Currently,the demand for electromagnetic wave(EMW)absorbing materials with specific functions and capable of withstanding harsh environments is becoming increasingly urgent.Multi-component interface engineering is con...Currently,the demand for electromagnetic wave(EMW)absorbing materials with specific functions and capable of withstanding harsh environments is becoming increasingly urgent.Multi-component interface engineering is considered an effective means to achieve high-efficiency EMW absorption.However,interface modulation engineering has not been fully discussed and has great potential in the field of EMW absorption.In this study,multi-component tin compound fiber composites based on carbon fiber(CF)substrate were prepared by electrospinning,hydrothermal synthesis,and high-temperature thermal reduction.By utilizing the different properties of different substances,rich heterogeneous interfaces are constructed.This effectively promotes charge transfer and enhances interfacial polarization and conduction loss.The prepared SnS/SnS_(2)/SnO_(2)/CF composites with abundant heterogeneous interfaces have and exhibit excellent EMW absorption properties at a loading of 50 wt%in epoxy resin.The minimum reflection loss(RL)is−46.74 dB and the maximum effective absorption bandwidth is 5.28 GHz.Moreover,SnS/SnS_(2)/SnO_(2)/CF epoxy composite coatings exhibited long-term corrosion resistance on Q235 steel surfaces.Therefore,this study provides an effective strategy for the design of high-efficiency EMW absorbing materials in complex and harsh environments.展开更多
Research efforts on electromagnetic interference(EMI)shielding materials have begun to converge on green and sustainable biomass materials.These materials offer numerous advantages such as being lightweight,porous,and...Research efforts on electromagnetic interference(EMI)shielding materials have begun to converge on green and sustainable biomass materials.These materials offer numerous advantages such as being lightweight,porous,and hierarchical.Due to their porous nature,interfacial compatibility,and electrical conductivity,biomass materials hold significant potential as EMI shielding materials.Despite concerted efforts on the EMI shielding of biomass materials have been reported,this research area is still relatively new compared to traditional EMI shielding materials.In particular,a more comprehensive study and summary of the factors influencing biomass EMI shielding materials including the pore structure adjustment,preparation process,and micro-control would be valuable.The preparation methods and characteristics of wood,bamboo,cellulose and lignin in EMI shielding field are critically discussed in this paper,and similar biomass EMI materials are summarized and analyzed.The composite methods and fillers of various biomass materials were reviewed.this paper also highlights the mechanism of EMI shielding as well as existing prospects and challenges for development trends in this field.展开更多
Cleat serves as the primary flow pathway for coalbed methane(CBM)and water.However,few studies consider the impact of local contact on two-phase flow within cleats.A visual generalized model of endogenous cleats was c...Cleat serves as the primary flow pathway for coalbed methane(CBM)and water.However,few studies consider the impact of local contact on two-phase flow within cleats.A visual generalized model of endogenous cleats was constructed based on microfluidics.A microscopic and mesoscopic observation technique was proposed to simultaneously capture gas-liquid interface morphology of pores and throat and the two-phase flow characteristics in entire cleat system.The local contact characteristics of cleats reduced absolute permeability,which resulted in a sharp increase in the starting pressure.The reduced gas flow capacity narrowed the co-infiltration area and decreased water saturation at the isotonic point in a hydrophilic environment.The increased local contact area of cleats weakened gas phase flow capacity and narrowed the co-infiltration area.Jumping events occurred in methane-water flow due to altered porosity caused by local contact in cleats.The distribution of residual phases changed the jumping direction on the micro-scale as well as the dominant channel on the mesoscale.Besides,jumping events caused additional energy dissipation,which was ignored in traditional two-phase flow models.This might contribute to the overestimation of relative permeability.The work provides new methods and insights for investigating unsaturated flow in complex porous media.展开更多
Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that...Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that involve carbon composites or nanostructures,primarily due to the un-controllable effects arising from the substantial formation of a solid electrolyte interphase(SEI)during the cycling.Here,an ultra-thin and homogeneous Ti doping alumina oxide catalytic interface is meticulously applied on the porous Si through a synergistic etching and hydrolysis process.This defect-rich oxide interface promotes a selective adsorption of fluoroethylene carbonate,leading to a catalytic reaction that can be aptly described as“molecular concentration-in situ conversion”.The resultant inorganic-rich SEI layer is electrochemical stable and favors ion-transport,particularly at high-rate cycling and high temperature.The robustly shielded porous Si,with a large surface area,achieves a high initial Coulombic efficiency of 84.7%and delivers exceptional high-rate performance at 25 A g^(−1)(692 mAh g^(−1))and a high Coulombic efficiency of 99.7%over 1000 cycles.The robust SEI constructed through a precious catalytic layer promises significant advantages for the fast development of silicon-based anode in fast-charging batteries.展开更多
Global interest in lithium-sulfur batteries as one of the most promising energy storage technologies has been sparked by their low sulfur cathode cost,high gravimetric,volumetric energy densities,abundant resources,an...Global interest in lithium-sulfur batteries as one of the most promising energy storage technologies has been sparked by their low sulfur cathode cost,high gravimetric,volumetric energy densities,abundant resources,and environmental friendliness.However,their practical application is significantly impeded by several serious issues that arise at the cathode-electrolyte interface,such as interface structure degradation including the uneven deposition of Li_(2)S,unstable cathode-electrolyte interphase(CEI)layer and intermediate polysulfide shuttle effect.Thus,an optimized cathode-electrolyte interface along with optimized electrodes is required for overall improvement.Herein,we comprehensively outline the challenges and corresponding strategies,including electrolyte optimization to create a dense CEI layer,regulating the Li_(2)S deposition pattern,and inhibiting the shuttle effect with regard to the solid-liquid-solid pathway,the transformation from solid-liquid-solid to solid-solid pathway,and solid-solid pathway at the cathode-electrolyte interface.In order to spur more perceptive research and hasten the widespread use of lithium-sulfur batteries,viewpoints on designing a stable interface with a deep comprehension are also put forth.展开更多
In-situ polymer electrolytes prepared by Li salt-initiated polymerization are promising electrolytes for solid-state Li metal batteries owing to their enhanced interface contact and facile and green preparation proces...In-situ polymer electrolytes prepared by Li salt-initiated polymerization are promising electrolytes for solid-state Li metal batteries owing to their enhanced interface contact and facile and green preparation process.However,conventional in-situ polymer electrolytes suffer from poor interface stability,low mechanical strength,low oxidation stability,and certain flammability.Herein,a silsesquioxane(POSS)-nanocage-crosslinked in-situ polymer electrolyte(POSS-DOL@PI-F)regulated by fluorinated plasticizer and enhanced by polyimide skeleton is fabricated by Li salt initiated in-situ polymerization.Polyimide skeleton and POSS-nanocage-crosslinked network significantly enhance the tensile strength(22.8 MPa)and thermal stability(200℃)of POSS-DOL@PI-F.Fluorinated plasticizer improves ionic conductivity(6.83×10^(-4)S cm^(-1)),flame retardance,and oxidation stability(5.0 V)of POSS-DOL@PI-F.The fluorinated plasticizer of POSS-DOL@PI-F constructs robust LiF-rich solid electrolyte interphases and cathode electrolyte interphases,thereby dramatically enhancing the interface stability of Li metal anodes and LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811)cathodes.POSS-DOL@PI-F enables stable,long-term(1200 h),and dendrite-free cycle of Li‖Li cells.POSS-DOL@PI-F significantly boosts the performance of Li‖NCM811cells,which display superior cycle stability under harsh conditions of high voltage(4.5 V),high temperature(60℃),low temperature(-20℃),and high areal capacity.This work provides a rational design strategy for safe and efficient polymer electrolytes.展开更多
The anchoring capacity of the anchor cable is closely related to the bonding length and radial pressure conditions.Through field pull-out tests,theoretical analysis,numerical simulation,and industrial tests,this study...The anchoring capacity of the anchor cable is closely related to the bonding length and radial pressure conditions.Through field pull-out tests,theoretical analysis,numerical simulation,and industrial tests,this study clarifies the relationship between radial pressure and bonding length for the ultimate pullout force and reveals the microscopic failure process of the resin-rock interface in the anchoring system.The results show that the ultimate load increases with the increase of bonding length in three different stages:rapid,slow,and uniform growth.The new mechanical model developed considering radial pressure describes the inverse relationship between radial pressure and the plastic zone on the bonding section,and quantifies the reinforcing effect of confining pressure on the anchoring force.During the pull-out process of the anchor cable,the generation of failure cracks is in the order of orifice,bottom,and middle of the hole.Radial pressure can effectively enhance the ultimate pull-out force,alleviate the oscillation increase of pull-out force,and inhibit resin cracking,but will produce an external crushing zone.It also reveals the synergistic effect between bonding length and radial pressure,and successfully carries out industrial tests of anchor cable support,which ensures the stability of the stope roof and provides an important reference for the design of anchor cable support in deep high-stress mines.展开更多
The reversibility and stability of aqueous Zn metal batteries(AZMBs)are largely limited by Zn dendrites and interfacial parasitic reactions.Herein,we propose a parallel modulation strategy to boost the reversibility o...The reversibility and stability of aqueous Zn metal batteries(AZMBs)are largely limited by Zn dendrites and interfacial parasitic reactions.Herein,we propose a parallel modulation strategy to boost the reversibility of the Zn anode by introducing N,N,N',N'-tetramethylchloroformamidinium hexafluorophosphate(TCFH)as an additive in the electrolyte.TCFH is composed of PF6-and TN+with opposite charges.PF6-can spontaneously induce the in-situ generation of ZnF_(2)solid electrolyte interface(SEI)on the anode,which can improve the transport kinetics of Zn^(2+)at the interface,thus promoting the rapid and uniform deposition of Zn as well as inhibiting the growth of dendrites.In addition,TN+is enriched at the anode surface during Zn deposition through the anchoring effect,which brings a reconfiguration of the ion/molecule distribution.The anchored-TN+reduces the concentrations of H_(2)O and SO_(4)^(2-),sufficiently restraining the parasitic reaction.Thanks to the dual-phase interface engineering constructed of PF6-and TN+in parallel,the symmetric cell with the proposed electrolyte survives long cycling stability over750 h at 20 mA cm^(-2),10 mAh cm^(-2).This study offers a distinct viewpoint to the multidimensional optimization of Zn anodes for high-performance AZMBs.展开更多
All-solid-state batteries(ASSBs)assembled with sulfide solid electrolytes(SSEs)and nickel(Ni)-rich oxide cathode materials are expected to achieve high energy density and safety,representing potential candidates for t...All-solid-state batteries(ASSBs)assembled with sulfide solid electrolytes(SSEs)and nickel(Ni)-rich oxide cathode materials are expected to achieve high energy density and safety,representing potential candidates for the next-generation energy storage systems.However,interfacial issues between SSEs and Nirich oxide cathode materials,attributed to space charge layer,interfacial side reactions,and mechanical contact failure,significantly restrict the performances of ASSBs.The interface degradation is closely related to the components of the composite cathode and the process of electrode fabrication.Focusing on the influencing factors of interface compatibility between SSEs and Ni-rich oxide cathode,this article systematically discusses how cathode active materials(CAMs),electrolytes,conductive additives,binders,and electrode fabrication impact the interface compatibility.In addition,the strategies for the compatibility modification are reviewed.Furthermore,the challenges and prospects of intensive research on the degradation and modification of the SSE/Ni-rich cathode material interface are discussed.This review is intended to inspire the development of high-energy-density and high-safety all-solid-state batteries.展开更多
The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process o...The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.展开更多
Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogena...Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogenation reaction,involving surface carbonate hydrogenation and CO_(2)chemisorption.Nonetheless,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO_(2)conversion.This work demonstrated that the incorporation of CaH_(2)in Ni/CaCO_(3)enhances the CO_(2)methanation activity of the catalysts.The CO_(2)conversion for Ni/CaH_(2)-CaCO_(3)reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO_(3)(31.6%) and Ni/CaH_(2)-CaO (42.4%) catalysts.Furthermore,the Ni/CaH_(2)-CaCO_(3)catalysts remained stable during the stability test for 24 h at 400°C and 8 bar.Our research revealed that CaH_(2)played a crucial role in promoting the activity of the Ni-carbonate interface for CO_(2)methanation.CaH_(2)could modify the electronic structure of Ni and tune the structural properties of CaCO_(3)to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO_(2).In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO_(2)activation occurs at the hydroxyl group (OH) on the CaH_(2)-modified Ni-carbonate surface,leading to the formation of CO_(3)H*species.Furthermore,our study has confirmed that CO_(2)methanation over the Ni/CaH_(2)-CaCO_(3)catalysts proceeds via the formate pathway.展开更多
The growth of dendrites and the side reactions occurring at the Zn anode pose significant challenges to the commercialization of aqueous Zn-ion batteries(AZIBs). These challenges arise from the inherent conflict betwe...The growth of dendrites and the side reactions occurring at the Zn anode pose significant challenges to the commercialization of aqueous Zn-ion batteries(AZIBs). These challenges arise from the inherent conflict between mass transfer and electrochemical kinetics. In this study, we propose the use of a multifunctional electrolyte additive based on the xylose(Xylo) molecule to address these issues by modulating the solvation structure and electrode/electrolyte interface, thereby stabilizing the Zn anode. The introduction of the additive alters the solvation structure, creating steric hindrance that impedes charge transfer and then reduces electrochemical kinetics. Furthermore, in-situ analyses demonstrate that the reconstructed electrode/electrolyte interface facilitates stable and rapid Zn^(2+)ion migration and suppresses corrosion and hydrogen evolution reactions. As a result, symmetric cells incorporating the Xylo additive exhibit significantly enhanced reversibility during the Zn plating/stripping process, with an impressively long lifespan of up to 1986 h, compared to cells using pure ZnSO4electrolyte. When combined with a polyaniline cathode, the full cells demonstrate improved capacity and long-term cyclic stability. This work offers an effective direction for improving the stability of Zn anode via electrolyte design, as well as highperformance AZIBs.展开更多
The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of ...The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).展开更多
Electrical and thermal transport at two-dimensional(2D) interfaces is critical for semiconductor technology, yet their interplay remains unclear. We report a theoretical proposal to separate electronic and phononic co...Electrical and thermal transport at two-dimensional(2D) interfaces is critical for semiconductor technology, yet their interplay remains unclear. We report a theoretical proposal to separate electronic and phononic contributions to thermal conductance at 2D interfaces with graphene, which is validated by non-equilibrium Green's function calculations and molecular dynamics simulations for graphene–gold contacts. Our results reveal that while metal–graphene interfaces are transparent for both electrons and phonons, non-covalent graphene interfaces block electronic tunneling beyond two layers but not phonon transport. This suggests that the Wiedemann–Franz law can be experimentally tested by measuring transport across interfaces with varying graphene layers.展开更多
基金financially supported by the National Natural Science Foundation of China(No.52377026 and No.52301192)Taishan Scholars and Young Experts Program of Shandong Province(No.tsqn202103057)+4 种基金Postdoctoral Fellowship Program of CPSF under Grant Number(No.GZB20240327)Shandong Postdoctoral Science Foundation(No.SDCXZG-202400275)Qingdao Postdoctoral Application Research Project(No.QDBSH20240102023)China Postdoctoral Science Foundation(No.2024M751563)the Qingchuang Talents Induction Program of Shandong Higher Education Institution(Research and Innovation Team of Structural-Functional Polymer Composites).
文摘Currently,the demand for electromagnetic wave(EMW)absorbing materials with specific functions and capable of withstanding harsh environments is becoming increasingly urgent.Multi-component interface engineering is considered an effective means to achieve high-efficiency EMW absorption.However,interface modulation engineering has not been fully discussed and has great potential in the field of EMW absorption.In this study,multi-component tin compound fiber composites based on carbon fiber(CF)substrate were prepared by electrospinning,hydrothermal synthesis,and high-temperature thermal reduction.By utilizing the different properties of different substances,rich heterogeneous interfaces are constructed.This effectively promotes charge transfer and enhances interfacial polarization and conduction loss.The prepared SnS/SnS_(2)/SnO_(2)/CF composites with abundant heterogeneous interfaces have and exhibit excellent EMW absorption properties at a loading of 50 wt%in epoxy resin.The minimum reflection loss(RL)is−46.74 dB and the maximum effective absorption bandwidth is 5.28 GHz.Moreover,SnS/SnS_(2)/SnO_(2)/CF epoxy composite coatings exhibited long-term corrosion resistance on Q235 steel surfaces.Therefore,this study provides an effective strategy for the design of high-efficiency EMW absorbing materials in complex and harsh environments.
基金National Natural Science Foundation of China(32201491)Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)The authors extend their appreciation to the Deanship of Scientific Research at Northern Border University,Arar,KSA for funding this research work through the project number“NBU-FPEJ-2024-1101-02”.
文摘Research efforts on electromagnetic interference(EMI)shielding materials have begun to converge on green and sustainable biomass materials.These materials offer numerous advantages such as being lightweight,porous,and hierarchical.Due to their porous nature,interfacial compatibility,and electrical conductivity,biomass materials hold significant potential as EMI shielding materials.Despite concerted efforts on the EMI shielding of biomass materials have been reported,this research area is still relatively new compared to traditional EMI shielding materials.In particular,a more comprehensive study and summary of the factors influencing biomass EMI shielding materials including the pore structure adjustment,preparation process,and micro-control would be valuable.The preparation methods and characteristics of wood,bamboo,cellulose and lignin in EMI shielding field are critically discussed in this paper,and similar biomass EMI materials are summarized and analyzed.The composite methods and fillers of various biomass materials were reviewed.this paper also highlights the mechanism of EMI shielding as well as existing prospects and challenges for development trends in this field.
基金the financial support from the National Natural Science Foundation of China (No.42102127)the Postdoctoral Research Foundation of China (No.2024 M751860)。
文摘Cleat serves as the primary flow pathway for coalbed methane(CBM)and water.However,few studies consider the impact of local contact on two-phase flow within cleats.A visual generalized model of endogenous cleats was constructed based on microfluidics.A microscopic and mesoscopic observation technique was proposed to simultaneously capture gas-liquid interface morphology of pores and throat and the two-phase flow characteristics in entire cleat system.The local contact characteristics of cleats reduced absolute permeability,which resulted in a sharp increase in the starting pressure.The reduced gas flow capacity narrowed the co-infiltration area and decreased water saturation at the isotonic point in a hydrophilic environment.The increased local contact area of cleats weakened gas phase flow capacity and narrowed the co-infiltration area.Jumping events occurred in methane-water flow due to altered porosity caused by local contact in cleats.The distribution of residual phases changed the jumping direction on the micro-scale as well as the dominant channel on the mesoscale.Besides,jumping events caused additional energy dissipation,which was ignored in traditional two-phase flow models.This might contribute to the overestimation of relative permeability.The work provides new methods and insights for investigating unsaturated flow in complex porous media.
基金the National Key R&D Plan of the Ministry of Science and Technology of China(2022YFE0122400)National Natural Science Foundation of China(52002238,22102207)+1 种基金Science and Technology Commission of Shanghai Municipality(22ZR1423800,21ZR1465200,23ZR1423600)Shanghai Municipal Education Commission and the NSRF via the Program Management Unit for Human Resources&Institutional Development,Research and Innovation(B49G680115).
文摘Silicon stands as a key anode material in lithium-ion battery ascribing to its high energy density.Nevertheless,the poor rate performance and limited cycling life remain unresolved through conventional approaches that involve carbon composites or nanostructures,primarily due to the un-controllable effects arising from the substantial formation of a solid electrolyte interphase(SEI)during the cycling.Here,an ultra-thin and homogeneous Ti doping alumina oxide catalytic interface is meticulously applied on the porous Si through a synergistic etching and hydrolysis process.This defect-rich oxide interface promotes a selective adsorption of fluoroethylene carbonate,leading to a catalytic reaction that can be aptly described as“molecular concentration-in situ conversion”.The resultant inorganic-rich SEI layer is electrochemical stable and favors ion-transport,particularly at high-rate cycling and high temperature.The robustly shielded porous Si,with a large surface area,achieves a high initial Coulombic efficiency of 84.7%and delivers exceptional high-rate performance at 25 A g^(−1)(692 mAh g^(−1))and a high Coulombic efficiency of 99.7%over 1000 cycles.The robust SEI constructed through a precious catalytic layer promises significant advantages for the fast development of silicon-based anode in fast-charging batteries.
基金supported by the National Natural Science Foundation of China(Grant Nos.52102302,22409161 and 52472249)the Young Talent Support Plan of Xi’an Jiaotong University(Grant No.DQ6J011)+4 种基金the Natural Science Foundation of Shaanxi Province(2023-JC-QN-0115)the China Postdoctoral Science Foundation(2022M712499)Beilin District Science and Technology Plan(GX2328)the support from Young Elite Scientists Sponsorship Program by Chinese Association for Science and Technologythe“High-Level Talent Introduction Plan”of Shaanxi Province and Siyuan Scholar of Xi’an Jiaotong University。
文摘Global interest in lithium-sulfur batteries as one of the most promising energy storage technologies has been sparked by their low sulfur cathode cost,high gravimetric,volumetric energy densities,abundant resources,and environmental friendliness.However,their practical application is significantly impeded by several serious issues that arise at the cathode-electrolyte interface,such as interface structure degradation including the uneven deposition of Li_(2)S,unstable cathode-electrolyte interphase(CEI)layer and intermediate polysulfide shuttle effect.Thus,an optimized cathode-electrolyte interface along with optimized electrodes is required for overall improvement.Herein,we comprehensively outline the challenges and corresponding strategies,including electrolyte optimization to create a dense CEI layer,regulating the Li_(2)S deposition pattern,and inhibiting the shuttle effect with regard to the solid-liquid-solid pathway,the transformation from solid-liquid-solid to solid-solid pathway,and solid-solid pathway at the cathode-electrolyte interface.In order to spur more perceptive research and hasten the widespread use of lithium-sulfur batteries,viewpoints on designing a stable interface with a deep comprehension are also put forth.
基金supported by the National Natural Science Foundation of China(22375116,22001057)the Science Foundation of High-Level Talents of Wuyi University(2019AL017,2021AL002)Tianjin Lishen Battery Co.,Ltd。
文摘In-situ polymer electrolytes prepared by Li salt-initiated polymerization are promising electrolytes for solid-state Li metal batteries owing to their enhanced interface contact and facile and green preparation process.However,conventional in-situ polymer electrolytes suffer from poor interface stability,low mechanical strength,low oxidation stability,and certain flammability.Herein,a silsesquioxane(POSS)-nanocage-crosslinked in-situ polymer electrolyte(POSS-DOL@PI-F)regulated by fluorinated plasticizer and enhanced by polyimide skeleton is fabricated by Li salt initiated in-situ polymerization.Polyimide skeleton and POSS-nanocage-crosslinked network significantly enhance the tensile strength(22.8 MPa)and thermal stability(200℃)of POSS-DOL@PI-F.Fluorinated plasticizer improves ionic conductivity(6.83×10^(-4)S cm^(-1)),flame retardance,and oxidation stability(5.0 V)of POSS-DOL@PI-F.The fluorinated plasticizer of POSS-DOL@PI-F constructs robust LiF-rich solid electrolyte interphases and cathode electrolyte interphases,thereby dramatically enhancing the interface stability of Li metal anodes and LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM811)cathodes.POSS-DOL@PI-F enables stable,long-term(1200 h),and dendrite-free cycle of Li‖Li cells.POSS-DOL@PI-F significantly boosts the performance of Li‖NCM811cells,which display superior cycle stability under harsh conditions of high voltage(4.5 V),high temperature(60℃),low temperature(-20℃),and high areal capacity.This work provides a rational design strategy for safe and efficient polymer electrolytes.
基金Financial supports for this work,provided by the National Natural Science Foundation Project of China(No.52374152)the Guangxi Science and Technology Plan Project of China(No.2022AB31023)the National Basic Research Development Program of China(No.2022YFC2904602)are gratefully acknowledged。
文摘The anchoring capacity of the anchor cable is closely related to the bonding length and radial pressure conditions.Through field pull-out tests,theoretical analysis,numerical simulation,and industrial tests,this study clarifies the relationship between radial pressure and bonding length for the ultimate pullout force and reveals the microscopic failure process of the resin-rock interface in the anchoring system.The results show that the ultimate load increases with the increase of bonding length in three different stages:rapid,slow,and uniform growth.The new mechanical model developed considering radial pressure describes the inverse relationship between radial pressure and the plastic zone on the bonding section,and quantifies the reinforcing effect of confining pressure on the anchoring force.During the pull-out process of the anchor cable,the generation of failure cracks is in the order of orifice,bottom,and middle of the hole.Radial pressure can effectively enhance the ultimate pull-out force,alleviate the oscillation increase of pull-out force,and inhibit resin cracking,but will produce an external crushing zone.It also reveals the synergistic effect between bonding length and radial pressure,and successfully carries out industrial tests of anchor cable support,which ensures the stability of the stope roof and provides an important reference for the design of anchor cable support in deep high-stress mines.
基金financially supported by the National Natural Science Foundation of China(52172159)the Postdoctoral Fellowship Program of CPSF(GZB20230631).
文摘The reversibility and stability of aqueous Zn metal batteries(AZMBs)are largely limited by Zn dendrites and interfacial parasitic reactions.Herein,we propose a parallel modulation strategy to boost the reversibility of the Zn anode by introducing N,N,N',N'-tetramethylchloroformamidinium hexafluorophosphate(TCFH)as an additive in the electrolyte.TCFH is composed of PF6-and TN+with opposite charges.PF6-can spontaneously induce the in-situ generation of ZnF_(2)solid electrolyte interface(SEI)on the anode,which can improve the transport kinetics of Zn^(2+)at the interface,thus promoting the rapid and uniform deposition of Zn as well as inhibiting the growth of dendrites.In addition,TN+is enriched at the anode surface during Zn deposition through the anchoring effect,which brings a reconfiguration of the ion/molecule distribution.The anchored-TN+reduces the concentrations of H_(2)O and SO_(4)^(2-),sufficiently restraining the parasitic reaction.Thanks to the dual-phase interface engineering constructed of PF6-and TN+in parallel,the symmetric cell with the proposed electrolyte survives long cycling stability over750 h at 20 mA cm^(-2),10 mAh cm^(-2).This study offers a distinct viewpoint to the multidimensional optimization of Zn anodes for high-performance AZMBs.
基金financially supported by the National Natural Science Foundation of China(52072036,52272187)the China Petroleum&Chemical Corporation(SINOPEC)project(223128).
文摘All-solid-state batteries(ASSBs)assembled with sulfide solid electrolytes(SSEs)and nickel(Ni)-rich oxide cathode materials are expected to achieve high energy density and safety,representing potential candidates for the next-generation energy storage systems.However,interfacial issues between SSEs and Nirich oxide cathode materials,attributed to space charge layer,interfacial side reactions,and mechanical contact failure,significantly restrict the performances of ASSBs.The interface degradation is closely related to the components of the composite cathode and the process of electrode fabrication.Focusing on the influencing factors of interface compatibility between SSEs and Ni-rich oxide cathode,this article systematically discusses how cathode active materials(CAMs),electrolytes,conductive additives,binders,and electrode fabrication impact the interface compatibility.In addition,the strategies for the compatibility modification are reviewed.Furthermore,the challenges and prospects of intensive research on the degradation and modification of the SSE/Ni-rich cathode material interface are discussed.This review is intended to inspire the development of high-energy-density and high-safety all-solid-state batteries.
基金financial support provided by the Sichuan Science and Technology Program(No.2022NSFSC0226)Sichuan Science and Technology Program(No.2023ZYD0163)+6 种基金the Production-Education Integration Demonstration Project of Sichuan Provincethe Photovoltaic Industry Production-Education Integration Comprehensive Demonstration Base of Sichuan Province(Sichuan Financial Education[2022]No.106)China Tianfu Yongxing Laboratory Science and Technology Key Project(2023KJGG15)National Key Research and Development Program of China(2022YFB3803300)Beijing Natural Science Foundation(IS23037)the Department for Energy Security and Net Zero(project ID:NEXTCCUS)the ACT program(Accelerating CCS Technologies,Horizon2020 project NO.691712)。
文摘The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.
基金National Natural Science Foundation of China (Nos. 22371244 and 21573192)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX22_3463)。
文摘Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogenation reaction,involving surface carbonate hydrogenation and CO_(2)chemisorption.Nonetheless,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO_(2)conversion.This work demonstrated that the incorporation of CaH_(2)in Ni/CaCO_(3)enhances the CO_(2)methanation activity of the catalysts.The CO_(2)conversion for Ni/CaH_(2)-CaCO_(3)reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO_(3)(31.6%) and Ni/CaH_(2)-CaO (42.4%) catalysts.Furthermore,the Ni/CaH_(2)-CaCO_(3)catalysts remained stable during the stability test for 24 h at 400°C and 8 bar.Our research revealed that CaH_(2)played a crucial role in promoting the activity of the Ni-carbonate interface for CO_(2)methanation.CaH_(2)could modify the electronic structure of Ni and tune the structural properties of CaCO_(3)to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO_(2).In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO_(2)activation occurs at the hydroxyl group (OH) on the CaH_(2)-modified Ni-carbonate surface,leading to the formation of CO_(3)H*species.Furthermore,our study has confirmed that CO_(2)methanation over the Ni/CaH_(2)-CaCO_(3)catalysts proceeds via the formate pathway.
文摘The growth of dendrites and the side reactions occurring at the Zn anode pose significant challenges to the commercialization of aqueous Zn-ion batteries(AZIBs). These challenges arise from the inherent conflict between mass transfer and electrochemical kinetics. In this study, we propose the use of a multifunctional electrolyte additive based on the xylose(Xylo) molecule to address these issues by modulating the solvation structure and electrode/electrolyte interface, thereby stabilizing the Zn anode. The introduction of the additive alters the solvation structure, creating steric hindrance that impedes charge transfer and then reduces electrochemical kinetics. Furthermore, in-situ analyses demonstrate that the reconstructed electrode/electrolyte interface facilitates stable and rapid Zn^(2+)ion migration and suppresses corrosion and hydrogen evolution reactions. As a result, symmetric cells incorporating the Xylo additive exhibit significantly enhanced reversibility during the Zn plating/stripping process, with an impressively long lifespan of up to 1986 h, compared to cells using pure ZnSO4electrolyte. When combined with a polyaniline cathode, the full cells demonstrate improved capacity and long-term cyclic stability. This work offers an effective direction for improving the stability of Zn anode via electrolyte design, as well as highperformance AZIBs.
基金National Key R&D Program of China(2022YFE0105900)National Natural Science Foundation of China(52306179)+1 种基金Science and Technology Innovation Program of Hunan Province(2021RC4006)High Performance Computing Center of Central South University。
文摘The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 12425201 and 52090032)the National Key Basic Research Program of China (Grant No. 2022YFA1205400)。
文摘Electrical and thermal transport at two-dimensional(2D) interfaces is critical for semiconductor technology, yet their interplay remains unclear. We report a theoretical proposal to separate electronic and phononic contributions to thermal conductance at 2D interfaces with graphene, which is validated by non-equilibrium Green's function calculations and molecular dynamics simulations for graphene–gold contacts. Our results reveal that while metal–graphene interfaces are transparent for both electrons and phonons, non-covalent graphene interfaces block electronic tunneling beyond two layers but not phonon transport. This suggests that the Wiedemann–Franz law can be experimentally tested by measuring transport across interfaces with varying graphene layers.
