Towards advanced zinc anodes by interfacial modification strategies for efficient aqueous zinc metal batteries

Developing sustainable and clean energy sources(e.g.,solar,wind,and tide energy)is essential to achieve the goal of carbon neutrality.Due to the discontinuous and inco nsistent nature of common clean energy sources,high-performance energy storage technologies are a critical part of achieving this target.Aqueous zinc metal batteries(AZMBs)with inherent safety,low cost,and competitive performance are regarded as one of the promising candidates for grid-scale energy storage.However,zinc metal anodes(ZMAs)with irreversible problems of dendrite growth,hydrogen evolution reaction,self-corrosio n,and other side reactions have seriously hindered the development and commercialization of AZMBs.An increasing number of researchers are focusing on the stability of ZMAs,so assessing the effectiveness of existing research strategies is critical to the development of AZMBs.This review aims to provide a comprehensive overview of the fundamentals and challenges of AZMBs.Resea rch strategies for interfacial modification of ZMAs are systematically presented.The features of artificial interfacial coating and in-situ interfacial coating of ZMAs are compared and discussed in detail,as well as the effect of modified interfacial ZMA on the full-battery performance.Finally,perspectives are provided on the problems and challenges of ZMAs.This review is expected to offer a constructive reference for the further development and commercialization of AZMBs.

Effect of phosphorus content on interfacial heat transfer and film deposition behavior during the high-temperature simulation of strip casting

The interfacial wettability and heat transfer behavior are crucial in the strip casting of high phosphorus-containing steel.A hightemperature simulation of strip casting was conducted using the droplet solidification technique with the aims to reveal the effects of phosphorus content on interfacial wettability,deposited film,and interfacial heat transfer behavior.Results showed that when the phosphorus content increased from 0.014wt%to 0.406wt%,the mushy zone enlarged,the complete solidification temperature delayed from1518.3 to 1459.4℃,the final contact angle decreased from 118.4°to 102.8°,indicating improved interfacial contact,and the maximum heat flux increased from 6.9 to 9.2 MW/m2.Increasing the phosphorus content from 0.081wt%to 0.406wt%also accelerated the film deposition rate from 1.57 to 1.73μm per test,resulting in a thickened naturally deposited film with increased thermal resistance that advanced the transition point of heat transfer from the fifth experiment to the third experiment.

A Review on Engineering Design for Enhancing Interfacial Contact in Solid-State Lithium–Sulfur Batteries

The utilization of solid-state electrolytes(SSEs)presents a promising solution to the issues of safety concern and shuttle effect in Li–S batteries,which has garnered significant interest recently.However,the high interfacial impedances existing between the SSEs and the electrodes(both lithium anodes and sulfur cathodes)hinder the charge transfer and intensify the uneven deposition of lithium,which ultimately result in insufficient capacity utilization and poor cycling stability.Hence,the reduction of interfacial resistance between SSEs and electrodes is of paramount importance in the pursuit of efficacious solid-state batteries.In this review,we focus on the experimental strategies employed to enhance the interfacial contact between SSEs and electrodes,and summarize recent progresses of their applications in solidstate Li–S batteries.Moreover,the challenges and perspectives of rational interfacial design in practical solid-state Li–S batteries are outlined as well.We expect that this review will provide new insights into the further technique development and practical applications of solid-state lithium batteries.

Multiphase Interfacial Regulation Based on Hierarchical Porous Molybdenum Selenide to Build Anticorrosive and Multiband Tailorable Absorbers

Electromagnetic wave(EMW)absorbing materials have an irreplaceable position in the field of military stealth as well as in the field of electromagnetic pollution control.And in order to cope with the complex electromagnetic environment,the design of multifunctional and multiband high efficiency EMW absorbers remains a tremendous challenge.In this work,we designed a three-dimensional porous structure via the salt melt synthesis strategy to optimize the impedance matching of the absorber.Also,through interfacial engineering,a molybdenum carbide transition layer was introduced between the molybdenum selenide nanoparticles and the three-dimensional porous carbon matrix to improve the absorption behavior of the absorber.The analysis indicates that the number and components of the heterogeneous interfaces have a significant impact on the EMW absorption performance of the absorber due to mechanisms such as interfacial polarization and conduction loss introduced by interfacial engineering.Wherein,the prepared MoSe_(2)/MoC/PNC composites showed excellent EMW absorption performance in C,X,and Ku bands,especially exhibiting a reflection loss of−59.09 dB and an effective absorption bandwidth of 6.96 GHz at 1.9 mm.The coordination between structure and components endows the absorber with strong absorption,broad bandwidth,thin thickness,and multi-frequency absorption characteristics.Remarkably,it can effectively reinforce the marine anticorrosion property of the epoxy resin coating on Q235 steel substrate.This study contributes to a deeper understanding of the relationship between interfacial engineering and the performance of EMW absorbers,and provides a reference for the design of multifunctional,multiband EMW absorption materials.

Eudragit®-PEG Nanoparticles: Physicochemical Characterization and Interfacial Tension Measurements

The objectives of this study are to understand the mechanisms involved in the stabilization of water/oil interfaces by polymeric nanoparticles (NPs) (Eudragit®). Eudragit L100 NPs of various sizes and Zeta potentials were studied and compared at a water/cyclohexane model interface using a droplet tensiometer (Tracker Teclis, Longessaigne, France). The progressive interfacial adsorption of the NPs in the aqueous phase was monitored by tensiometry. The model interface was maintained and observed in a drop tensiometer, analyzed via axisymmetric drop shape analysis (ADSA), to determine the interfacial properties. Given the direct relationship between the stability of Pickering emulsions (emulsions stabilized by solid nanoparticles) and the interfacial properties of these layers, different nanoparticle systems were compared. Specifically, Eudragit NPs of different sizes were examined. Moreover, the reduction of the Zeta potential with PEG-6000 induces partial aggregation of the NPs (referred to as NP flocs), significantly impacting the stability of the interfacial layer. Dynamic surface tension measurements indicate a significant decrease in interfacial tension with Eudragit® nanoparticles (NPs). This reduction correlates with the size of the NPs, highlighting that this parameter does not operate in isolation. Other factors, such as the contact angle and wettability of the nanoparticles, also play a critical role. Notably, larger NPs further diminished the interfacial tension. This study enhances our understanding of the stability of Pickering emulsions stabilized by Eudragit® L100 polymeric nanoparticles.

The reaction mechanism and interfacial crystallization of Al nanoparticle-embedded Ni under shock loading

The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics simulation.For the shock melting of Al nanoparticle,interfacial crystallization and dissolution are the main characteristics.The reaction degree of Al particle first increases linearly and then logarithmically with time driven by rapid mechanical mixing and following dissolution.The reaction rate increases with the decrease of particle diameter,however,the reaction is seriously hindered by interfacial crystallization when the diameter is lower than 9 nm in our simulations.Meanwhile,we found a negative exponential growth in the fraction of crystallized Al atoms,and the crystallinity of B2-NiAl(up to 20%)is positively correlated with the specific surface area of Al particle.This can be attributed to the formation mechanism of B2-NiAl by structural evolution of finite mixing layer near the collapsed interface.For shock melting of both Al particle and Ni matrix,the liquid-liquid phase inter-diffusion is the main reaction mechanism that can be enhanced by the formation of internal jet.In addition,the enhanced diffusion is manifested in the logarithmic growth law of mean square displacement,which results in an almost constant reaction rate similar to the mechanical mixing process.

Exploring the Cation Regulation Mechanism for Interfacial Water Involved in the Hydrogen Evolution Reaction by In Situ Raman Spectroscopy

Interfacial water molecules are the most important participants in the hydrogen evolution reaction(HER).Hence,understanding the behavior and role that interfacial water plays will ultimately reveal the HER mechanism.Unfortunately,investigating interfacial water is extremely challenging owing to the interference caused by bulk water molecules and complexity of the interfacial environment.Here,the behaviors of interfacial water in different cationic electrolytes on Pd surfaces were investigated by the electrochemistry,in situ core-shell nanostructure enhanced Raman spectroscopy and theoretical simulation techniques.Direct spectral evidence reveals a red shift in the frequency and a decrease in the intensity of interfacial water as the potential is shifted in the positively direction.When comparing the different cation electrolyte systems at a given potential,the frequency of the interfacial water peak increases in the specified order:Li+<Na^(+)<K^(+)<Ca^(2+)<Sr^(2+).The structure of interfacial water was optimized by adjusting the radius,valence,and concentration of cation to form the two-H down structure.This unique interfacial water structure will improve the charge transfer efficiency between the water and electrode further enhancing the HER performance.Therefore,local cation tuning strategies can be used to improve the HER performance by optimizing the interfacial water structure.

Interfacial engineering through lead binding using crown ethers in perovskite solar cells

In the domain of perovskite solar cells(PSCs),the imperative to reconcile impressive photovoltaic performance with lead-related issue and environmental stability has driven innovative solutions.This study pioneers an approach that not only rectifies lead leakage but also places paramount importance on the attainment of rigorous interfacial passivation.Crown ethers,notably benzo-18-crown-6-ether(B18C6),were strategically integrated at the perovskite-hole transport material interface.Crown ethers exhibit a dual role:efficiently sequestering and immobilizing Pb^(2+)ions through host-guest complexation and simultaneously establishing a robust interfacial passivation layer.Selected crown ether candidates,guided by density functional theory(DFT)calculations,demonstrated proficiency in binding Pb2+ions and optimizing interfacial energetics.Photovoltaic devices incorporating these materials achieved exceptional power conversion efficiency(PCE),notably 21.7%for B18C6,underscoring their efficacy in lead binding and interfacial passivation.Analytical techniques,including time-of-flight secondary ion mass spectrometry(ToF-SIMS),ultraviolet photoelectron spectroscopy(UPS),time-resolved photoluminescence(TRPL),and transient absorption spectroscopy(TAS),unequivocally affirmed Pb^(2+)ion capture and suppression of non-radiative recombination.Notably,these PSCs maintained efficiency even after enduring 300 h of exposure to 85%relative humidity.This research underscores the transformative potential of crown ethers,simultaneously addressing lead binding and stringent interfacial passivation for sustainable PSCs poised to commercialize and advance renewable energy applications.

Interfacial reinforcement of core-shell HMX@energetic polymer composites featuring enhanced thermal and safety performance

The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves the pretreatment of HMX to endow—OH groups on the surface via polyalcohol bonding agent modification and in situ coating with nitrate ester-containing polymer,was proposed to address the problem.Two types of energetic polyether—glycidyl azide polymer(GAP)and nitrate modified GAP(GNP)were grafted onto HMX crystal based on isocyanate addition reaction bridged through neutral polymeric bonding agent(NPBA)layer.The morphology and structure of the HMX-based composites were characterized in detail and the core-shell structure was validated.The grafted polymers obviously enhanced the adhesion force between HMX crystals and fluoropolymer(F2314)binder.Due to the interfacial reinforcement among the components,the two HMX-based composites exhibited a remarkable increment of phase transition peak temperature by 10.2°C and 19.6°C with no more than 1.5%shell content,respectively.Furthermore,the impact and friction sensitivity of the composites decreased significantly as a result of the barrier produced by the grafted polymers.These findings will enhance the future prospects for the interface design of energetic composites aiming to solve the weak interface and safety concerns.

Regulating interfacial behavior of zinc metal anode via metal-organic framework functionalized separator

Aqueous zinc ion batteries(AZIBs)are one of the promising energy storage devices.However,uncontrolled dendrite and side reactions have seriously hindered its further application.In this study,the metal-organic framework(MOF)functionalized glass fiber separator(GF-PFC-31)was used to regulate interfacial behavior of zinc metal anode,enabling the development of high-performance AZIBs.In PFC-31,there areπ-πinteractions between two adjacent benzene rings with a spacing of 3.199 A.This spacing can block the passage of[Zn(H_(2)O)_6]^(2+)(8.6 A in diameter)through the GF-PFC-31 separator to a certain extent,which promotes the deposition process of Zn ions.In addition,the sulfonic acid group(-S03H)contained in GF-PFC-31 can form a hydrogen bonding network with H_(2)O,which can provide a desolvation effect and reduce the side reaction.Consequently,GF-PFC-31 separator achieves uniform deposition of Zn ions.The Zn‖GF-PFC-31‖Zn symmetric cell exhibits stable cycle life(3000 h at 1.2 mA cm^(-2),2000 h at 0.3 mA cm^(-2),and 2000 h at 5.0 mA cm^(-2)),and Zn‖GF-PFC-31‖MnO_(2) full cell with GF-PFC-31 separator can cycle for 1000 cycles at 1.2 A g^(-1)with capacity retention rate of 82.5%.This work provides a promising method to achieve high-performance AZIBs.

In-situ interfacial passivation and self-adaptability synergistically stabilizing all-solid-state lithium metal batteries

The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.

Metal-free two-dimensional phosphorene-based electrocatalyst with covalent P-N heterointerfacial reconstruction for electrolyte-lean lithium-sulfur batteries

The use of lithium-sulfur batteries under high sulfur loading and low electrolyte concentrations is severely restricted by the detrimental shuttling behavior of polysulfides and the sluggish kinetics in redox processes.Two-dimensional(2D)few layered black phosphorus with fully exposed atoms and high sulfur affinity can be potential lithium-sulfur battery electrocatalysts,which,however,have limitations of restricted catalytic activity and poor electrochemical/chemical stability.To resolve these issues,we developed a multifunctional metal-free catalyst by covalently bonding few layered black phosphorus nanosheets with nitrogen-doped carbon-coated multiwalled carbon nanotubes(denoted c-FBP-NC).The experimental characterizations and theoretical calculations show that the formed polarized P-N covalent bonds in c-FBP-NC can efficiently regulate electron transfer from NC to FBP and significantly promote the capture and catalysis of lithium polysulfides,thus alleviating the shuttle effect.Meanwhile,the robust 1D-2D interwoven structure with large surface area and high porosity allows strong physical confinement and fast mass transfer.Impressively,with c-FBP-NC as the sulfur host,the battery shows a high areal capacity of 7.69 mAh cm^(−2) under high sulfur loading of 8.74 mg cm^(−2) and a low electrolyte/sulfur ratio of 5.7μL mg^(−1).Moreover,the assembled pouch cell with sulfur loading of 4 mg cm^(−2) and an electrolyte/sulfur ratio of 3.5μL mg^(−1) shows good rate capability and outstanding cyclability.This work proposes an interfacial and electronic structure engineering strategy for fast and durable sulfur electrochemistry,demonstrating great potential in lithium-sulfur batteries.

Interfacial design of silicon/carbon anodes for rechargeable batteries:A review

Silicon(Si)has been studied as a promising alloying type anode for lithium-ion batteries due to its high specific capacity,low operating potential and abundant resources.Nevertheless,huge volume expansion during alloying/dealloying processes and low electronic conductivity of Si anodes restrict their electrochemical performance.Thus,carbon(C)materials with special physical and chemical properties are applied in Si anodes to effectively solve these problems.This review focuses on current status in the exploration of Si/C anodes,including the lithiation mechanism and solid electrolyte interface formation,various carbon sources in Si/C anodes,such as traditional carbon sources(graphite,pitch,biomass),and novel carbon sources(MXene,graphene,MOFs-derived carbon,graphdiyne,etc.),as well as interfacial bonding modes of Si and C in the Si/C anodes.Finally,we summarize and prospect the selection of carbonaceous materials,structural design and interface control of Si/C anodes,and application of Si/C anodes in all-solid-state lithium-ion batteries and sodium-ion batteries et al.This review will help researchers in the design of novel Si/C anodes for rechargeable batteries.

Recent advances in interfacial modification of zinc anode for aqueous rechargeable zinc ion batteries

To tackle energy crisis and achieve sustainable development, aqueous rechargeable zinc ion batteries have gained widespread attention in large-scale energy storage for their low cost, high safety, high theoretical capacity, and environmental compatibility in recent years. However, zinc anode in aqueous zinc ion batteries is still facing several challenges such as dendrite growth and side reactions(e.g., hydrogen evolution), which cause poor reversibility and the failure of batteries. To address these issues, interfacial modification of Zn anodes has received great attention by tuning the interaction between the anode and the electrolyte. Herein, we present recent advances in the interfacial modification of zinc anode in this review. Besides, the challenges of reported approaches of interfacial modification are also discussed.Finally, we provide an outlook for the exploration of novel zinc anode for aqueous zinc ion batteries.We hope that this review will be helpful in designing and fabricating dendrite-free and hydrogenevolution-free Zn anodes and promoting the practical application of aqueous rechargeable zinc ion batteries.

Boosting Interfacial Polarization Through Heterointerface Engineering in MXene/Graphene Intercalated-Based Microspheres for Electromagnetic Wave Absorption

Multi-layer 2D material assemblies provide a great number of interfaces beneficial for electromagnetic wave absorption.However,avoiding agglomeration and achieving layer-by-layer ordered intercalation remain chal-lenging.Here,3D reduced graphene oxide(rGO)/MXene/TiO_(2)/Fe_(2)C lightweight porous microspheres with periodical intercalated structures and pronounced inter-facial effects were constructed by spray-freeze-drying and microwave irradiation based on the Maxwell–Wagner effect.Such approach reinforced interfacial effects via defects introduction,porous skeleton,multi-layer assembly and multi-compo-nent system,leading to synergistic loss mechanisms.The abundant 2D/2D/0D/0D intercalated heterojunctions in the microspheres provide a high density of polari-zation charges while generating abundant polarization sites,resulting in boosted interfacial polarization,which is verified by CST Microwave Studio simulations.By precisely tuning the 2D nanosheets intercalation in the heterostructures,both the polarization loss and impedance matching improve significantly.At a low filler loading of 5 wt%,the polarization loss rate exceeds 70%,and a minimum reflection loss(RLmin)of-67.4 dB can be achieved.Moreover,radar cross-section simulations further confirm the attenuation ability of the optimized porous microspheres.These results not only provide novel insights into understanding and enhancing interfacial effects,but also constitute an attractive platform for implementing heterointerface engineering based on customized 2D hierarchical architectures.

Anode Interfacial Issues in Solid-State Li Batteries:Mechanistic Understanding and Mitigating Strategies

All-solid-state Li metal batteries(ASSLBs)using inorganic solid electrolyte(SE)are considered promising alternatives to conventional Li-ion batteries,offering improved safety and boosted energy density.While significant progress has been made on improving the ionic conductivity of SEs,the degradation and instability of Li metal/inorganic SE interfaces have become the critical challenges that limit the coulombic efficiency,power performance,and cycling stability of ASSLBs.Understanding the mechanisms of complex/dynamic interfacial phenomena is of great importance in addressing these issues.Herein,recent studies on identifying,understanding,and solving interfacial issues on anode side in ASSLBs are comprehensively reviewed.Typical issues at Li metal/SE interface include Li dendrite growth/propagation,SE cracking,physical contact loss,and electrochemical reactions,which lead to high interfacial resistance and cell failure.The causes of these issues relating to the chemical,physical,and mechanical properties of Li metal and SEs are systematically discussed.Furthermore,effective mitigating strategies are summarized and their effects on suppressing interfacial reactions,improving interfacial Li-ion transport,maintaining interfacial contact,and stabilizing Li plating/stripping are highlighted.The in-depth mechanistic understanding of interfacial issues and complete investigations on current solutions provide foundations and guidance for future research and development to realize practical application of high-performance ASSLB.

Mixed Cations Enabled Combined Bulk and Interfacial Passivation for Efficient and Stable Perovskite Solar Cells

Here,we report a mixed GAI and MAI(MGM)treatment method by forming a 2D alternating-cation-interlayer(ACI)phase(n=2)perovskite layer on the 3D perovskite,modulating the bulk and interfacial defects in the perovskite films simultaneously,leading to the suppressed nonradiative recombination,longer lifetime,higher mobility,and reduced trap density.Consequently,the devices’performance is enhanced to 24.5%and 18.7%for 0.12 and 64 cm^(2),respectively.In addition,the MGM treatment can be applied to a wide range of perovskite compositions,including MA-,FA-,MAFA-,and CsFAMA-based lead halide perovskites,making it a general method for preparing efficient perovskite solar cells.Without encapsulation,the treated devices show improved stabilities.

Recent Progress in Interfacial Dipole Engineering for Perovskite Solar Cells

Design and modification of interfaces have been the main strategies in developing perovskite solar cells(PSCs). Among the interfacial treatments, dipole molecules have emerged as a practical approach to improve the efficiency and stability of PSCs due to their unique and versatile abilities to control the interfacial properties. Despite extensive applications in conventional semiconductors, working principles and design of interfacial dipoles in the performance/stability enhancement of PSCs are lacking an insightful elucidation. In this review, we first discuss the fundamental properties of electric dipoles and the specific roles of interfacial dipoles in PSCs. Then we systematically summarize the recent progress of dipole materials in several key interfaces to achieve efficient and stable PSCs. In addition to such discussions, we also dive into reliable analytical techniques to support the characterization of interfacial dipoles in PSCs. Finally, we highlight future directions and potential avenues for research in the development of dipolar materials through tailored molecular designs. Our review sheds light on the importance of continued efforts in this exciting emerging field, which holds great potential for the development of high-performance and stable PSCs as commercially demanded.

Preparation, interfacial regulation and strengthening of Mg/Al bimetal fabricated by compound casting: A review

Mg/Al bimetal combines the advantages of both aluminum and magnesium and has broad application prospects in automotive, aerospace,weapons, digital products and so on. The compound casting has the characteristics of low cost, easy to achieve metallurgical combination and suitable for the preparation of complex bimetallic parts. However, bimetallic joint strength is low due to differences of physical properties between Al and Mg, oxide film on metallic surface and interfacial Al-Mg IMCs, which is closely related to the interfacial microstructure and properties. Therefore, how to control the interface of the bimetal to achieve performance enhancement is the focus and difficulty in this field. At present, there are mainly the following strengthening methods. First, the “zincate galvanizing” and “electrolytic polishing+anodic oxidation” technology were exert on the surface of Al alloy to remove and break the oxide film, which improved the wettability between Al and Mg. Second, the undesirable Al-Mg IMCs were reduce or elimination by adding the interlayers(Zn, Ni and Ni-Cu). Thirdly, the evolution process of interfacial microstructure was changed and fine strengthening phases were formed by adding Si element to Al alloy or rare earth element to Mg alloy. Fourthly, mechanical vibration and ultrasonic vibration were applied in the process of the filling and solidification to refine and homogenize the interfacial structure. Finally, some other methods, including secondary rolling, thermal modification, heat treatment and constructing exterior 3D morphology, also can be used to regulate the interfacial microstructure and compositions. The above strengthening methods can be used alone or in combination to achieve bimetallic strengthening. Finally, the future development direction of the Mg/Al bimetal is prospected, which provides some new ideas for the development and application of the Mg/Al bimetal.

Engineering hollow core-shell hetero-structure box to induce interfacial charge modulation for promoting bidirectional sulfur conversion in lithium-sulfur batteries

Severe polysulfide shuttling and sluggish sulfur redox kinetics significantly decrease sulfur utilization and cycling stability in lithium-sulfur batteries(LSBs).Herein,we develop a hollow CoO/CoP-Box core-shell heterostructure as a model and multifunctional catalyst modified on separators to induce interfacial charge modulation and expose more active sites for promoting the adsorption and catalytic conversion ability of sulfur species.Theoretical and experimental findings verify that the in-situ formed core-shell hetero-interface induces the formation of P-Co-O binding and charge redistribution to activate surface O active sites for binding lithium polysulfides(LiPSs)via strong Li-O bonding,thus strongly adsorbing with Li PSs.Meanwhile,the strong Li-O bonding weakens the competing Li-S bonding in LiPSs or Li2S adsorbed on CoO/CoP-Box surface,plus the hollow heterostructure provides abundant active sites and fast electron/Li+transfer,so reducing Li2S nucleation/dissolution activation energy.As expected,LSBs with CoO/CoP-Box modified separator and traditional sulfur/carbon black cathode display a large initial capacity of 1240 mA h g^(-1)and a long cycling stability with 300 cycles(~60.1%capacity retention)at 0.5C.Impressively,the thick sulfur cathode(sulfur loading:5.2 mg cm^(-2))displays a high initial areal capacity of 6.9 mA h cm^(-2).This work verifies a deep mechanism understanding and an effective strategy to induce interfacial charge modulation and enhance active sites for designing efficient dual-directional Li-S catalysts via engineering hollow core-shell hetero-structure.