Although significant progress has been made in many aspects of the emerging aprotic Li-O2 battery system, an indepth understanding of the oxygen reactions is still underway. The oxygen reactions occurring in the posit...Although significant progress has been made in many aspects of the emerging aprotic Li-O2 battery system, an indepth understanding of the oxygen reactions is still underway. The oxygen reactions occurring in the positive electrode distinguish Li-O2 batteries from the conventional Li-ion cells and play a crucial role in the Li-O2 cell＇s performance （capacity, rate capability, and cycle life）. Recent advances in fundamental studies of oxygen reactions in aprotic Li-O2 batteries are reviewed, including the reaction route, kinetics, morphological evolution of Li2O2, and charge transport within Li2O2. Prospects are also provided for future fundamental investigations of Li-O2 chemistry.展开更多
Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy density.However,due to the difficulty of decomposition of Li2 O2,Li-O2 batteries have high charge overpotential and poor cycling life....Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy density.However,due to the difficulty of decomposition of Li2 O2,Li-O2 batteries have high charge overpotential and poor cycling life.So all kinds of catalysts have been studied on the cathode.Compared to heterogeneous solid catalysts,soluble catalysts achieve faster and more effective transport of electrons by reversible redox pairs.Here,we first report ruthenocene(Ruc) as a mobile redox mediator in a Li-O2 battery.0.01 mol/L Ruc in the electrolyte effectively reduces the charging voltage by 610 mV.Additionally,Ruc greatly increases the cycling life by four-fold(up to 83 cycles) with a simple ketjen black(KB) cathode.The results of SEM,XPS and XRD confirm that less discharge product residue accumulated after recharge.To verify the reaction mechanisms of the mediato r,free energy profiles of the possible reaction pathways based on DFT are provided.展开更多
As one of the next-generation energy-storage devices,Li-O_2 battery has become the main research direction for the academic researchers due to its characteristics of environmental friendship,relatively simple structur...As one of the next-generation energy-storage devices,Li-O_2 battery has become the main research direction for the academic researchers due to its characteristics of environmental friendship,relatively simple structures,high energy density of 3500Wh/kg and low cost.However,Li-O_2 battery cannot be commercialized on a large scale because of the challenging issues including high-efficient electrocatalysts,membranes,Li-based anode and so on.In this review,we focused on the recent development of electrocatalyst materials as cathodes for the non-aqueous Li-O_2 batteries which are relatively simpler than other Li-O_2 batteries＇ structures.Electrocatalysts were summarized including noble metals,nanocarbon materials,transition metals and their hybrids.We points out that the challenges of preparation high-efficient catalysts not only require high catalytic activity and conductivity,but also have novel nanoarchitectures with large interface and porous volume for LiO_x storage.Furthermore,the further investigation of reaction mechanism and advanced in situ analysis technologies are welcome in the coming work.展开更多
Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X...Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.展开更多
We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-...We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.展开更多
Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a no...Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.展开更多
As a high-energy-density primary battery,the Li-SOCl_(2) battery offers significant advantages over other primary systems,including a high operating voltage,wide temperature tolerance,and low self-discharge rate.Howev...As a high-energy-density primary battery,the Li-SOCl_(2) battery offers significant advantages over other primary systems,including a high operating voltage,wide temperature tolerance,and low self-discharge rate.However,owing to the irreversible electrochemical reaction mechanism,despite its energy density of up to 700 Wh kg^(-1) at the cell level,this battery system has remained confined to the category of primary batteries,thereby limiting its use in cyclic applications.Recent advances in electrochemical technologies have enabled the reversible redox chemistry of Li-SOCl_(2) batteries,transforming them into rechargeable systems.This article provides a systematic overview of the technical evolution,reaction mechanisms,safety constraints,engineering countermeasures,and electrochemical performance enhancement of Li-SOCl_(2) primary batteries since their introduction.First,the modification methods for the lithium anode,carbon cathode,electrolyte,and electrocatalyst in Li-SOCl_(2) primary batteries are discussed,along with their mechanisms for improving electrochemical performance.We then review the SOCl_(2)-based rechargeable Li metal batteries(LMBs)that evolved from the Li-SOCl_(2) primary batteries.With their higher energy density,these systems have become promising candidates to replace traditional Li-ion batteries(LIBs).This review focuses on the construction of key components,such as the positive electrode carrier,novel alloy anode,and electrolyte,as well as their impact on electrochemical performance in rechargeable batteries.Finally,we summarize current research progress and propose future directions for SOCl_(2)-based LMBs aimed at enhancing overall electrochemical performance.These insights provide a theoretical foundation for the development of next-generation high-energy-density energy-storage technologies.展开更多
Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by t...Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by the poor conductivity andthe irreversible dissolution of conventionalε-MnO_(2)deposits.Herein,we report a scalable semisolid slurryelectrode architecture that enables stable MnO_(2)deposition/dissolution using a three-dimensional percolatingnetwork of carbon nanotubes(CNTs)as both conductivematrix and deposition host.The slurry systempromotes the formation of highly conductiveγ-MnO_(2)owing to enhanced charge transfer kinetics,enablingoverall dissolution rather than the localized separationtypically seen in traditional electrodes.The Zn-MnO_(2)slurry cell exhibits a reversible areal capacity approaching 60 mAh cm^(-2).Moreover,theflowable nature of the slurry allows electrochemically inactive MnO_(2)formed during dissolution to be reconnected and reactivated by CNTs inthe rheological network,ensuring deep utilization and cycling stability.This work establishes a slurry electrode strategy to improve electrolyticMnO_(2)reactions and offers a viable pathway toward renewable aqueous batteries for grid-scale applications.展开更多
Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_...Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.展开更多
The structural stress/strain induced by K-ion intercalation remains a critical challenge for K-ion batteries.To address this,a dopamine-intercalated WS_(2) hybrid(Dam-WS1.87)with a unique strain-self-relaxation archit...The structural stress/strain induced by K-ion intercalation remains a critical challenge for K-ion batteries.To address this,a dopamine-intercalated WS_(2) hybrid(Dam-WS1.87)with a unique strain-self-relaxation architecture was fabricated.Interestingly,the WS_(2) matrix undergoes a structural transformation owing to the intense infiltration effect of dopamine molecules,expanding interlayer spacing(0.813 nm)and introducing 6.5%S-vacancies while preserving high compaction density(4.0874 gcm^(-3)).The engineered structure demonstrates remarkable mechanical stability,exhibiting only 19.0%crystallite expansion upon full potassiation(vs.101.3%for pristine WS_(2)),demonstrating efficient strain alleviation through its strain-self-relaxation architecture.As a result,Dam-WS1.87delivers reversible capacities of 312.6 m A h g^(-1)/1277.7 mA h cm^(-3)at 0.125 C,along with superior rate capability(maintaining 210.4 m A h g^(-1)at 5 C)and unprecedented cycling stability(85.3%capacity retention after 1400 cycles at 1 C).This work provides new insights into designing strain-tolerant electrode materials for nextgeneration energy storage systems.展开更多
Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challeng...Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challenges such as structural phase transitions,Na^(+)/vacancy ordering,and Jahn–Teller distortion effect,resulting in severe capacity decay and sluggish ion kinetics.We develop a novel Cu/Y dual-doping strategy that leads to the formation of"Na–Y"interlayer aggregates,which act as structural pillars within alkali metal layers,enhancing structural stability and disrupting the ordered arrangement of Na^(+)/vacancies.This disruption leads to a unique coexistence of ordered and disordered Na^(+)/vacancy states with near-zero strain,which significantly improves Na^(+)diffusion kinetics.This structural innovation not only mitigates the unfavorable P2–O2 phase transition but also facilitates rapid ion transport.As a result,the doped material demonstrates exceptional electrochemical performance,including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of~70 mAh g^(−1)at 50 C.The discovery of this novel interlayer pillar,along with its role in modulating Na^(+)/vacancy arrangements,provides a fresh perspective on engineering layered oxides.It opens up promising new pathways for the structural design of advanced cathode materials toward efficient,stable,and high-rate SIBs.展开更多
Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen ba...Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.展开更多
Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on ...Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on energy storage and conversion applications,such as use as anodes in lithium-ion batteries.In this paper,all-inorganic lead-free halide perovskite Cs_(3)Bi_(2)Cl_(9)powders were synthesized by the grinding method,and the lattice was successfully adjusted via introducing Mn^(2+).The characterization results show that Mn-ion substitution can cause local lattice distortion to restructure the lattice,which will cause a mixed arrangement of[BiCl_(6)]octahedra to improve the performance of the anode material.This new material can provide a feasible solution for solving the problem of low specific capacity anode materials caused by unstable crystal structures,and also indicates that such perovskites with unique crystal structures and lattice tunability have broad application prospects in lithium-ion batteries.展开更多
TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperat...TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperature conditions.Herein,we introduce crystallographic engineering to enhance structure stability and promote Li+diffusion kinetics of TiNb_(2)O_(7)(TNO).The density functional theory computation reveals that Ti^(4+)is replaced by Sb^(5+)and Nb^(5+)in crystal lattices,which can reduce the Li+diffusion impediment and improve electronic conductivity.Synchrotron radiation X-ray 3D nano-computed tomography and in situ X-ray diffraction measurement confirm the introduction of Sb/Nb alleviates volume expansion during lithiation and delithiation processes,contributing to enhancing structure stability.Extended X-ray absorption fine structure spectra results verify that crystallographic engineering also increases short Nb-O bond length in TNO-Sb/Nb.Accordingly,the TNO-Sb/Nb anode delivers an outstanding capacity retention rate of 89.8%at 10 C after 700 cycles and excellent rate performance(140.4 mAh g^(−1) at 20 C).Even at−30℃,TNO-Sb/Nb anode delivers a capacity of 102.6 mAh g^(−1) with little capacity degeneration for 500 cycles.This work provides guidance for the design of fast-charging batteries at low-temperature condition.展开更多
Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosize...Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosized anatase TiO_(2) exposed(001)facet doubles the capacity compared to the micro-sized sample ascribed to the interfacial Mg^(2+)ion storage.First-principles calculations reveal that the diffusion energy barrier of Mg^(2+)on the(001)facet is significantly lower than those in the bulk phase and on(100)facet,and the adsorption energy of Mg^(2+)on the(001)facet is also considerably lower than that on(100)facet,which guarantees superior interfacial Mg^(2+)storage of(001)facet.Moreover,anatase TiO_(2) exposed(001)facet displays a significantly higher capacity of 312.9 mAh g^(−1) in Mg-Li dual-salt electrolyte compared to 234.3 mAh g^(−1) in Li salt electrolyte.The adsorption energies of Mg^(2+)on(001)facet are much lower than the adsorption energies of Li+on(001)facet,implying that the Mg^(2+)ion interfacial storage is more favorable.These results highlight that controlling the crystal facet of the nanocrystals effectively enhances the interfacial storage of multivalent ions.This work offers valuable guidance for the rational design of high-capacity storage systems.展开更多
To promote CO_(2)redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO_(2))batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and ...To promote CO_(2)redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO_(2))batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and dopamine monomers,respectively,and coupled with high-temperature heat treatment to obtain nitrogen-carbon encapsulated Cu_(x)S@NC_(PPy)and Cu_(x)S@NCPDA catalysts.The results show that the encapsulation of nitrogen-doped carbon not only increases the specific surface area and improves the electron affinity but also promotes the synergistic interaction between the CuS-based active species and the defect carbon,thus providing abundant active sites for CO_(2)conversion.The electrochemical performances of the carbon-coated modified samples were all improved,especially the hybrid Na-CO_(2)battery based on Cu_(x)S@NC_(PPy),which showed a low voltage gap of 0.74 V at 0.1 mA/cm^(2)and a high power density of 3.42 mW/cm^(2).展开更多
Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantia...Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.展开更多
2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems...2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems,critical challenges such as interfacial resistance,limited ion transport,dendrite growth,and mechanical degradation hinder their widespread adoption.This review aims to provide a comprehensive analysis of the roles and fu nctions of Ti_(3)C_(2)T_(x) MXenes in SSBs,emphasizing their application as interlayers,anode/cathode additives,and current collectors,and highlighting their impact on interracial stability,ionic/electro nic transport,electrochemical performance,and cycling durability in SSB architectures.Unlike other 2D materials,Ti_(3)C_(2)T_(x) exhibits outsta nding metallic conductivity,tu nable surface terminations,hydrophilicity,and excellent mechanical flexibility,making it ideal for multifu nctional integration in SSBs,As a component in solid-state electrolytes(SSEs),Ti_(3)C_(2)T_(x) improves ionic conductivity and mecha nical strength.When used in electrodes,it serves as a conductive scaffold that enhances charge transport and structural durability.Additionally,its role as an interfacial interlayer effectively reduces interfacial impedance,accommodates volume changes,and suppresses dendrite formation.Its lightweight and high conductivity enable its use as a current collector.This review highlights recent advances in Ti_(3)C_(2)T_(x)-based components for SSBs like Li-,Na-,Zn,Li-S,etc.,emphasizing enha ncements in ion/electron transport,interfacial stability,and structural robustness.Finally,the review outlines challenges and opportunities along with a future outlook focused on improving the MXene oxidation,tailoring surface terminations,improving long-term stability,and exploring scalable fabrication strategies for MXene-based SSB components.展开更多
Ceramic-gel composite electrolytes(CGEs)attract significant attention as solid-state electrolytes(SSEs)for sodium metal batteries owing to their favorable ionic conductivity and interfacial compatibility.However,conve...Ceramic-gel composite electrolytes(CGEs)attract significant attention as solid-state electrolytes(SSEs)for sodium metal batteries owing to their favorable ionic conductivity and interfacial compatibility.However,conventional CGEs generally feature insufficient mechanical strength and consequent uncontrollable dendrite growth,remaining long-standing fundamental challenges that severely limit practical applications.Herein,this study presents a high-strength CGE that enables efficient stress transfer,achieving a compressive strength of 20.1 MPa(20 times higher than conventional gel electrolytes),while maintaining excellent ionic conductivity and effectively suppressing sodium dendrites.The 3D-Na_(3)Zr_(2)Si_(2)PO_(12)framework further serves as a thermal barrier,imparting the CGE with superior flame retardancy.Additionally,Na/CGE/NVP-K_(0.05)cells exhibit 75.9%capacity retention after 10,000 cycles at 5C(25℃)and deliver78.5 mAh g^(-1)at 30C(60℃).Remarkably,the CGE exhibits excellent low-temperature adaptability,retaining nearly 100% capacity at-20℃.These results highlight a viable strategy for designing safe and high-performance solid-state sodium metal batteries toward practical deployment.展开更多
Low-cost and high-safety aqueous Zn-I_(2) batteries attract extensive attention for large-scale energy storage systems.However,polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capabi...Low-cost and high-safety aqueous Zn-I_(2) batteries attract extensive attention for large-scale energy storage systems.However,polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capability and severe capacity decay.Herein,a three-dimensional polyaniline is wrapped by carboxylcarbon nanotubes(denoted as C-PANI)which is designed as a catalytic cathode to effectively boost iodine conversion with suppressed polyiodide shuttling,thereby improving Zn-I_(2) batteries.Specifically,carboxyl-carbon nanotubes serve as a proton reservoir for more protonated-NH+=sites in PANI chains,achieving a direct I0/I−reaction for suppressed polyiodide generation and Zn corrosion.Attributing to this“proton-iodine”regulation,catalytic protonated C-PANI strongly fixes electrolytic iodine species and stores proton ions simultaneously through reversible-N=/-NH^(+)-reaction.Therefore,the electrolytic Zn-I_(2) battery with C-PANI cathode exhibits an impressive capacity of 420 mAh g^(−1) and ultra-long lifespan over 40,000 cycles.Additionally,a 60 mAh pouch cell was assembled with excellent cycling stability after 100 cycles,providing new insights into exploring effective organocatalysts for superb Zn-halogen batteries.展开更多
基金supported by the Recruitment Program of Global Youth Experts of Chinathe Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA09010401)+1 种基金the Science and Technology Development Program of Jilin Province,China(Grant No.20150623002TC)the Natural Science Foundation of Jiangsu Province,China(Grant No.BK20131139)
文摘Although significant progress has been made in many aspects of the emerging aprotic Li-O2 battery system, an indepth understanding of the oxygen reactions is still underway. The oxygen reactions occurring in the positive electrode distinguish Li-O2 batteries from the conventional Li-ion cells and play a crucial role in the Li-O2 cell＇s performance （capacity, rate capability, and cycle life）. Recent advances in fundamental studies of oxygen reactions in aprotic Li-O2 batteries are reviewed, including the reaction route, kinetics, morphological evolution of Li2O2, and charge transport within Li2O2. Prospects are also provided for future fundamental investigations of Li-O2 chemistry.
基金the National Natural Science Foundation of China (Nos.U1732111 and 21676241)“The Recruitment Program of Global Youth Experts” from the Chinese government+2 种基金the “Hundred Talents Program” of Zhejiang UniversityHubei Natural Science Foundation of China (No.2018CFB531)Self-determined Research Funds of CCNU from Colleges’ Basic Research and Operation of MOE (No.CCNU18TS045)。
文摘Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy density.However,due to the difficulty of decomposition of Li2 O2,Li-O2 batteries have high charge overpotential and poor cycling life.So all kinds of catalysts have been studied on the cathode.Compared to heterogeneous solid catalysts,soluble catalysts achieve faster and more effective transport of electrons by reversible redox pairs.Here,we first report ruthenocene(Ruc) as a mobile redox mediator in a Li-O2 battery.0.01 mol/L Ruc in the electrolyte effectively reduces the charging voltage by 610 mV.Additionally,Ruc greatly increases the cycling life by four-fold(up to 83 cycles) with a simple ketjen black(KB) cathode.The results of SEM,XPS and XRD confirm that less discharge product residue accumulated after recharge.To verify the reaction mechanisms of the mediato r,free energy profiles of the possible reaction pathways based on DFT are provided.
基金supported by the Natural Science Foundation of China(No.21303038)Scientific Research Foundation for the Returned Overseas Chinese Scholars+1 种基金State Education Ministry One Hundred,Talents Program of Anhui ProvinceOpen Funds of the State Key Laboratory of Rare Earth Resource Utilization(No.RERU2016004)
文摘As one of the next-generation energy-storage devices,Li-O_2 battery has become the main research direction for the academic researchers due to its characteristics of environmental friendship,relatively simple structures,high energy density of 3500Wh/kg and low cost.However,Li-O_2 battery cannot be commercialized on a large scale because of the challenging issues including high-efficient electrocatalysts,membranes,Li-based anode and so on.In this review,we focused on the recent development of electrocatalyst materials as cathodes for the non-aqueous Li-O_2 batteries which are relatively simpler than other Li-O_2 batteries＇ structures.Electrocatalysts were summarized including noble metals,nanocarbon materials,transition metals and their hybrids.We points out that the challenges of preparation high-efficient catalysts not only require high catalytic activity and conductivity,but also have novel nanoarchitectures with large interface and porous volume for LiO_x storage.Furthermore,the further investigation of reaction mechanism and advanced in situ analysis technologies are welcome in the coming work.
基金sponsored by the National Natural Science Foundation of China(21475021 and 21427807)the Fundamental Research Funds for the Central Universities(2242017 K41023)
文摘Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.
基金Funded by the National Natural Science Foundation of China(No.22075035)the Technology Planning Project of Liaoning Province(No.2020JH2/10700008)the Dalian Science and Technology Innovation Fund Project(No.2022JJ11CG005)。
文摘We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O_(2)batteries.It is observed that the intermediate LiMnO_(4)rather than Li_(2)O_(2)is formed when LiO_(2)interactes with MnO(111)during the discharge process.It is precisely because of LiMnO_(4)that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO_(4)further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.
文摘Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.
基金financially supported by the National Natural Science Foundation of China(No.22309138)the Hubei Province Natural Science Foundation(No.2024AFB815)+1 种基金the Postdoctoral Project of Hubei Province(No.2024HBBHXF056)the Department of Science and Technology of Hubei Province(No.2025CSA001)。
文摘As a high-energy-density primary battery,the Li-SOCl_(2) battery offers significant advantages over other primary systems,including a high operating voltage,wide temperature tolerance,and low self-discharge rate.However,owing to the irreversible electrochemical reaction mechanism,despite its energy density of up to 700 Wh kg^(-1) at the cell level,this battery system has remained confined to the category of primary batteries,thereby limiting its use in cyclic applications.Recent advances in electrochemical technologies have enabled the reversible redox chemistry of Li-SOCl_(2) batteries,transforming them into rechargeable systems.This article provides a systematic overview of the technical evolution,reaction mechanisms,safety constraints,engineering countermeasures,and electrochemical performance enhancement of Li-SOCl_(2) primary batteries since their introduction.First,the modification methods for the lithium anode,carbon cathode,electrolyte,and electrocatalyst in Li-SOCl_(2) primary batteries are discussed,along with their mechanisms for improving electrochemical performance.We then review the SOCl_(2)-based rechargeable Li metal batteries(LMBs)that evolved from the Li-SOCl_(2) primary batteries.With their higher energy density,these systems have become promising candidates to replace traditional Li-ion batteries(LIBs).This review focuses on the construction of key components,such as the positive electrode carrier,novel alloy anode,and electrolyte,as well as their impact on electrochemical performance in rechargeable batteries.Finally,we summarize current research progress and propose future directions for SOCl_(2)-based LMBs aimed at enhancing overall electrochemical performance.These insights provide a theoretical foundation for the development of next-generation high-energy-density energy-storage technologies.
基金supported by the National Natural Science Foundation of China(No.22109181,U24A2060,22279023,and 22309031)the National Key R&D Program of China(2024YFE0101100)+6 种基金the Hunan Provincial Science and Technology Plan Projects of China(No.2017TP1001)the Hunan Provincial Natural Science Foundation of China(No.2025JJ40011)the Fundamental Research Funds for the Central Universities(20720250005)the Science and Technology Commission of Shanghai Municipality(25DZ3002901,2024ZDSYS02,25PY2600100)the Shanghai Pilot Program for Basic Research-Fudan University 21TQ1400100(25TQ012)the AI for Science Foundation of Fudan University(FudanX24A1035)the National Research Foundation,Singapore,under its Singapore-China Joint Flagship Project(Clean Energy).
文摘Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by the poor conductivity andthe irreversible dissolution of conventionalε-MnO_(2)deposits.Herein,we report a scalable semisolid slurryelectrode architecture that enables stable MnO_(2)deposition/dissolution using a three-dimensional percolatingnetwork of carbon nanotubes(CNTs)as both conductivematrix and deposition host.The slurry systempromotes the formation of highly conductiveγ-MnO_(2)owing to enhanced charge transfer kinetics,enablingoverall dissolution rather than the localized separationtypically seen in traditional electrodes.The Zn-MnO_(2)slurry cell exhibits a reversible areal capacity approaching 60 mAh cm^(-2).Moreover,theflowable nature of the slurry allows electrochemically inactive MnO_(2)formed during dissolution to be reconnected and reactivated by CNTs inthe rheological network,ensuring deep utilization and cycling stability.This work establishes a slurry electrode strategy to improve electrolyticMnO_(2)reactions and offers a viable pathway toward renewable aqueous batteries for grid-scale applications.
文摘Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.
基金financially supported by the National Natural Science Foundation of China(22578493,22238012,52270115)the Beijing Nova Program(20240484570)+4 种基金the Postdoctoral Fellowship Program of CPSF(2024GZB20240847)the China Postdoctoral Science Foundation(M753609)the CNPC Innovation Found(2024DQ02-0206,2022DQ02-0410)the Science Foundation of China University of Petroleum(Beijing)(2462023QNXZ015,2462024PTJS011)the Open Project Fund of the Ministry of Education Engineering Research Center for Clean Low Carbon Energy(ZX20240167)。
文摘The structural stress/strain induced by K-ion intercalation remains a critical challenge for K-ion batteries.To address this,a dopamine-intercalated WS_(2) hybrid(Dam-WS1.87)with a unique strain-self-relaxation architecture was fabricated.Interestingly,the WS_(2) matrix undergoes a structural transformation owing to the intense infiltration effect of dopamine molecules,expanding interlayer spacing(0.813 nm)and introducing 6.5%S-vacancies while preserving high compaction density(4.0874 gcm^(-3)).The engineered structure demonstrates remarkable mechanical stability,exhibiting only 19.0%crystallite expansion upon full potassiation(vs.101.3%for pristine WS_(2)),demonstrating efficient strain alleviation through its strain-self-relaxation architecture.As a result,Dam-WS1.87delivers reversible capacities of 312.6 m A h g^(-1)/1277.7 mA h cm^(-3)at 0.125 C,along with superior rate capability(maintaining 210.4 m A h g^(-1)at 5 C)and unprecedented cycling stability(85.3%capacity retention after 1400 cycles at 1 C).This work provides new insights into designing strain-tolerant electrode materials for nextgeneration energy storage systems.
基金supported by the “Pioneer” and “Leading Goose” R&D Program of Zhejiang Province of China (No. 2024C01056)the support from London South Bank University
文摘Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challenges such as structural phase transitions,Na^(+)/vacancy ordering,and Jahn–Teller distortion effect,resulting in severe capacity decay and sluggish ion kinetics.We develop a novel Cu/Y dual-doping strategy that leads to the formation of"Na–Y"interlayer aggregates,which act as structural pillars within alkali metal layers,enhancing structural stability and disrupting the ordered arrangement of Na^(+)/vacancies.This disruption leads to a unique coexistence of ordered and disordered Na^(+)/vacancy states with near-zero strain,which significantly improves Na^(+)diffusion kinetics.This structural innovation not only mitigates the unfavorable P2–O2 phase transition but also facilitates rapid ion transport.As a result,the doped material demonstrates exceptional electrochemical performance,including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of~70 mAh g^(−1)at 50 C.The discovery of this novel interlayer pillar,along with its role in modulating Na^(+)/vacancy arrangements,provides a fresh perspective on engineering layered oxides.It opens up promising new pathways for the structural design of advanced cathode materials toward efficient,stable,and high-rate SIBs.
基金financially supported by the National Natural Science Foundation of China(U21A20311,U24A2040,52171141,52272117)the Natural Science Foundation of Shandong Province(ZR2022JQ19)+3 种基金the Key Technology Research Project of Shandong Province(2023CXGC010202)the Taishan Industrial Experts Program(TSCX202306142)the Core Facility Sharing Platform of Shandong Universitythe Foundation of Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University。
文摘Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.
基金supported by the Foundation of Yunnan Province(Nos.202301AU070021,202201BE070001-027)the Test Foundation of KUST(No.2022T20210208).
文摘Halide perovskite materials have received considerable attention for solar cells,LEDs,lasers etc.owing to their controllable physicochemical properties and structural advantages.However,little research has focused on energy storage and conversion applications,such as use as anodes in lithium-ion batteries.In this paper,all-inorganic lead-free halide perovskite Cs_(3)Bi_(2)Cl_(9)powders were synthesized by the grinding method,and the lattice was successfully adjusted via introducing Mn^(2+).The characterization results show that Mn-ion substitution can cause local lattice distortion to restructure the lattice,which will cause a mixed arrangement of[BiCl_(6)]octahedra to improve the performance of the anode material.This new material can provide a feasible solution for solving the problem of low specific capacity anode materials caused by unstable crystal structures,and also indicates that such perovskites with unique crystal structures and lattice tunability have broad application prospects in lithium-ion batteries.
基金supported by the National Natural Science Foundation of China(22279026,2247090373)the Natural Science Foundation of Chongqing(CSTB2022NSCQ-MSX1401)+2 种基金the China Postdoctoral Science Foundation(2024M764198)the National Natural Science Foundation of China(22509044)the Fundamental Research Funds for the Central Universities(grant no.HIT.OCEF.2022017).
文摘TiNb_(2)O_(7)represents an up-and-coming anode material for fast-charging lithium-ion batteries,but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperature conditions.Herein,we introduce crystallographic engineering to enhance structure stability and promote Li+diffusion kinetics of TiNb_(2)O_(7)(TNO).The density functional theory computation reveals that Ti^(4+)is replaced by Sb^(5+)and Nb^(5+)in crystal lattices,which can reduce the Li+diffusion impediment and improve electronic conductivity.Synchrotron radiation X-ray 3D nano-computed tomography and in situ X-ray diffraction measurement confirm the introduction of Sb/Nb alleviates volume expansion during lithiation and delithiation processes,contributing to enhancing structure stability.Extended X-ray absorption fine structure spectra results verify that crystallographic engineering also increases short Nb-O bond length in TNO-Sb/Nb.Accordingly,the TNO-Sb/Nb anode delivers an outstanding capacity retention rate of 89.8%at 10 C after 700 cycles and excellent rate performance(140.4 mAh g^(−1) at 20 C).Even at−30℃,TNO-Sb/Nb anode delivers a capacity of 102.6 mAh g^(−1) with little capacity degeneration for 500 cycles.This work provides guidance for the design of fast-charging batteries at low-temperature condition.
基金supported by the National Key R&D Program of China(No.2023YFB3809500)the Fundamental Research Funds for the Central Universities(No.2024CDJXY003)+1 种基金the Venture&Innovation Support Program for Chongqing Overseas Returnees(cx2023087)The Chongqing Technology Innovation and Application Development Project(No.2024TIAD-KPX0003).
文摘Micro-sized anatase TiO_(2) displays inferior capacity as cathode material for magnesium ion batteries because of the higher diffusion energy barrier of Mg^(2+)in anatase TiO_(2) lattice.Herein,we report that nanosized anatase TiO_(2) exposed(001)facet doubles the capacity compared to the micro-sized sample ascribed to the interfacial Mg^(2+)ion storage.First-principles calculations reveal that the diffusion energy barrier of Mg^(2+)on the(001)facet is significantly lower than those in the bulk phase and on(100)facet,and the adsorption energy of Mg^(2+)on the(001)facet is also considerably lower than that on(100)facet,which guarantees superior interfacial Mg^(2+)storage of(001)facet.Moreover,anatase TiO_(2) exposed(001)facet displays a significantly higher capacity of 312.9 mAh g^(−1) in Mg-Li dual-salt electrolyte compared to 234.3 mAh g^(−1) in Li salt electrolyte.The adsorption energies of Mg^(2+)on(001)facet are much lower than the adsorption energies of Li+on(001)facet,implying that the Mg^(2+)ion interfacial storage is more favorable.These results highlight that controlling the crystal facet of the nanocrystals effectively enhances the interfacial storage of multivalent ions.This work offers valuable guidance for the rational design of high-capacity storage systems.
基金financially supported by the National Natural Science Foundation of China(No.52172264)the National Key Research and Development Program of China(No.2022YFC3900802)。
文摘To promote CO_(2)redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO_(2))batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and dopamine monomers,respectively,and coupled with high-temperature heat treatment to obtain nitrogen-carbon encapsulated Cu_(x)S@NC_(PPy)and Cu_(x)S@NCPDA catalysts.The results show that the encapsulation of nitrogen-doped carbon not only increases the specific surface area and improves the electron affinity but also promotes the synergistic interaction between the CuS-based active species and the defect carbon,thus providing abundant active sites for CO_(2)conversion.The electrochemical performances of the carbon-coated modified samples were all improved,especially the hybrid Na-CO_(2)battery based on Cu_(x)S@NC_(PPy),which showed a low voltage gap of 0.74 V at 0.1 mA/cm^(2)and a high power density of 3.42 mW/cm^(2).
基金National Natural Science Foundation of China,Grant/Award Number:52272225。
文摘Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.
基金supported by a National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2020R1A6A1A03043435 and 2020R1A2C1099862)supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(P0012451,The Competency Development Program for Industry Specialist)。
文摘2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems,critical challenges such as interfacial resistance,limited ion transport,dendrite growth,and mechanical degradation hinder their widespread adoption.This review aims to provide a comprehensive analysis of the roles and fu nctions of Ti_(3)C_(2)T_(x) MXenes in SSBs,emphasizing their application as interlayers,anode/cathode additives,and current collectors,and highlighting their impact on interracial stability,ionic/electro nic transport,electrochemical performance,and cycling durability in SSB architectures.Unlike other 2D materials,Ti_(3)C_(2)T_(x) exhibits outsta nding metallic conductivity,tu nable surface terminations,hydrophilicity,and excellent mechanical flexibility,making it ideal for multifu nctional integration in SSBs,As a component in solid-state electrolytes(SSEs),Ti_(3)C_(2)T_(x) improves ionic conductivity and mecha nical strength.When used in electrodes,it serves as a conductive scaffold that enhances charge transport and structural durability.Additionally,its role as an interfacial interlayer effectively reduces interfacial impedance,accommodates volume changes,and suppresses dendrite formation.Its lightweight and high conductivity enable its use as a current collector.This review highlights recent advances in Ti_(3)C_(2)T_(x)-based components for SSBs like Li-,Na-,Zn,Li-S,etc.,emphasizing enha ncements in ion/electron transport,interfacial stability,and structural robustness.Finally,the review outlines challenges and opportunities along with a future outlook focused on improving the MXene oxidation,tailoring surface terminations,improving long-term stability,and exploring scalable fabrication strategies for MXene-based SSB components.
基金the financial support from the National Natural Science Foundation of China(52072091 and 22479091)Heilongjiang Touyan Team and the Fundamental Research Funds for the Central Universities(Grant No.HIT.OCEF.2021015)the financial support from the China Scholarship Council(No.202406120138)。
文摘Ceramic-gel composite electrolytes(CGEs)attract significant attention as solid-state electrolytes(SSEs)for sodium metal batteries owing to their favorable ionic conductivity and interfacial compatibility.However,conventional CGEs generally feature insufficient mechanical strength and consequent uncontrollable dendrite growth,remaining long-standing fundamental challenges that severely limit practical applications.Herein,this study presents a high-strength CGE that enables efficient stress transfer,achieving a compressive strength of 20.1 MPa(20 times higher than conventional gel electrolytes),while maintaining excellent ionic conductivity and effectively suppressing sodium dendrites.The 3D-Na_(3)Zr_(2)Si_(2)PO_(12)framework further serves as a thermal barrier,imparting the CGE with superior flame retardancy.Additionally,Na/CGE/NVP-K_(0.05)cells exhibit 75.9%capacity retention after 10,000 cycles at 5C(25℃)and deliver78.5 mAh g^(-1)at 30C(60℃).Remarkably,the CGE exhibits excellent low-temperature adaptability,retaining nearly 100% capacity at-20℃.These results highlight a viable strategy for designing safe and high-performance solid-state sodium metal batteries toward practical deployment.
基金supported by the National Natural Science Foundation of China(22209006,21935001)the Natural Science Foundation of Shandong Province(ZR2022QE009)+1 种基金Fundamental Research Funds for the Central Universities(buctrc202307)the Beijing Natural Science Foundation(Z210016).
文摘Low-cost and high-safety aqueous Zn-I_(2) batteries attract extensive attention for large-scale energy storage systems.However,polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capability and severe capacity decay.Herein,a three-dimensional polyaniline is wrapped by carboxylcarbon nanotubes(denoted as C-PANI)which is designed as a catalytic cathode to effectively boost iodine conversion with suppressed polyiodide shuttling,thereby improving Zn-I_(2) batteries.Specifically,carboxyl-carbon nanotubes serve as a proton reservoir for more protonated-NH+=sites in PANI chains,achieving a direct I0/I−reaction for suppressed polyiodide generation and Zn corrosion.Attributing to this“proton-iodine”regulation,catalytic protonated C-PANI strongly fixes electrolytic iodine species and stores proton ions simultaneously through reversible-N=/-NH^(+)-reaction.Therefore,the electrolytic Zn-I_(2) battery with C-PANI cathode exhibits an impressive capacity of 420 mAh g^(−1) and ultra-long lifespan over 40,000 cycles.Additionally,a 60 mAh pouch cell was assembled with excellent cycling stability after 100 cycles,providing new insights into exploring effective organocatalysts for superb Zn-halogen batteries.
