr sheets create robust and sustainable electron diffusion pathways while suppressing the passivation of the active carbon surface.As a unique point,during the first charging process,the proposed cathode is fully activated through the direct conversion of Li_(2)S into S_(8) without inducing lithium polysulfide formation.The direct conversion of Li_(2)S into S_(8) in the composite cathode is ubiquitously investigated using the combined study of in situ Raman spectroscopy,in situ optical microscopy,and cryogenic transmission electron microscopy.The composite cathode demonstrates unprecedented electrochemical properties even with a high Li_(2)S loading of 10 mg cm^(–2);in particular,the practical and safe Li–S full cell coupled with a graphite anode shows ultra-long-term cycling stability over 800 cycles.
基金the Innovation-Driven Project of Central South University(2019CX033)the National Natural Science Foundation of China(51904344 and 52172264)the Natural Science Foundation of Hunan Province of China(2021JJ10060 and 2022GK2033)。
文摘The electrolyte integrated with lithium metal anodes is subjected to the issues of interfacial compatibility and stability,which strongly influence the performances of high-energy lithium metal batteries.Here,we report a new electrolyte recipe viz.a moderately concentrated electrolyte comprising of 2.4 M lithium bis(fluorosulfonyl)imide(LiFSI)in a cosolvent mixture of fluorinated ethylene carbonate(FEC)and dimethyl carbonate(DMC)with relatively high ion conductivity.Owing to the preferential decomposition of LiFSI and FEC,an inorganic-rich interphase with abundant Li_(2)O and LiF nanocrystals is formed on lithium metal with improved robustness and ion transfer kinetics,enabling lithium plating/stripping with an extremely low overpotential of~8 mV and the average CE of 97%.When tested in Li||LiFePO_(4) cell,this electrolyte provides long-term cycling with a capacity retention of 98.3%after 1000 cycles at 1 C and an excellent rate performance of 20 C,as well as an areal capacity of 1.35 mA h cm^(-2)at the cathode areal loading of 9 mg cm^(-2).Moreover,the Li||LiFePO_(4) cell exhibits excellent wide-temperature performances(-40~60℃),including long-term cycling stability over 2600 cycles without visible capacity fading at 0℃,as well as extremely high average CEs of 99.6%and 99.8% over 400 cycles under-20℃ and 45℃.
基金supported by the National R&D Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2018M3D1A1058793 and 2021R1A3B1068920)supported by the Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2018M3D1A1058744)the Yonsei Signature Research Cluster Program of 2021 (2021-22-0002)。
文摘To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a strategy to effectively capture soluble lithium polysulfide intermediates and promote their conversion reaction by integrating highly polar metal oxides with catalytically active metals sulfides.However,to fully exploit the outstanding properties of heterostructure-based composites,their detailed structure and interfacial contacts should be designed rationally.Herein,optimally arranged TiO_(2)and MoS_(2)-based heterostructures(TiO_(2)@MoS_(2)) are fabricated on carbon cloth as a multifunctional interlayer to efficiently trap polysulfide intermediates and accelerate their redox kinetics.Owing to the synergistic effects between TiO_(2)and MoS_(2)and the uniform heterointerface distribution that induces the ideally oriented built-in electric field,Li-S batteries with TiO_(2)@MoS_(2)interlayers exhibit high rate capability(601 mA h g^(-1)at 5 C),good cycling stability(capacity-fade rate of 0.067% per cycle over 500 cycles at2 C),and satisfactory areal capacity(5.2 mA h cm^(-2)) under an increased sulfur loading of 5.2 mg cm^(-2).Moreover,by comparing with a MoS_(2)@TiO_(2)interlayer composed of reversely arranged heterostructures,the effect of the built-in electric field’s direction on the electrocatalytic reactions of polysulfide intermediates is thoroughly investigated for the first time.The superior electrocatalytic activities of the rationally arranged TiO_(2)@MoS_(2)interlayer demonstrate the importance of optimizing the built-in electric field of heterostructures for producing high-performance Li-S batteries.
基金supported by the National Natural Science Foundation of China (No.52222311)the Shanghai RisingStar Program (20QA1406600)+2 种基金ChEM,SPST of Shanghai Tech University (#EM02161943)Shanghai Science and Technology Plan (21DZ2260400)Double First-Class Initiative Fund of Shanghai Tech University for supporting
文摘The use of carbonized wood in various functional devices is attracting considerable attention due to its low cost,vertical channels,and high electrical conduction.However,the conventional carbonization method requires a long processing time and an inert atmosphere.Here,a microwave-assisted ultrafast carbonization technique was developed that carbonizes natural wood in seconds without the need for an inert atmosphere,and the obtained aligned-porous carbonized wood provided an excellent electrochemical performance as an anode material for lithium-ion batteries.This ultrafast carbonization technique simultaneously produced ZnO nanoparticles during the carbonization process that were uniformly distributed on the alignedporous carbon.The hierarchical structure of carbonized wood functionalized with ZnO nanoparticles was used as a host for achieving high-performance lithium-sulfur batteries:the highly conductive carbonized wood framework with vertical channels provided good electron transport pathways,and the homogeneously dispersed ZnO nanoparticles effectively adsorbed lithium polysulfide and catalyzed its conversion reactions.In summary,a new method was developed to realize the ultrafast carbonization of biomass materials with decorated metal oxide nanoparticles.
基金supported by the 2022 Yeungnam University Research Grant。
文摘Lithium-sulfur(Li-S)batteries with high energy density are considered promising energy storage devices for the next generation.Nevertheless,the shuttle effect and the passive layer between the separator and the electrodes still seriously affect the cycle stability and life.Herein,a bimetallic Ni-Co metal-organic framework(MOF)with adsorption and catalytic synergism for polysulfides was successfully synthesized as an electrospinning separator sandwich for Li-S batteries.Introducing porous Ni-Co MOF coatings into the separator provides more adsorption catalytic sites for polysulfides,prevents their diffusion to the anode,and enhances sulfur utilization.Consequently,the improved Li-S batteries with a Ni-Co MOF@PAN(NCMP)electrospun separator delivered excellent rate performance and outstanding cycle stability,yielding an ultra-high initial capacity of 1560 mA h g^(-1)at 0.1 C.Notably,remarkable Li-S battery performance with a discharge capacity of 794 mA h g^(-1)(84.1%capacity retention)was obtained after500 cycles,while delivering a low capacity decay rate of 0.032%during long-term cycling(up to 500cycles)at 1 C.Surprisingly,even at the current density of 2 C,the capacity attenuation rate of 2000 cycles is only 0.034%per cycle.In addition,compared with the Celgard separator,the NCMP separator also had high thermal stability(keeping the separator outline at 200℃)that ensured battery safety and excellent electrolyte wettability(73%porosity and 535%electrolyte absorption)and significantly enhanced the ionic conductivity and Li^(+) transfer number,and protected the surface integrity of the anode.
基金supported by the Interdisciplinary Research Project for Young Teachers of USTB (Fundamental Research Funds for the Central Universities) (No.FRFIDRY-21-023)the Beijing Natural Science Foundation (Nos.2194079 and 2222062)the National Natural Science Foundation of China (Nos.52074023 and 52102205)。
文摘Na_(3)V_(2)(PO_(4))_(2)O_(2)F(NVPOF)has received considerable interest as a promising cathode material for sodium-ion batteries because of its high working voltage and good structural/thermal stability.However,the sluggish electrode reaction resulting from its low intrinsic electronic conductivity significantly restricts its electrochemical performance and thus its practical application.Herein,Nb-doped Na_(3)V_(2-x)Nb_(x)(PO_(4))_(2)O_(2)F/graphene(rGO)composites(x=0,0.05,0.1)were prepared using a solvothermal method followed by calcination.Compared to the un-doped NVPOF/r GO,doping V-site with high-valence Nb element(Nb^(5+))(Na_(3)V_(1.95)Nb_(0.05)(PO_(4))_(2)O_(2)F/r GO(NVN05POF/rGO))can result in the generated V4^(+)/V3^(+)mixed-valence,ensuring the lower bandgap and thus the increased intrinsic electronic conductivity.Besides,the expanded lattice space favors the Na^(+)migration.With the structure feature where NVN05POF particles are attached to the rGO sheets,the electrode reaction kinetics is further accelerated owing to the well-constructed electron conductive network.As a consequence,the as-prepared NVN05POF/r GO sample exhibits a high specific capacity of~72 m Ah·g^(-1)at 10C(capacity retention of 65.2%(vs.0.5C))and excellent long-term cycling stability with the capacity fading rate of~0.099%per cycle in 500 cycles at 5C.
基金financially supported by the National Natural Science Foundation of China (Nos.51974222 and 52034011)。
文摘Natural minerals-based energy materials have attracted enormous attention because of the advantages of good materials consistency,high production,environmental friendliness,and low cost.The uniform distribution of grains can effectively inhibit the aggregation of active materials,improving lithium storage performance.In this work,natural graphite is modified by polyvinylpyrrolidone to obtain modified graphite with reduced size and better dispersion.Natural pyrite composite polyvinylpyrrolidone-modified graphite(pyrite/PG)material with uniform particle distribution is obtained by the ball milling process.The subsequent calcination process converts pyrite/PG into Fe_(1-x)Scompounded with polyvinylpyrrolidone-modified graphite(Fe_(1-x)S/PG).The homogeneous grain distributions of active material can facilitate the faster transfer of electrons and promote the efficient utilization of active materials.The as-prepared Fe_(1-x)S/PG electrode exhibits a remarkably reversible specific capacity of 613.0 mAh·g^(-1)at 0.2 A·g^(-1)after 80 cycles and an excellent rate capability of 523.0 mAh·g^(-1)at 5 A·g^(-1).Even at a higher current density of 10 A·g^(-1),it can deliver a specific capacity of 348.0 mAh·g^(-1).Moreover,the dominant pseudocapacitance in redox reactions accounts for the impressive rate and cycling stability.This work provides a low-cost and facile method to fabricate natural mineral-based anode materials and apprise readers about the impact of uniform particle distribution on lithium storage performance.