With the rise of aqueous multivalent rechargeable batteries,inorganic-organic hybrid cathodes have attracted more and more attention due to the complement of each other’s advantages.Herein,a strategy of designing hyb...With the rise of aqueous multivalent rechargeable batteries,inorganic-organic hybrid cathodes have attracted more and more attention due to the complement of each other’s advantages.Herein,a strategy of designing hybrid cathode is adopted for high efficient aqueous zinc-ion batteries(AZIBs).Methylene blue(MB)intercalated vanadium oxide(HVO-MB)was synthesized through sol-gel and ion exchange method.Compared with other organic-inorganic intercalation cathode,not only can the MB intercalation enlarge the HVO interlayer spacing to improve ion mobility,but also provide coordination reactions with the Zn^(2+)to enhance the intrinsic electrochemical reaction kinetics of the hybrid electrode.As a key component for the cathode of AZIBs,HVO-MB contributes a specific capacity of 418 mA h g^(-1) at 0.1 A g^(-1),high rate capability(243 mA h g^(-1) at 5 A g^(-1))and extraordinary stability(88%of capacity retention after 2000cycles at a high current density of 5 A g^(-1))in 3 M Zn(CF_(3)SO_(3))_(2) aqueous electrolyte.The electrochemical kinetics reveals HVO-MB characterized with large pseudocapacitance charge storage behavior due to the fast ion migration provided by the coordination reaction and expanded interlayer distance.Furthermore,a mixed energy storage mechanism involving Zn^(2+)insertion and coordination reaction is confirmed by various ex-situ characterization.Thus,this work opens up a new path for constructing the high performance cathode of AZIBs through organic-inorganic hybridization.展开更多
Potassium-ion batteries(PIBs)are potential“Beyond Li-ion Batteries”candidates for their resource advantage and low standard electrode potential.To date,the research on PIBs is in its early stages,the most urgent tas...Potassium-ion batteries(PIBs)are potential“Beyond Li-ion Batteries”candidates for their resource advantage and low standard electrode potential.To date,the research on PIBs is in its early stages,the most urgent task is to develop high-performance electrode materials and reveal their potassium storage mechanism.For PIBs anode materials,carbon with tunable microstructure,excellent electrochemical activity,nontoxicity and low price is considered as one of the most promising anode materials for commercialization.Although some breakthrough works have emerged,the overall electrochemical performance of the reported carbon anode is still far away from practical application.Herein,we carry out a comprehensive overview of PIBs carbon anode in terms of three aspects of rational design of structure,performance evaluation criteria and characterization of potassium storage mechanism.First,the regulation mechanism of key structural features of carbon anode on its potassium storage performance and the representative structural regulation strategies are introduced.Then,in view of the undefined performance evaluation criteria of PIBs carbon anode,a reference principle for evaluating the potassium storage performance of carbon anode is proposed.Finally,the advanced characterization techniques for the potassium storage mechanism of carbon anode are summarize.This review aims to provide guidance for the development of practical PIBs anode.展开更多
Though secondary aqueous Zn ion batteries(AZIBs)have been received broad concern in recent years,the development of suitable cathode materials of AZIBs is still a big challenge.The MnO_(2) has been deemed as one of mo...Though secondary aqueous Zn ion batteries(AZIBs)have been received broad concern in recent years,the development of suitable cathode materials of AZIBs is still a big challenge.The MnO_(2) has been deemed as one of most hopeful cathode materials of AZIBs on account of some extraordinary merits,such as richly natural resources,low toxicity,high discharge potential,and large theoretical capacity.However,the crystal structure diversity of MnO_(2) results in an obvious various of charge storage mechanisms,which can cause great differences in electrochemical performance.Furthermore,several challenges,including intrinsic poor conductivity,dissolution of manganese and sluggish ion transport dynamics should be conquered before real practice.This work focuses on the reaction mechanisms and recent progress of MnO_(2)-based materials of AZIBs.In this review,a detailed review of the reaction mechanisms and optimal ways for enhancing electrochemical performance for MnO_(2)-based materials is proposed.At last,a number of viewpoints on challenges,future development direction,and foreground of MnO_(2)-based materials of aqueous zinc ions batteries are put forward.This review clarifies reaction mechanism of MnO_(2)-based materials of AZIBs,and offers a new perspective for the future invention in MnO_(2)-based cathode materials,thus accelerate the extensive development and commercialization practice of aqueous zinc ions batteries.展开更多
The pursuit of high-performance electrode materials is highly desired to meet the demand of batteries with high energy and power density.However,a deep understanding of the charge storage mechanism is always challengi...The pursuit of high-performance electrode materials is highly desired to meet the demand of batteries with high energy and power density.However,a deep understanding of the charge storage mechanism is always challenging,which limits the development of advanced electrode materials.Herein,high-resolution mass spectroscopy(HR-MS)is employed to detect the evolution of organic electrode materials during the redox process and reveal the charge storage mechanism,by using small molecular oxamides as an example,which have ortho-carbonyls and are therefore potential electrochemical active materials for batteries.The HR-MS results adequately proved that the oxamides could reversibly store lithium ions in the voltage window of 1.5–3.8 V.Upon deeper reduction,the oxamides would decompose due to the cleavage of the C–N bonds in oxamide structures,which could be proved by the fragments detected by HR-MS,^(1)H NMR,and the generation of NH_(3)after the reduction of oxamide by Li.This work provides a strategy to deeply understand the charge storage mechanism of organic electrode materials and will stimulate the further development of characterization techniques to reveal the charge storage mechanism for developing high-performance electrode materials.展开更多
Aqueous rechargeable zinc-ion batteries(ZIBs)have recently attracted increasing research interest due to their unparalleled safety,fantastic cost competitiveness and promising capacity advantages compared with the com...Aqueous rechargeable zinc-ion batteries(ZIBs)have recently attracted increasing research interest due to their unparalleled safety,fantastic cost competitiveness and promising capacity advantages compared with the commercial lithium ion batteries.However,the disputed energy storage mechanism has been a confusing issue restraining the development of ZIBs.Although a lot of efforts have been dedicated to the exploration in battery chemistry,a comprehensive review that focuses on summarizing the energy storage mechanisms of ZIBs is needed.Herein,the energy storage mechanisms of aqueous rechargeable ZIBs are systematically reviewed in detail and summarized as four types,which are traditional Zn^(2+)insertion chemistry,dual ions co-insertion,chemical conversion reaction and coordination reaction of Zn^(2+)with organic cathodes.Furthermore,the promising exploration directions and rational prospects are also proposed in this review.展开更多
Aqueous Zinc-ion batteries(ZIB) are attracting immense attention because of their merits of excellent safety and quite cheap properties compared with lithium-ion batteries(LIB).Manganese oxide is one of the most impor...Aqueous Zinc-ion batteries(ZIB) are attracting immense attention because of their merits of excellent safety and quite cheap properties compared with lithium-ion batteries(LIB).Manganese oxide is one of the most important cathode materials of ZIB.In this paper,α-Mn2O3 used as cathode of ZIB is synthesized via Metal-Organic Framework(MOF)-derived method,which delivers a high specific capacity of225 mAh g^(-1) at 0.05 A g^(-1) and 92.7 mAh g^(-1) after 1700 cycles at 2 A g^(-1).The charge storage mechanism of α-Mn2O3 cathode is found to greatly depend on the discharge current density.At lower current density discharging,the H+ and Zn2+ are successively intercalated into the α-Mn2O3 before and after the "turning point" of discharge voltage and their discharging products present obviously different morphologies changing from flower-like to large plate-like products.At a higher current density,the low-voltage plateau after the turning point disappears due to the decrease of amount of Zn2+ intercalation and the H+intercalation is dominated in α-Mn2 O3.This study provides significant understanding for future design and research of high-performance Mn-based cathodes of ZIB.展开更多
Hard carbon has been regarded as the most promising anode material for sodiumion batteries(SIBs)due to its low cost,high reversible capacity,and low working potential.However,the uncertain sodium storage mechanism hin...Hard carbon has been regarded as the most promising anode material for sodiumion batteries(SIBs)due to its low cost,high reversible capacity,and low working potential.However,the uncertain sodium storage mechanism hinders the rational design and synthesis of high-performance hard carbon anode materials for practical SIBs.During the past decades,tremendous efforts have been put to stimulate the development of hard carbon materials.In this review,we discuss the recent progress of the study on the sodium storage mechanism of hard carbon anodes,and the effective strategies to improve their sodium storage performance have been summarized.It is anticipated that hard carbon anodes with high electrochemical properties will be inspired and fabricated for large-scale energy storage applications.展开更多
As the number of sensor network application scenarios continues to grow,the security problems inherent in this approach have become obstacles that hinder its wide application.However,it has attracted increasing attent...As the number of sensor network application scenarios continues to grow,the security problems inherent in this approach have become obstacles that hinder its wide application.However,it has attracted increasing attention from industry and academia.The blockchain is based on a distributed network and has the characteristics of non-tampering and traceability of block data.It is thus naturally able to solve the security problems of the sensor networks.Accordingly,this paper first analyzes the security risks associated with data storage in the sensor networks,then proposes using blockchain technology to ensure that data storage in the sensor networks is secure.In the traditional blockchain,the data layer uses a Merkle hash tree to store data;however,the Merkle hash tree cannot provide non-member proof,which makes it unable to resist the attacks of malicious nodes in networks.To solve this problem,this paper utilizes a cryptographic accumulator rather than a Merkle hash tree to provide both member proof and non-member proof.Moreover,the number of elements in the existing accumulator is limited and unable to meet the blockchain’s expansion requirements.This paper therefore proposes a new type of unbounded accumulator and provides its definition and security model.Finally,this paper constructs an unbounded accumulator scheme using bilinear pairs and analyzes its performance.展开更多
As a promising anode material in supercapacitors,vanadium nitride has been widely concerned due to its ultra-high theoretical specific capacitance.However,its routine test capacitance value is still far from the theor...As a promising anode material in supercapacitors,vanadium nitride has been widely concerned due to its ultra-high theoretical specific capacitance.However,its routine test capacitance value is still far from the theoretical value and its energy storage mechanism is controversial.In order to solve these two key problems,here we prepare interplanar spacing expanded vanadium nitride materials with different impurity atoms intercalation from two anionic precursors of vanadium-based metal organic frameworks with different functional groups.The obtained vanadium nitride reaches a higher specific capacitance;and further,through ex situ X-Ray diffraction and in situ Raman,the charge storage of vanadium nitride is contributed by two processes:the first benefit is from the K^(+) de/intercalation in the interplanar spacing,and the other one is derived from the redox reaction with OH−by adsorption on surface.Furthermore,both of the first principle calculation and extended experiments support this idea.We believe that such detailed research on the energy storage mechanism can provide a clear idea for the application of metal nitrides in supercapacitors and other energy storage devices.展开更多
Computational modeling methods,including molecular dynamics(MD)and Monte Carlo(MC)simulations,and density functional theory(DFT),are receiving booming interests for exploring charge storage mechanisms of electrochemic...Computational modeling methods,including molecular dynamics(MD)and Monte Carlo(MC)simulations,and density functional theory(DFT),are receiving booming interests for exploring charge storage mechanisms of electrochemical energy storage devices.These methods can effectively be used to obtain molecular scale local information or provide clear explanations for novel experimental findings that cannot be directly interpreted through experimental investigations.This short review is dedicated to emphasizing recent advances in computational simulation methods for exploring the charge storage mechanisms in typical nanoscale materials,such as nanoporous carbon materials,2 D MXene materials,and metal-organic framework electrodes.Beyond a better understanding of charge storage mechanisms and experimental observations,fast and accurate enough models would be helpful to provide theoretical guidance and experimental basis for the design of new high-performance electrochemical energy storage devices.展开更多
The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical perfo...The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical performance.Herein,metallic Cu_(2)Se encapsulated with N-doped carbon(Cu_(2)Se@NC)was prepared using Cu_(2)O nanocubes as templates through a combination of dopamine polymerization and hightemperature selenization.The unique nanocubic structure and uniform N-doped carbon coating could shorten the ion transport distance,accelerate electron/charge diffusion,and suppress volume variation,ultimately ensuring Cu_(2)Se@NC with excellent electrochemical performance in sodium ion batteries(SIBs)and potassium ion batteries(PIBs).The composite exhibited excellent rate performance(187.7 mA h g^(-1)at 50 A g^(-1)in SIBs and 179.4 mA h g^(-1)at 5 A g^(-1)in PIBs)and cyclic stability(246,8 mA h g^(-1)at 10 A g^(-1)in SIBs over 2500 cycles).The reaction mechanism of intercalation combined with conversion in both SIBs and PIBs was disclosed by in situ X-ray diffraction(XRD)and ex situ transmission electron microscope(TEM).In particular,the final products in PIBs of K_(2)Se and K_(2)Se_(3)species were determined after discharging,which is different from that in SIBs with the final species of Na_(2)Se.The density functional theory calculation showed that carbon induces strong coupling and charge interactions with Cu_(2)Se,leading to the introduction of built-in electric field on heterojunction to improve electron mobility.Significantly,the theoretical calculations discovered that the underlying cause for the relatively superior rate capability in SIBs to that in PIBs is the agile Na~+diffusion with low energy barrier and moderate adsorption energy.These findings offer theoretical support for in-depth understanding of the performance differences of Cu-based materials in different ion storage systems.展开更多
The emerging rocking-chair aqueous zinc-ion battery(AZIB)configuration provides a promising approach for realizing their practical applications by avoiding the critical drawbacks of Zn metal anodes including unsatisfa...The emerging rocking-chair aqueous zinc-ion battery(AZIB)configuration provides a promising approach for realizing their practical applications by avoiding the critical drawbacks of Zn metal anodes including unsatisfactory Coulombic efficiency and low Zn utilization.Therefore,exploiting appropriate insertion-type anodes with fast charge-transfer kinetics is of great importance,and many modifications focusing on the improvement of electron transport and bulk Zn^(2+)diffusion have been proposed.However,the interfacial Zn^(2+)transfer determined by the desolvation process actually dominates the kinetics of overall battery reactions,which is mainly overlooked.Herein,the interlayer structure of Mo S_(2)is rationally co-intercalated with water and ethylene glycol(EG)molecules(Mo S2@EG),giving rise to a fast non-desolvation Zn^(2+)storage mechanism,which is verified by the extraordinarily smaller activation energy of interfacial Zn^(2+)transfer(4.66 k J mol^(-1))compared with that of pristine Mo S_(2)(56.78 k J mol^(-1)).Furthermore,the results of theoretical calculations,in-situ Raman and ex-situ characterizations also indicate the enhanced structural integrity of Mo S2@EG during cycling due to the enlarged interlayer spacing and charge screening effect induced by interlaminar EG molecules.Consequently,the Mo S_(2)@EG anode enables excellent cycling stability of both high-energy-density Mo_S2@EG||PVO(polyaniline intercalated V_(2)O_(5))and high-voltage Mo S2@EG||Na_(3)V_(2)(PO_(4))_2O_(2)F(NVPF)full batteries with neglectable capacity decay at-20℃.展开更多
Cation additives can efficiently enhance the total electrochemical capabilities of zinc-ion hybrid capacitors (ZHCs).However their energy storage mechanisms in zinc-based systems are still under debate.Herein,we modul...Cation additives can efficiently enhance the total electrochemical capabilities of zinc-ion hybrid capacitors (ZHCs).However their energy storage mechanisms in zinc-based systems are still under debate.Herein,we modulate the electrolyte and achieve dual-ion storage by adding magnesium ions.And we assemble several Zn//activated carbon devices with different electrolyte concentrations and investigate their electrochemical reaction dynamic behaviors.The zinc-ion capacitor with Mg^(2+)mixed solution delivers 82 mAh·g^(-1)capacity at 1 A·g^(-1) and maintains 91%of the original capacitance after 10000 cycling.It is superior to the other assembled zinc-ion devices in single-component electrolytes.The finding demonstrates that the double-ion storage mechanism enables the superior rate performance and long cycle lifetime of ZHCs.展开更多
Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn ...Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into d-MnO_(2) nanosheets irreversibly,thus results in a change of the reaction mechanism with Kþion intercalation.However,the low capacity has greatly limited its practical application.Herein,we found that the tetrahedrally-coordinated Co_(2) þions were leached when MnCo_(2)_(4) was equilibrated in 1 mol L^(-1) HCl solution,leading to the formation of layered CoOOH on MnCo_(2)_(4) surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free Co_(6) octahedra.The as-formed CoOOH is stable upon cycling in alkaline electrolyte,exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution,thus enables utilization of the bulk electrode material and realizes enhanced specific capacity as well as facilitated charge transfer and ion diffusion.In general,our work not only offers a feasible approach to deliberate modification of MnCo_(2)_(4)'s surface structure,but also provides an in-depth understanding of its charge storage mechanism,which enables rational design of the spinel oxides with promising charge storage properties.展开更多
Molybdenum disulfide(MoS_(2)),a typical two-dimensional transition metallic layered material,attracts tremendous attentions in the electrochemical energy storage due to its excellent physicochemical properties.However...Molybdenum disulfide(MoS_(2)),a typical two-dimensional transition metallic layered material,attracts tremendous attentions in the electrochemical energy storage due to its excellent physicochemical properties.However,with the deepening of the research and exploration of the lithium storage mechanism of these advanced MoS_(2)-based anode materials,the complex reaction process influenced by internal and external factors hinders the exhaustive understanding of the lithium storage process.To design stable anode material with high performance,it is urgent to review the mechanisms of reported anode materials and summarize the related factors that influence the reaction processes.This review aims to dissect all possible side reactions during charging and discharging process,uncover internal and external factors inducing various anode reactions and finally put forward strategies of controlling high cycling capacity and super-stable lithium storage capability of MoS_(2).This review will be helpful to the design of MoS_(2)-based lithium-ion batteries(LIBs) with excellent cycle performance to enlarge the application fields of these advanced electrochemical energy storage devices.展开更多
Molybdenum oxide(MoO_(3)), with superior features of multi-electrochemical states, high theoretical capacitance, and low cost, is a desirable supercapacitor electrode material but suffers from low conductivity and ins...Molybdenum oxide(MoO_(3)), with superior features of multi-electrochemical states, high theoretical capacitance, and low cost, is a desirable supercapacitor electrode material but suffers from low conductivity and insufficient active sites. The MoO_(3) capacitance can be largely amplified by introducing oxygen(O) vacancies, but the mechanisms at the atomic scale are still ambiguous.Herein, O vacancies are created at the O2 and O3 sites in the MoO_(3) nanobelts by carbonization to maximize the supercapacitance in the MoO_(2.39). The supercapacitive storage is mainly ascribed to the proton adsorption at the O1 sites to create Mo–OH, leading to an expansion of the interlayer spacing along the lattice B-axis. Roughly 98% of the initial supercapacitance is retained after 1000 cycles,due to the reversible change in the interlayer spacing. Our results provide an insight into the oxygen deficiency-related mechanisms of the supercapacitive performance at the atomic scale and devise a facile method to enhance the supercapacitance for energy storage and conversion.展开更多
A new method is proposed to analyze the pore-scale mechanisms and characterization of light oil storage in shale nanopores,which is based on the Hydrocarbon Vapor Adsorption(HVA)and Pore Calculation Model(PCM).First,t...A new method is proposed to analyze the pore-scale mechanisms and characterization of light oil storage in shale nanopores,which is based on the Hydrocarbon Vapor Adsorption(HVA)and Pore Calculation Model(PCM).First,the basic principle of the HVA-PCM method is introduced,and the experimental/mathematical analysis processes are given.Then,the HVA-PCM method is applied to shale samples to analyze the mechanisms and characterization of light oil storage in shale nanopores.The results provide insights into the pore-scale oil storage mechanisms,oil storage structure,oil film thickness,oil distribution within different sized pores,and the oil storage state.Finally,the advantages and limitations of the HVA-PCM method are discussed,and suggestions for further improvement are proposed.Overall,the HVA-PCM method is a powerful tool for extracting quantitative information on the light oil storage in shale nanopores.展开更多
Transition-metal dichalcogenides (TMDs) exhibit immense potential as lithium/ sodium-ion electrode materials owing to their sandwich-like layered structures. To optimize their lithium/sodium-storage performance, two...Transition-metal dichalcogenides (TMDs) exhibit immense potential as lithium/ sodium-ion electrode materials owing to their sandwich-like layered structures. To optimize their lithium/sodium-storage performance, two issues should be addressed: fundamentally understanding the chemical reaction occurring in TMD electrodes and developing novel TMDs. In this study, WSe2 hexagonal nanoplates were synthesized as lithium/sodium-ion battery (LIB/SIB) electrode materials. For LIBs, the WSe2-nanoplate electrodes achieved a stable reversible capacity and a high rate capability, as well as an ultralong cycle life of up to 1,500 cycles at 1,000 mA·g^-1. Most importantly, in situ Raman spectroscopy, ex situ X-ray diffraction (XRD), transmission electron microscopy, and electrochemical impedance spectroscopy measurements performed during the discharge-charge process clearly verified the reversible conversion mechanism, which can be summarized as follows: WSe2 + 4Li^+ + 4e^- ←→ W + 2Li2Se. The WSe2 nanoplates also exhibited excellent cycling performance and a high rate capability as SIB electrodes. Ex situ XRD and Raman spectroscopy results demonstrate that WSe2 reacted with Na^+ more easily and thoroughly than with Li^+ and converted to Na2Se and tungsten in the Ist sodiated state. The subsequent charging reaction can be expressed as Na2Se → Se + 2Na^++ 2e^-, which differs from the traditional conversion mechanism for LIBs. To our knowledge, this is the first systematic exploration of the lithium/sodium-storage performance of WSe2 and the mechanism involved.展开更多
Rechargeable aluminum batteries(RABs)have attracted great interest as one of the most promising candidates for large-scale energy storage because of their high volumetric capacity,low cost,high safety and the abundanc...Rechargeable aluminum batteries(RABs)have attracted great interest as one of the most promising candidates for large-scale energy storage because of their high volumetric capacity,low cost,high safety and the abundance of aluminum.However,compared with the aluminum anodes,the cathode materials face more problems including low specific capacity,relatively sluggish kinetics in most host structures and/or limited cycle lifespan,which pose the major challenge for RABs in further practical applications.During the past years,intensive efforts have been devoted to developing new cathode materials and/or designing engineered nanostructures to greatly improve RABs’electrochemical performances.In addition to nanotechnologybased electrode structure designs,the intrinsic chemical structures and charge storage mechanisms of cathode materials play an equally crucial role,if not more,in revolutionizing the battery performances.This review,here,focuses on current understandings into the charge storage mechanisms of cathode materials in RABs from a chemical reaction point of view.First,the fundamental chemistry,charge storage mechanisms and design principles of RAB cathode materials are highlighted.Based on different ion charge carriers,the current cathode materials are classified into four groups,including Al^(3+)-hosting,Al Cl_(4)^(-)-hosting,Al Cl_(2)^(+)/Al Cl_(2)^(+)-hosting,and Cl^(-)-hosting cathode materials.Next,the respective typical electrode structures,optimization strategies,electrochemical performances and charge storage mechanisms are discussed in detail to establish their chemistry-structure-property relationships.This review on current understandings of the cathode charge storage mechanisms will lay the ground and hopefully set new directions into the rational design of high-performance cathode materials in RABs,and open up new opportunities for designing new electrolyte systems with respect to the targeted cathode systems.展开更多
Besides lithium-ion batteries, it is imperative to develop new battery energystorage system with high energy density. In conjunction with the developmentof Li-S batteries, emerging sulfur-containing polymers with tuna...Besides lithium-ion batteries, it is imperative to develop new battery energystorage system with high energy density. In conjunction with the developmentof Li-S batteries, emerging sulfur-containing polymers with tunable sulfur-chain length and organic groups gradually attract much attention as cathodematerials. This can avoid the problems that are impeding the development ofthe typical Li-S batteries, such as volume expansion, active material dissolu-tion, shuttle effect, and so on. This review aims to generalize the type ofsulfur-containing polymers and the working principles in Li-S batteries. Thesulfur-containing polymers (R-Sn-R) with different sulfur-chain length (n > 6,n ≤ 2, and 3 ≤ n ≤ 6) are summarized. It also discusses several organic groupssuch as phenyl rings, N-heterocycles, and unique structure with cross-linkednetworks and multi-micropores skeleton. This review also explores other strat-egies of sulfur-containing polymers in the rest of Li-S batteries, providing asummary of the advantages of sulfur-containing polymers, recent develop-ment, in-depth discussion of the mechanism in Li-S batteries, and organicgroup-structure-performance relationship. This review would have guidelinesfor future development of sulfur-containing polymers in Li-S batteries.展开更多
基金supported by the National Natural Science Foundation of China(21965027 and 22065030)the Natural Science Foundation of Ningxia Province(2022AAC03109)the National First-rate Discipline Construction Project of Ningxia:Chemical Engineering and Technology(NXY-LXK2017A04)。
文摘With the rise of aqueous multivalent rechargeable batteries,inorganic-organic hybrid cathodes have attracted more and more attention due to the complement of each other’s advantages.Herein,a strategy of designing hybrid cathode is adopted for high efficient aqueous zinc-ion batteries(AZIBs).Methylene blue(MB)intercalated vanadium oxide(HVO-MB)was synthesized through sol-gel and ion exchange method.Compared with other organic-inorganic intercalation cathode,not only can the MB intercalation enlarge the HVO interlayer spacing to improve ion mobility,but also provide coordination reactions with the Zn^(2+)to enhance the intrinsic electrochemical reaction kinetics of the hybrid electrode.As a key component for the cathode of AZIBs,HVO-MB contributes a specific capacity of 418 mA h g^(-1) at 0.1 A g^(-1),high rate capability(243 mA h g^(-1) at 5 A g^(-1))and extraordinary stability(88%of capacity retention after 2000cycles at a high current density of 5 A g^(-1))in 3 M Zn(CF_(3)SO_(3))_(2) aqueous electrolyte.The electrochemical kinetics reveals HVO-MB characterized with large pseudocapacitance charge storage behavior due to the fast ion migration provided by the coordination reaction and expanded interlayer distance.Furthermore,a mixed energy storage mechanism involving Zn^(2+)insertion and coordination reaction is confirmed by various ex-situ characterization.Thus,this work opens up a new path for constructing the high performance cathode of AZIBs through organic-inorganic hybridization.
基金supported financially by the National Key Research and Development Program of China (Grants No. 2017YFA0206301)the National Natural Science Foundation of China (Grants No. 51631001 and 51631001)the China-Germany Collaboration Project (Grants No. M-0199)
文摘Potassium-ion batteries(PIBs)are potential“Beyond Li-ion Batteries”candidates for their resource advantage and low standard electrode potential.To date,the research on PIBs is in its early stages,the most urgent task is to develop high-performance electrode materials and reveal their potassium storage mechanism.For PIBs anode materials,carbon with tunable microstructure,excellent electrochemical activity,nontoxicity and low price is considered as one of the most promising anode materials for commercialization.Although some breakthrough works have emerged,the overall electrochemical performance of the reported carbon anode is still far away from practical application.Herein,we carry out a comprehensive overview of PIBs carbon anode in terms of three aspects of rational design of structure,performance evaluation criteria and characterization of potassium storage mechanism.First,the regulation mechanism of key structural features of carbon anode on its potassium storage performance and the representative structural regulation strategies are introduced.Then,in view of the undefined performance evaluation criteria of PIBs carbon anode,a reference principle for evaluating the potassium storage performance of carbon anode is proposed.Finally,the advanced characterization techniques for the potassium storage mechanism of carbon anode are summarize.This review aims to provide guidance for the development of practical PIBs anode.
基金supported by the National Natural Science Foundation of China(U1960107)the Natural Science Foundation of Hebei Province(E2022501014)+4 种基金the"333"Talent Project of Hebei Province(A202005018)the Fundamental Research Funds for the Central Universities(N2123001)the Science and Technology Research Youth Fund Project of Higher Education Institutions of Hebei Province(QN2022196)the 2023 Hebei Provincial Postgraduate Student Innovation Ability training funding project(CXZZSS2023196)the Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(22567627H)。
文摘Though secondary aqueous Zn ion batteries(AZIBs)have been received broad concern in recent years,the development of suitable cathode materials of AZIBs is still a big challenge.The MnO_(2) has been deemed as one of most hopeful cathode materials of AZIBs on account of some extraordinary merits,such as richly natural resources,low toxicity,high discharge potential,and large theoretical capacity.However,the crystal structure diversity of MnO_(2) results in an obvious various of charge storage mechanisms,which can cause great differences in electrochemical performance.Furthermore,several challenges,including intrinsic poor conductivity,dissolution of manganese and sluggish ion transport dynamics should be conquered before real practice.This work focuses on the reaction mechanisms and recent progress of MnO_(2)-based materials of AZIBs.In this review,a detailed review of the reaction mechanisms and optimal ways for enhancing electrochemical performance for MnO_(2)-based materials is proposed.At last,a number of viewpoints on challenges,future development direction,and foreground of MnO_(2)-based materials of aqueous zinc ions batteries are put forward.This review clarifies reaction mechanism of MnO_(2)-based materials of AZIBs,and offers a new perspective for the future invention in MnO_(2)-based cathode materials,thus accelerate the extensive development and commercialization practice of aqueous zinc ions batteries.
基金financialy supported by the National Natural Science Foundation of China(52173163,22279038,and 22205069)the National 1000-Talents Program,the Innovation Fund of WNLO,the Open Fund of the State Key Laboratory of Integrated Optoelectronics(IOSKL2020KF02)+1 种基金Wenzhou Science&Technology Bureau(ZG2022020,G20220022,and G20220026)the China Postdoctoral Science Foundation(2021TQ0115,2021 M701302,and 2020 M672323)
文摘The pursuit of high-performance electrode materials is highly desired to meet the demand of batteries with high energy and power density.However,a deep understanding of the charge storage mechanism is always challenging,which limits the development of advanced electrode materials.Herein,high-resolution mass spectroscopy(HR-MS)is employed to detect the evolution of organic electrode materials during the redox process and reveal the charge storage mechanism,by using small molecular oxamides as an example,which have ortho-carbonyls and are therefore potential electrochemical active materials for batteries.The HR-MS results adequately proved that the oxamides could reversibly store lithium ions in the voltage window of 1.5–3.8 V.Upon deeper reduction,the oxamides would decompose due to the cleavage of the C–N bonds in oxamide structures,which could be proved by the fragments detected by HR-MS,^(1)H NMR,and the generation of NH_(3)after the reduction of oxamide by Li.This work provides a strategy to deeply understand the charge storage mechanism of organic electrode materials and will stimulate the further development of characterization techniques to reveal the charge storage mechanism for developing high-performance electrode materials.
基金supported by the National Natural Science Foundation of China(21571080)。
文摘Aqueous rechargeable zinc-ion batteries(ZIBs)have recently attracted increasing research interest due to their unparalleled safety,fantastic cost competitiveness and promising capacity advantages compared with the commercial lithium ion batteries.However,the disputed energy storage mechanism has been a confusing issue restraining the development of ZIBs.Although a lot of efforts have been dedicated to the exploration in battery chemistry,a comprehensive review that focuses on summarizing the energy storage mechanisms of ZIBs is needed.Herein,the energy storage mechanisms of aqueous rechargeable ZIBs are systematically reviewed in detail and summarized as four types,which are traditional Zn^(2+)insertion chemistry,dual ions co-insertion,chemical conversion reaction and coordination reaction of Zn^(2+)with organic cathodes.Furthermore,the promising exploration directions and rational prospects are also proposed in this review.
基金supported by the National Natural Science Foundation of China (51672156)Local Innovative Research Teams Project of Guangdong Pearl River Talents Program (No. 2017BT01N111)+2 种基金Guangdong Province Technical Plan Project (2017B010119001)Shenzhen Technical Plan Project (JCYJ20170817161221958 and JCYJ20170412170706047)Shenzhen Graphene Manufacturing Innovation Center (201901161513)。
文摘Aqueous Zinc-ion batteries(ZIB) are attracting immense attention because of their merits of excellent safety and quite cheap properties compared with lithium-ion batteries(LIB).Manganese oxide is one of the most important cathode materials of ZIB.In this paper,α-Mn2O3 used as cathode of ZIB is synthesized via Metal-Organic Framework(MOF)-derived method,which delivers a high specific capacity of225 mAh g^(-1) at 0.05 A g^(-1) and 92.7 mAh g^(-1) after 1700 cycles at 2 A g^(-1).The charge storage mechanism of α-Mn2O3 cathode is found to greatly depend on the discharge current density.At lower current density discharging,the H+ and Zn2+ are successively intercalated into the α-Mn2O3 before and after the "turning point" of discharge voltage and their discharging products present obviously different morphologies changing from flower-like to large plate-like products.At a higher current density,the low-voltage plateau after the turning point disappears due to the decrease of amount of Zn2+ intercalation and the H+intercalation is dominated in α-Mn2 O3.This study provides significant understanding for future design and research of high-performance Mn-based cathodes of ZIB.
基金Key Research Program of Hubei Province,Grant/Award Number:2020BAA030National Nature Science Foundation of China,Grant/Award Number:U20A20249 and 21972108。
文摘Hard carbon has been regarded as the most promising anode material for sodiumion batteries(SIBs)due to its low cost,high reversible capacity,and low working potential.However,the uncertain sodium storage mechanism hinders the rational design and synthesis of high-performance hard carbon anode materials for practical SIBs.During the past decades,tremendous efforts have been put to stimulate the development of hard carbon materials.In this review,we discuss the recent progress of the study on the sodium storage mechanism of hard carbon anodes,and the effective strategies to improve their sodium storage performance have been summarized.It is anticipated that hard carbon anodes with high electrochemical properties will be inspired and fabricated for large-scale energy storage applications.
基金supported by the NSFC(61772454)the Researchers Supporting Project No.RSP-2020/102 King Saud University,Riyadh,Saudi Arabiafunded by National Key Research and Development Program of China(2019YFC1511000).
文摘As the number of sensor network application scenarios continues to grow,the security problems inherent in this approach have become obstacles that hinder its wide application.However,it has attracted increasing attention from industry and academia.The blockchain is based on a distributed network and has the characteristics of non-tampering and traceability of block data.It is thus naturally able to solve the security problems of the sensor networks.Accordingly,this paper first analyzes the security risks associated with data storage in the sensor networks,then proposes using blockchain technology to ensure that data storage in the sensor networks is secure.In the traditional blockchain,the data layer uses a Merkle hash tree to store data;however,the Merkle hash tree cannot provide non-member proof,which makes it unable to resist the attacks of malicious nodes in networks.To solve this problem,this paper utilizes a cryptographic accumulator rather than a Merkle hash tree to provide both member proof and non-member proof.Moreover,the number of elements in the existing accumulator is limited and unable to meet the blockchain’s expansion requirements.This paper therefore proposes a new type of unbounded accumulator and provides its definition and security model.Finally,this paper constructs an unbounded accumulator scheme using bilinear pairs and analyzes its performance.
基金supported by the National Natural Science Foundation of China(51763014 and 52073133)Joint fund between Shenyang National Laboratory for Materials Science and State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals(18LHPY002)the Program for Hongliu Distinguished Young Scholars in Lanzhou University of Technology。
文摘As a promising anode material in supercapacitors,vanadium nitride has been widely concerned due to its ultra-high theoretical specific capacitance.However,its routine test capacitance value is still far from the theoretical value and its energy storage mechanism is controversial.In order to solve these two key problems,here we prepare interplanar spacing expanded vanadium nitride materials with different impurity atoms intercalation from two anionic precursors of vanadium-based metal organic frameworks with different functional groups.The obtained vanadium nitride reaches a higher specific capacitance;and further,through ex situ X-Ray diffraction and in situ Raman,the charge storage of vanadium nitride is contributed by two processes:the first benefit is from the K^(+) de/intercalation in the interplanar spacing,and the other one is derived from the redox reaction with OH−by adsorption on surface.Furthermore,both of the first principle calculation and extended experiments support this idea.We believe that such detailed research on the energy storage mechanism can provide a clear idea for the application of metal nitrides in supercapacitors and other energy storage devices.
基金funding from the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation program(grant agreement no.714581)supported by the Fundamental Research Funds for the Central Universities(No.YJ201886)+1 种基金the National Natural Science Foundation of China(No.501902215)Sichuan Science and Technology Program(No.2020ZDZX0005)
文摘Computational modeling methods,including molecular dynamics(MD)and Monte Carlo(MC)simulations,and density functional theory(DFT),are receiving booming interests for exploring charge storage mechanisms of electrochemical energy storage devices.These methods can effectively be used to obtain molecular scale local information or provide clear explanations for novel experimental findings that cannot be directly interpreted through experimental investigations.This short review is dedicated to emphasizing recent advances in computational simulation methods for exploring the charge storage mechanisms in typical nanoscale materials,such as nanoporous carbon materials,2 D MXene materials,and metal-organic framework electrodes.Beyond a better understanding of charge storage mechanisms and experimental observations,fast and accurate enough models would be helpful to provide theoretical guidance and experimental basis for the design of new high-performance electrochemical energy storage devices.
基金The Natural Science Foundation of Henan Province(222300420083)the Opening Foundation of State Key Laboratory of Chemistry and Utilization of Carbon-based Energy Resource of Xinjiang University(KFKT2021004)。
文摘The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical performance.Herein,metallic Cu_(2)Se encapsulated with N-doped carbon(Cu_(2)Se@NC)was prepared using Cu_(2)O nanocubes as templates through a combination of dopamine polymerization and hightemperature selenization.The unique nanocubic structure and uniform N-doped carbon coating could shorten the ion transport distance,accelerate electron/charge diffusion,and suppress volume variation,ultimately ensuring Cu_(2)Se@NC with excellent electrochemical performance in sodium ion batteries(SIBs)and potassium ion batteries(PIBs).The composite exhibited excellent rate performance(187.7 mA h g^(-1)at 50 A g^(-1)in SIBs and 179.4 mA h g^(-1)at 5 A g^(-1)in PIBs)and cyclic stability(246,8 mA h g^(-1)at 10 A g^(-1)in SIBs over 2500 cycles).The reaction mechanism of intercalation combined with conversion in both SIBs and PIBs was disclosed by in situ X-ray diffraction(XRD)and ex situ transmission electron microscope(TEM).In particular,the final products in PIBs of K_(2)Se and K_(2)Se_(3)species were determined after discharging,which is different from that in SIBs with the final species of Na_(2)Se.The density functional theory calculation showed that carbon induces strong coupling and charge interactions with Cu_(2)Se,leading to the introduction of built-in electric field on heterojunction to improve electron mobility.Significantly,the theoretical calculations discovered that the underlying cause for the relatively superior rate capability in SIBs to that in PIBs is the agile Na~+diffusion with low energy barrier and moderate adsorption energy.These findings offer theoretical support for in-depth understanding of the performance differences of Cu-based materials in different ion storage systems.
基金supported by the National Natural Science Foundation of China(22109030,22021001)the Fundamental Research Funds for the Central Universities(20720220073)+3 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Fujian Industrial Technology Development and Application Plan(2022I0002)the Guangdong Basic and Applied Basic Research Foundation(2019A1515111069,2021A1515010177)the financial support from Guangdong Basic and Applied Basic Research Foundation(2020A1515010886)。
文摘The emerging rocking-chair aqueous zinc-ion battery(AZIB)configuration provides a promising approach for realizing their practical applications by avoiding the critical drawbacks of Zn metal anodes including unsatisfactory Coulombic efficiency and low Zn utilization.Therefore,exploiting appropriate insertion-type anodes with fast charge-transfer kinetics is of great importance,and many modifications focusing on the improvement of electron transport and bulk Zn^(2+)diffusion have been proposed.However,the interfacial Zn^(2+)transfer determined by the desolvation process actually dominates the kinetics of overall battery reactions,which is mainly overlooked.Herein,the interlayer structure of Mo S_(2)is rationally co-intercalated with water and ethylene glycol(EG)molecules(Mo S2@EG),giving rise to a fast non-desolvation Zn^(2+)storage mechanism,which is verified by the extraordinarily smaller activation energy of interfacial Zn^(2+)transfer(4.66 k J mol^(-1))compared with that of pristine Mo S_(2)(56.78 k J mol^(-1)).Furthermore,the results of theoretical calculations,in-situ Raman and ex-situ characterizations also indicate the enhanced structural integrity of Mo S2@EG during cycling due to the enlarged interlayer spacing and charge screening effect induced by interlaminar EG molecules.Consequently,the Mo S_(2)@EG anode enables excellent cycling stability of both high-energy-density Mo_S2@EG||PVO(polyaniline intercalated V_(2)O_(5))and high-voltage Mo S2@EG||Na_(3)V_(2)(PO_(4))_2O_(2)F(NVPF)full batteries with neglectable capacity decay at-20℃.
基金financially supported by the National Natural Science Foundation of China (No.52172218)。
文摘Cation additives can efficiently enhance the total electrochemical capabilities of zinc-ion hybrid capacitors (ZHCs).However their energy storage mechanisms in zinc-based systems are still under debate.Herein,we modulate the electrolyte and achieve dual-ion storage by adding magnesium ions.And we assemble several Zn//activated carbon devices with different electrolyte concentrations and investigate their electrochemical reaction dynamic behaviors.The zinc-ion capacitor with Mg^(2+)mixed solution delivers 82 mAh·g^(-1)capacity at 1 A·g^(-1) and maintains 91%of the original capacitance after 10000 cycling.It is superior to the other assembled zinc-ion devices in single-component electrolytes.The finding demonstrates that the double-ion storage mechanism enables the superior rate performance and long cycle lifetime of ZHCs.
基金supported by the National Key Research and Development Program of China(2022YFE0206300)the National Natural Science Foundation of China(22209047,U21A2081,22075074)+2 种基金Natural Science Foundation of Hunan Province(2020JJ5035)Hunan Provincial Department of Education Outstanding Youth Project(23B0037)Macao Science and Technology Development Fund(Macao SAR,FDCT-0096/2020/A2).
文摘Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into d-MnO_(2) nanosheets irreversibly,thus results in a change of the reaction mechanism with Kþion intercalation.However,the low capacity has greatly limited its practical application.Herein,we found that the tetrahedrally-coordinated Co_(2) þions were leached when MnCo_(2)_(4) was equilibrated in 1 mol L^(-1) HCl solution,leading to the formation of layered CoOOH on MnCo_(2)_(4) surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free Co_(6) octahedra.The as-formed CoOOH is stable upon cycling in alkaline electrolyte,exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution,thus enables utilization of the bulk electrode material and realizes enhanced specific capacity as well as facilitated charge transfer and ion diffusion.In general,our work not only offers a feasible approach to deliberate modification of MnCo_(2)_(4)'s surface structure,but also provides an in-depth understanding of its charge storage mechanism,which enables rational design of the spinel oxides with promising charge storage properties.
基金financially supported by the National Funds for Distinguished Young Scientists (No. 61825503)the National Natural Science Foundation of China (Nos. 51902101, 61775101,61804082)+3 种基金the Youth Natural Science Foundation of Hunan Province (No. 2019JJ50044)Natural Science Foundation of Jiangsu Province (No. BK20201381)Science Foundation of Nanjing University of Posts and Telecommunications (No. NY219144)China Postdoctoral Science Foundation (Nos. 2020TQ0202, 2021M692161)。
文摘Molybdenum disulfide(MoS_(2)),a typical two-dimensional transition metallic layered material,attracts tremendous attentions in the electrochemical energy storage due to its excellent physicochemical properties.However,with the deepening of the research and exploration of the lithium storage mechanism of these advanced MoS_(2)-based anode materials,the complex reaction process influenced by internal and external factors hinders the exhaustive understanding of the lithium storage process.To design stable anode material with high performance,it is urgent to review the mechanisms of reported anode materials and summarize the related factors that influence the reaction processes.This review aims to dissect all possible side reactions during charging and discharging process,uncover internal and external factors inducing various anode reactions and finally put forward strategies of controlling high cycling capacity and super-stable lithium storage capability of MoS_(2).This review will be helpful to the design of MoS_(2)-based lithium-ion batteries(LIBs) with excellent cycle performance to enlarge the application fields of these advanced electrochemical energy storage devices.
基金financially supported by the Hong Kong Baptist University(No.RMGS-2019-1-03A)。
文摘Molybdenum oxide(MoO_(3)), with superior features of multi-electrochemical states, high theoretical capacitance, and low cost, is a desirable supercapacitor electrode material but suffers from low conductivity and insufficient active sites. The MoO_(3) capacitance can be largely amplified by introducing oxygen(O) vacancies, but the mechanisms at the atomic scale are still ambiguous.Herein, O vacancies are created at the O2 and O3 sites in the MoO_(3) nanobelts by carbonization to maximize the supercapacitance in the MoO_(2.39). The supercapacitive storage is mainly ascribed to the proton adsorption at the O1 sites to create Mo–OH, leading to an expansion of the interlayer spacing along the lattice B-axis. Roughly 98% of the initial supercapacitance is retained after 1000 cycles,due to the reversible change in the interlayer spacing. Our results provide an insight into the oxygen deficiency-related mechanisms of the supercapacitive performance at the atomic scale and devise a facile method to enhance the supercapacitance for energy storage and conversion.
基金supported by the National Natural Science Foundation of China(Grant Nos.41872124,1972132,42072174,41730421,and 41972132)the Open Foundation of provincial and ministerial Key Laboratory of China University of Geosciences(Beijing)(Grant No.20210104)。
文摘A new method is proposed to analyze the pore-scale mechanisms and characterization of light oil storage in shale nanopores,which is based on the Hydrocarbon Vapor Adsorption(HVA)and Pore Calculation Model(PCM).First,the basic principle of the HVA-PCM method is introduced,and the experimental/mathematical analysis processes are given.Then,the HVA-PCM method is applied to shale samples to analyze the mechanisms and characterization of light oil storage in shale nanopores.The results provide insights into the pore-scale oil storage mechanisms,oil storage structure,oil film thickness,oil distribution within different sized pores,and the oil storage state.Finally,the advantages and limitations of the HVA-PCM method are discussed,and suggestions for further improvement are proposed.Overall,the HVA-PCM method is a powerful tool for extracting quantitative information on the light oil storage in shale nanopores.
基金The authors gratefully acknowledge financial support by National Natural Science Foundation of China (Nos. 51371106 and 51671115), and Young Tip-top Talent Support Project (the Organization Department of the Central Committee of the CPC).
文摘Transition-metal dichalcogenides (TMDs) exhibit immense potential as lithium/ sodium-ion electrode materials owing to their sandwich-like layered structures. To optimize their lithium/sodium-storage performance, two issues should be addressed: fundamentally understanding the chemical reaction occurring in TMD electrodes and developing novel TMDs. In this study, WSe2 hexagonal nanoplates were synthesized as lithium/sodium-ion battery (LIB/SIB) electrode materials. For LIBs, the WSe2-nanoplate electrodes achieved a stable reversible capacity and a high rate capability, as well as an ultralong cycle life of up to 1,500 cycles at 1,000 mA·g^-1. Most importantly, in situ Raman spectroscopy, ex situ X-ray diffraction (XRD), transmission electron microscopy, and electrochemical impedance spectroscopy measurements performed during the discharge-charge process clearly verified the reversible conversion mechanism, which can be summarized as follows: WSe2 + 4Li^+ + 4e^- ←→ W + 2Li2Se. The WSe2 nanoplates also exhibited excellent cycling performance and a high rate capability as SIB electrodes. Ex situ XRD and Raman spectroscopy results demonstrate that WSe2 reacted with Na^+ more easily and thoroughly than with Li^+ and converted to Na2Se and tungsten in the Ist sodiated state. The subsequent charging reaction can be expressed as Na2Se → Se + 2Na^++ 2e^-, which differs from the traditional conversion mechanism for LIBs. To our knowledge, this is the first systematic exploration of the lithium/sodium-storage performance of WSe2 and the mechanism involved.
基金supported by the National Natural Science Foundation of China(22075002)National Postdoctoral Program for Innovative Talents(BX2021002)the China Postdoctoral Science Foundation(2021M690194)。
文摘Rechargeable aluminum batteries(RABs)have attracted great interest as one of the most promising candidates for large-scale energy storage because of their high volumetric capacity,low cost,high safety and the abundance of aluminum.However,compared with the aluminum anodes,the cathode materials face more problems including low specific capacity,relatively sluggish kinetics in most host structures and/or limited cycle lifespan,which pose the major challenge for RABs in further practical applications.During the past years,intensive efforts have been devoted to developing new cathode materials and/or designing engineered nanostructures to greatly improve RABs’electrochemical performances.In addition to nanotechnologybased electrode structure designs,the intrinsic chemical structures and charge storage mechanisms of cathode materials play an equally crucial role,if not more,in revolutionizing the battery performances.This review,here,focuses on current understandings into the charge storage mechanisms of cathode materials in RABs from a chemical reaction point of view.First,the fundamental chemistry,charge storage mechanisms and design principles of RAB cathode materials are highlighted.Based on different ion charge carriers,the current cathode materials are classified into four groups,including Al^(3+)-hosting,Al Cl_(4)^(-)-hosting,Al Cl_(2)^(+)/Al Cl_(2)^(+)-hosting,and Cl^(-)-hosting cathode materials.Next,the respective typical electrode structures,optimization strategies,electrochemical performances and charge storage mechanisms are discussed in detail to establish their chemistry-structure-property relationships.This review on current understandings of the cathode charge storage mechanisms will lay the ground and hopefully set new directions into the rational design of high-performance cathode materials in RABs,and open up new opportunities for designing new electrolyte systems with respect to the targeted cathode systems.
基金Program for Hongliu Distinguished Young Scholars in Lanzhou University of TechnologyState Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals,Grant/Award Number:18LHPY002+1 种基金Shenyang National Laboratory for Materials ScienceNational Natural Science Foundation of China,Grant/Award Numbers:52073133,51763014。
文摘Besides lithium-ion batteries, it is imperative to develop new battery energystorage system with high energy density. In conjunction with the developmentof Li-S batteries, emerging sulfur-containing polymers with tunable sulfur-chain length and organic groups gradually attract much attention as cathodematerials. This can avoid the problems that are impeding the development ofthe typical Li-S batteries, such as volume expansion, active material dissolu-tion, shuttle effect, and so on. This review aims to generalize the type ofsulfur-containing polymers and the working principles in Li-S batteries. Thesulfur-containing polymers (R-Sn-R) with different sulfur-chain length (n > 6,n ≤ 2, and 3 ≤ n ≤ 6) are summarized. It also discusses several organic groupssuch as phenyl rings, N-heterocycles, and unique structure with cross-linkednetworks and multi-micropores skeleton. This review also explores other strat-egies of sulfur-containing polymers in the rest of Li-S batteries, providing asummary of the advantages of sulfur-containing polymers, recent develop-ment, in-depth discussion of the mechanism in Li-S batteries, and organicgroup-structure-performance relationship. This review would have guidelinesfor future development of sulfur-containing polymers in Li-S batteries.