V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve th...V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve the stability,organic small molecule choline chloride intercalation is used to expand the spacing of the vanadium pentoxide layers and increase the cycling stability.Therefore,we consider the introduction of Sr^(2+)to cointercalate with choline chloride.Here,we synthes-ized vanadium pentoxide cointercalated with Sr^(2+)and choline ions(Ch^(+))via a simple hydrothermal method.The electro-chemical performance shows an enhanced cathode capacitance contribution of Sr&Ch-V_(2)O_(5),with a discharge capacity of 526 mAh·g^(-1)at 0.1 A·g^(-1)and a retention rate of 78.9%after 2000 cycles at 5 A·g^(-1).This work offers a novel strategy for the design of organic‒inorganic hybrid materials for use as cathodes in aqueous zinc-ion batteries.展开更多
Intercalation catalysis research involves inserting metal ions,molecules,or ionic liquids into the layered structure of catalysts to adjust their electronic structure and surface properties,thereby optimizing catalyti...Intercalation catalysis research involves inserting metal ions,molecules,or ionic liquids into the layered structure of catalysts to adjust their electronic structure and surface properties,thereby optimizing catalytic reaction efficiency and selectivity[1–3].This technique has achieved significant progress in areas such as electrocatalysis,catalytic cracking,and energy conversion,especially in reactions like hydrogen generation,oxygen reduction,nitrogen reduction,and carbon dioxide reduction[4–6].Intercalation catalysis can enhance catalyst activity and selectivity,but challenges remain regarding stability,reusability,and industrial application.Future research will focus on developing new intercalation materials,optimizing catalyst design,and exploring their potential applications in complex environments[7].展开更多
Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chlori...Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chloride oxidation reactions make oxygen evolution reaction(OER)in seawater extremely challenging.Herein,the low-cost and scalable CoFe layered double hydroxides with Cl^(-)intercalation and decorated with Ce(OH)_(3)(named as CoFe-Cl^(-)/Ce(OH)_(3))catalyst is synthesized via rapid electrodeposition under ambient conditions,which is quickly reconstructed into a CeO_(2)decorated and Cl^(-)intercalated CoFeOOH(CoFeOOH-Cl^(-)/CeO_(2))during OER.Theoretical investigation reveals that Cl^(-)intercalation weakens the adsorption ability of Cl^(-)on Co/Fe atoms and hinders unfavorable coupling with chloride,thereby preventing the chlorine corrosion process and enhancing catalytic stability and activity.The CeO_(2)with hard Lewis acidity preferentially binds to OH-with harder Lewis base to ensure the OH-rich microenvironment around catalyst even under high current operating conditions,thus further enhancing stability and improving OER activity.The functionalized CoFe-Cl^(-)/Ce(OH)_(3)delivers 1000 mA cm^(-2)current density at only 329 mV overpotential with excellent stability for 1000 h under alkaline seawater.Electrochemical experiments elucidate the OER catalytic mechanism in which CeO_(2)serves as a co-catalyst for enriching OH-and CoFeOOH-Cl^(-)is the active species.Our work is a substantial step towards achieving massive and sustainable production of hydrogen fuel from immense seawater.展开更多
Two-dimensional(2D)organic-inorganic hybrid perovskites(OIHPs)have been developed as promising candidates for photodetection,owing to their excellent semiconducting features and structural tunability.However,as an imp...Two-dimensional(2D)organic-inorganic hybrid perovskites(OIHPs)have been developed as promising candidates for photodetection,owing to their excellent semiconducting features and structural tunability.However,as an important parameter for photodetection,the photoresponsive range of 2D OIHPs is usually modulated by finite metal-halide combinations,constraining their further development.The emerging aromatic amine-based alternating-cations-interlayered(A-ACI)hybrid perovskites that exhibit excellent charge transport and additional interlayered structural designability,provide an extra solution for achieving ideal photoresponsive range.Herein,for the first time,the photoresponsive range is successfully broadened in A-ACI hybrid perovskites(NMA)_(4)(FA)_(2)Pb_(3)Br_(12)(2)remolding from(NMA)_(4)(MA)_(2)Pb_(3)Br_(12)(1)(NMA=N-methylbenzylaminium,FA=formamidinium and MA=methylammonium).Particularly,1 and 2adopt an unprecedented configuration that NMA and MA/FA are alternately arranged in the interlayer in a 4:2 manner.Importantly,2 exhibits a narrower bandgap than 1,which can be ascribed to the lowlying conduct band composed of intercalation FAπ*orbitals.Meanwhile,2 possesses a shorter interlayer distance and flatter inorganic skeleton,synergistically facilitating the wider photo-absorption range and further endowing a broadening photoresponsive range(70 nm).This research not only enriches the perovskite family but also provides insights into structure-property relationships.展开更多
Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performa...Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performance Mg cathode materials.Utilizing the common characteristics of various ionic intercalation-type electrodes,we design and train a Crystal Graph Convolutional Neural Network model that can accurately predict electrode voltages for various ions with mean absolute errors(MAE)between0.25 and 0.33 V.By deploying the trained model to stable Mg compounds from Materials Project and GNoME AI dataset,we identify 160 high voltage structures out of 15,308 candidates with voltages above3.0 V and volumetric capacity over 800 mA h/cm^(3).We further train a precise NequIP model to facilitate accurate and rapid simulations of Mg ionic conductivity.From the 160 high voltage structures,the machine learning molecular dynamics simulations have selected 23 cathode materials with both high energy density and high ionic conductivity.This Al-driven workflow dramatically boosts the efficiency and precision of material discovery for multivalent ion batteries,paving the way for advanced Mg battery development.展开更多
MnBi_(2)Te_(4),which is emerging as an intrinsic antiferromagnetic(AFM)topological insulator,provides a unique platform to investigate the interplay between magnetism and topology.Modulating its magnetic properties en...MnBi_(2)Te_(4),which is emerging as an intrinsic antiferromagnetic(AFM)topological insulator,provides a unique platform to investigate the interplay between magnetism and topology.Modulating its magnetic properties enables the observation of exotic quantum phenomena such as the quantum anomalous Hall effect,axion insulator states,and Majorana fermions.While the intercalation of Bi_(2)Te_(3)can tune its magnetism,synthesizing pure-phase MnBi_(2)Te_(4)with uniform Bi_(2)Te_(3)intercalation remains challenging,and the fixed interlayer spacing of Bi_(2)Te_(3)limits magnetic coupling tunability.Here,we utilize electrochemical organic molecule intercalation to expand the van der Waals gap of MnBi_(2)Te_(4)and modulate its magnetic properties.Through x-ray diffraction(XRD)characterizations,we confirm that the interlayer spacing of MnBi_(2)Te_(4)is expanded from 13.6°A to 30.5°A and 61.0°A by intercalating quaternary ammonium cations(THA^(+)and CTA^(+)),respectively.The THA-MnBi_(2)Te_(4)exhibits dual complex magnetic behavior,combining AFM ordering with a Neel temperature(T_(N))of 12 K and a small ferromagnetic hysteresis loop at 2 K.The CTA-MnBi_(2)Te_(4)shows robust ferromagnetism,with a Curie point(T_(C))of 15 K,similar to that of the MnBi_(2)Te_(4)monolayer.These results demonstrate that remarkable changes in the magnetic properties of MnBi_(2)Te_(4)can be achieved via electrochemical intercalation,providing new insights into manipulating magnetism in layered magnetic materials.展开更多
Orthorhombic Nb_(2)O_(5)(T-Nb_(2)O_(5))is attractive for fast-charging Li-ion batteries,but it is still hard to realize rapid charge transfer kinetics for Li-ion storage.Herein,F-doped T-Nb_(2)O_(5) microflowers(F-Nb_(...Orthorhombic Nb_(2)O_(5)(T-Nb_(2)O_(5))is attractive for fast-charging Li-ion batteries,but it is still hard to realize rapid charge transfer kinetics for Li-ion storage.Herein,F-doped T-Nb_(2)O_(5) microflowers(F-Nb_(2)O_(5))are rationally synthesized through topotactic conversion.Specifically,F-Nb_(2)O_(5) are assembled by single-crystal nanoflakes with nearly 97%exposed(100)facet,which maximizes the exposure of the feasible Li^(+)transport pathways along loosely packed 4g atomic layers to the electrolytes,thus effectively enhancing the Li^(+)-intercalation performance.Besides,the band gap of F-Nb_(2)O_(5) is reduced to 2.87 eV due to the doping of F atoms,leading to enhanced electrical conductivity.The synergetic effects between tailored exposed crystal facets,F-doping,and ultrathin building blocks,speed up the Li^(+)/electron transfer kinetics and improve the pseudocapacitive properties of F-Nb_(2)O_(5).Therefore,F-Nb_(2)O_(5) exhibit superior rate capability(210.8 and 164.9 mAh g^(-1) at 1 and 10 C,respectively)and good long-term 10 C cycling performance(132.7 mAh g^(-1) after 1500 cycles).展开更多
Metallic zinc is an ideal anode material owing to its high theoretical capacity(819 mAh·g^(-1)),ecofriendliness,low cost and high safety,which have driven fast development of Zn-ion batteries(ZIBs).However,the pr...Metallic zinc is an ideal anode material owing to its high theoretical capacity(819 mAh·g^(-1)),ecofriendliness,low cost and high safety,which have driven fast development of Zn-ion batteries(ZIBs).However,the practical application of current ZIBs is significantly restricted by irregular dendrite growth of zinc anode and the low working voltage(usually<2 V)of cathode materials.Herein,we report a high-voltage Zn-based dualion battery(DIB),which is constructed by a graphite cathode,a Zn anode,and 3 M LiPF_(6)in the ethyl methyl carbonate(EMC)electrolyte.Under the corrosion interaction of Li^(+)ions,Zn^(2+)can be easily dissolved from Zn anode into the electrolyte to enable dendrite-free Zn^(2+)plating/stripping at the anode.Moreover,an aqueous carboxymethyl cellulose(CMC)binder is employed to generate a robust cathode electrolyte interface(CEI)layer on the graphite cathode,which renders ultrafast PF_(6)^(-)-de-/intercalation into graphite.The resultant Zn-graphite DIB operates stably at a high cut off voltage of 3.2 V,corresponding to an average output voltage of 2.2 V.After 9000cycles at 5C,the high capacity retention of 95.9% can be achieved with~100% Coulomb efficiency.Based on the mass of cathode material,our Zn-graphite battery exhibits ultrafast rate capability(60 C,a discharge time of 44 s)and high energy/power densities(208 Wh·kg^(-1)at 214 W·kg^(-1);142 Wh·kg^(-1)at 8692 W·kg^(-1)),which holds great promise for large-scale energy storage.展开更多
Developing anode materials with high specific/volumetric capacities,high-rate capability,long-term cycles and low cost is significant for advanced sodium-ion storage.Herein,we report the hybrid TiO_(2)/graphite(TiO_(2...Developing anode materials with high specific/volumetric capacities,high-rate capability,long-term cycles and low cost is significant for advanced sodium-ion storage.Herein,we report the hybrid TiO_(2)/graphite(TiO_(2)/G)anodes for fast(dis)charging sodium-ion storage.Taking advantage of the rapid pseudocapacitive surface-redox on anatase TiO_(2)nanoparticles(NPs)and fast[Na(diglyme)_(x)]^(+)co-intercalation into graphite,the hybrid anodes display excellent rate capabilities.Additionally,the TiO_(2)NPs are able to fill into the interspaces among graphite flakes and the graphite provides continuous electron pathways,which largely boosts the volumetric capacities and rate performance.展开更多
The typical metal chloride-graphite intercalation compounds(MC-GICs)inherit intercalation capacity,high charge conductivity,and high tap density from graphite,and these are considered as one of the promising alternati...The typical metal chloride-graphite intercalation compounds(MC-GICs)inherit intercalation capacity,high charge conductivity,and high tap density from graphite,and these are considered as one of the promising alternatives of graphite anode in rechargeable metal-ion batteries(MIBs).Notably,the special interlayer decoupling effects and the introduction of extra conversion capacity by metal chloride could greatly break the capacity limitation of graphite anodes and achieve higher energy density in MIBs.The optimization of both graphite host and metal chloride species with specific structures endows MC-GICs with design feasibility for different application requirements of different MIBs,such as several times the actual capacity compared to graphite anodes,rapid migration of large carriers,and other properties.Herein,a brief review has been provided with the latest understanding of conductivity characteristics and energy storage mechanisms of MC-GICs and their interesting performance features of full potential application in rechargeable MIBs.Based on the existing research of MC-GICs,necessary improvements and prospects in the near future have been put forward.展开更多
Highly dispersed tungsten carbide（WC） nanoparticles（NPs） sandwiched between few-layer reduced graphene oxide（RGO） have been successfully synthesized by using thiourea as an anchoring and inducing reagent.The met...Highly dispersed tungsten carbide（WC） nanoparticles（NPs） sandwiched between few-layer reduced graphene oxide（RGO） have been successfully synthesized by using thiourea as an anchoring and inducing reagent.The metatungstate ion,[H2W（12）O（40）]^6-,is assembled on thiourea-modified graphene oxide（GO） by an impregnation method.The WC NPs,with a mean diameter of 1.5 nm,are obtained through a process whereby ammonium metatungstate first turns to WS2,which then forms an intercalation compound with RGO before growing,in situ,to WC NPs.The Pt/WC-RGO electrocatalysts are fabricated by a microwave-assisted method.The intimate contacts between Pt,WC,and RGO are confirmed by X-ray diffraction,scanning electron microscope,transmission electron microscope,and Raman spectroscopy.For methanol oxidation,the Pt/WC-RGO electrocatalyst exhibited an electrochemical surface area value of 246.1 m^2/g Pt and a peak current density of1364.7 mA/mg Pt,which are,respectively,3.66 and 4.77 times greater than those of commercial Pt/C electrocatalyst（67.2 m^2/g Pt,286.0 mA/mg Pt）.The excellent CO-poisoning resistance and long-term stability of the electrocatalyst are also evidenced by CO stripping,chronoamperometry,and accelerated durability testing.Because Pt/WC-RGO has higher catalytic activity compared with that of commercial Pt/C,as a result of its intercalated structure and synergistic effect,less Pt will be required for the same performance,which in turn will reduce the cost of the fuel cell.The present method is facile,efficient,and scalable for mass production of the nanomaterials.展开更多
文摘V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve the stability,organic small molecule choline chloride intercalation is used to expand the spacing of the vanadium pentoxide layers and increase the cycling stability.Therefore,we consider the introduction of Sr^(2+)to cointercalate with choline chloride.Here,we synthes-ized vanadium pentoxide cointercalated with Sr^(2+)and choline ions(Ch^(+))via a simple hydrothermal method.The electro-chemical performance shows an enhanced cathode capacitance contribution of Sr&Ch-V_(2)O_(5),with a discharge capacity of 526 mAh·g^(-1)at 0.1 A·g^(-1)and a retention rate of 78.9%after 2000 cycles at 5 A·g^(-1).This work offers a novel strategy for the design of organic‒inorganic hybrid materials for use as cathodes in aqueous zinc-ion batteries.
文摘Intercalation catalysis research involves inserting metal ions,molecules,or ionic liquids into the layered structure of catalysts to adjust their electronic structure and surface properties,thereby optimizing catalytic reaction efficiency and selectivity[1–3].This technique has achieved significant progress in areas such as electrocatalysis,catalytic cracking,and energy conversion,especially in reactions like hydrogen generation,oxygen reduction,nitrogen reduction,and carbon dioxide reduction[4–6].Intercalation catalysis can enhance catalyst activity and selectivity,but challenges remain regarding stability,reusability,and industrial application.Future research will focus on developing new intercalation materials,optimizing catalyst design,and exploring their potential applications in complex environments[7].
基金financial support from the National Natural Science Foundation of China(52372173,52072034)。
文摘Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chloride oxidation reactions make oxygen evolution reaction(OER)in seawater extremely challenging.Herein,the low-cost and scalable CoFe layered double hydroxides with Cl^(-)intercalation and decorated with Ce(OH)_(3)(named as CoFe-Cl^(-)/Ce(OH)_(3))catalyst is synthesized via rapid electrodeposition under ambient conditions,which is quickly reconstructed into a CeO_(2)decorated and Cl^(-)intercalated CoFeOOH(CoFeOOH-Cl^(-)/CeO_(2))during OER.Theoretical investigation reveals that Cl^(-)intercalation weakens the adsorption ability of Cl^(-)on Co/Fe atoms and hinders unfavorable coupling with chloride,thereby preventing the chlorine corrosion process and enhancing catalytic stability and activity.The CeO_(2)with hard Lewis acidity preferentially binds to OH-with harder Lewis base to ensure the OH-rich microenvironment around catalyst even under high current operating conditions,thus further enhancing stability and improving OER activity.The functionalized CoFe-Cl^(-)/Ce(OH)_(3)delivers 1000 mA cm^(-2)current density at only 329 mV overpotential with excellent stability for 1000 h under alkaline seawater.Electrochemical experiments elucidate the OER catalytic mechanism in which CeO_(2)serves as a co-catalyst for enriching OH-and CoFeOOH-Cl^(-)is the active species.Our work is a substantial step towards achieving massive and sustainable production of hydrogen fuel from immense seawater.
基金financially supported by the National Natural Science Foundation of China(Nos.22435005,22193042,21921001,52202194,22305105,22201284)the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(No.ZDBSLY-SLH024)。
文摘Two-dimensional(2D)organic-inorganic hybrid perovskites(OIHPs)have been developed as promising candidates for photodetection,owing to their excellent semiconducting features and structural tunability.However,as an important parameter for photodetection,the photoresponsive range of 2D OIHPs is usually modulated by finite metal-halide combinations,constraining their further development.The emerging aromatic amine-based alternating-cations-interlayered(A-ACI)hybrid perovskites that exhibit excellent charge transport and additional interlayered structural designability,provide an extra solution for achieving ideal photoresponsive range.Herein,for the first time,the photoresponsive range is successfully broadened in A-ACI hybrid perovskites(NMA)_(4)(FA)_(2)Pb_(3)Br_(12)(2)remolding from(NMA)_(4)(MA)_(2)Pb_(3)Br_(12)(1)(NMA=N-methylbenzylaminium,FA=formamidinium and MA=methylammonium).Particularly,1 and 2adopt an unprecedented configuration that NMA and MA/FA are alternately arranged in the interlayer in a 4:2 manner.Importantly,2 exhibits a narrower bandgap than 1,which can be ascribed to the lowlying conduct band composed of intercalation FAπ*orbitals.Meanwhile,2 possesses a shorter interlayer distance and flatter inorganic skeleton,synergistically facilitating the wider photo-absorption range and further endowing a broadening photoresponsive range(70 nm).This research not only enriches the perovskite family but also provides insights into structure-property relationships.
基金supported by the National Key R&D Program of China(2022YFA1203400)the National Natural Science Foundation of China(W2441009)。
文摘Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performance Mg cathode materials.Utilizing the common characteristics of various ionic intercalation-type electrodes,we design and train a Crystal Graph Convolutional Neural Network model that can accurately predict electrode voltages for various ions with mean absolute errors(MAE)between0.25 and 0.33 V.By deploying the trained model to stable Mg compounds from Materials Project and GNoME AI dataset,we identify 160 high voltage structures out of 15,308 candidates with voltages above3.0 V and volumetric capacity over 800 mA h/cm^(3).We further train a precise NequIP model to facilitate accurate and rapid simulations of Mg ionic conductivity.From the 160 high voltage structures,the machine learning molecular dynamics simulations have selected 23 cathode materials with both high energy density and high ionic conductivity.This Al-driven workflow dramatically boosts the efficiency and precision of material discovery for multivalent ion batteries,paving the way for advanced Mg battery development.
基金supported by the National Key Research and Development Program of China(Grant Nos.2022YFA1402404 and 2023YFA1406304)the National Natural Science Foundation of China(Grant Nos.92161201,T2221003,12104221,12104220,12274208,12025404,12004174,91961101,T2394473,62274085,12374043,and U2032208)+1 种基金the Natural Science Foundation of Jiangsu Province(Grant Nos.BK20230079,BK20243013,and BK20233001)the Fundamental Research Funds for the Central Universities(Grant Nos.020414380192 and 2024300432).
文摘MnBi_(2)Te_(4),which is emerging as an intrinsic antiferromagnetic(AFM)topological insulator,provides a unique platform to investigate the interplay between magnetism and topology.Modulating its magnetic properties enables the observation of exotic quantum phenomena such as the quantum anomalous Hall effect,axion insulator states,and Majorana fermions.While the intercalation of Bi_(2)Te_(3)can tune its magnetism,synthesizing pure-phase MnBi_(2)Te_(4)with uniform Bi_(2)Te_(3)intercalation remains challenging,and the fixed interlayer spacing of Bi_(2)Te_(3)limits magnetic coupling tunability.Here,we utilize electrochemical organic molecule intercalation to expand the van der Waals gap of MnBi_(2)Te_(4)and modulate its magnetic properties.Through x-ray diffraction(XRD)characterizations,we confirm that the interlayer spacing of MnBi_(2)Te_(4)is expanded from 13.6°A to 30.5°A and 61.0°A by intercalating quaternary ammonium cations(THA^(+)and CTA^(+)),respectively.The THA-MnBi_(2)Te_(4)exhibits dual complex magnetic behavior,combining AFM ordering with a Neel temperature(T_(N))of 12 K and a small ferromagnetic hysteresis loop at 2 K.The CTA-MnBi_(2)Te_(4)shows robust ferromagnetism,with a Curie point(T_(C))of 15 K,similar to that of the MnBi_(2)Te_(4)monolayer.These results demonstrate that remarkable changes in the magnetic properties of MnBi_(2)Te_(4)can be achieved via electrochemical intercalation,providing new insights into manipulating magnetism in layered magnetic materials.
基金supported by the National Natural Science Foundation of China(No.51802163)the Natural Science Foundation of Henan Province of China(No.222300420252)the Natural Science Foundation of Henan Department of Education(No.20A480004).
文摘Orthorhombic Nb_(2)O_(5)(T-Nb_(2)O_(5))is attractive for fast-charging Li-ion batteries,but it is still hard to realize rapid charge transfer kinetics for Li-ion storage.Herein,F-doped T-Nb_(2)O_(5) microflowers(F-Nb_(2)O_(5))are rationally synthesized through topotactic conversion.Specifically,F-Nb_(2)O_(5) are assembled by single-crystal nanoflakes with nearly 97%exposed(100)facet,which maximizes the exposure of the feasible Li^(+)transport pathways along loosely packed 4g atomic layers to the electrolytes,thus effectively enhancing the Li^(+)-intercalation performance.Besides,the band gap of F-Nb_(2)O_(5) is reduced to 2.87 eV due to the doping of F atoms,leading to enhanced electrical conductivity.The synergetic effects between tailored exposed crystal facets,F-doping,and ultrathin building blocks,speed up the Li^(+)/electron transfer kinetics and improve the pseudocapacitive properties of F-Nb_(2)O_(5).Therefore,F-Nb_(2)O_(5) exhibit superior rate capability(210.8 and 164.9 mAh g^(-1) at 1 and 10 C,respectively)and good long-term 10 C cycling performance(132.7 mAh g^(-1) after 1500 cycles).
基金financially supported by the National Natural Science Foundation of China(No.22279122)Shenzhen Science and Technology Program(No.JCYJ20220530162402005)+2 种基金the Research on High Power Flexible Battery in All Sea Depth(2020-XXXX-XX-246-00)the Research Fund Program of Hubei Key Laboratory of Resources and EcoEnvironment Geology(No.HBREGKFJJ-202314)and the Fundamental Research Funds for the Central Universities,South-Central Minzu University(No.CZQ21013)。
文摘Metallic zinc is an ideal anode material owing to its high theoretical capacity(819 mAh·g^(-1)),ecofriendliness,low cost and high safety,which have driven fast development of Zn-ion batteries(ZIBs).However,the practical application of current ZIBs is significantly restricted by irregular dendrite growth of zinc anode and the low working voltage(usually<2 V)of cathode materials.Herein,we report a high-voltage Zn-based dualion battery(DIB),which is constructed by a graphite cathode,a Zn anode,and 3 M LiPF_(6)in the ethyl methyl carbonate(EMC)electrolyte.Under the corrosion interaction of Li^(+)ions,Zn^(2+)can be easily dissolved from Zn anode into the electrolyte to enable dendrite-free Zn^(2+)plating/stripping at the anode.Moreover,an aqueous carboxymethyl cellulose(CMC)binder is employed to generate a robust cathode electrolyte interface(CEI)layer on the graphite cathode,which renders ultrafast PF_(6)^(-)-de-/intercalation into graphite.The resultant Zn-graphite DIB operates stably at a high cut off voltage of 3.2 V,corresponding to an average output voltage of 2.2 V.After 9000cycles at 5C,the high capacity retention of 95.9% can be achieved with~100% Coulomb efficiency.Based on the mass of cathode material,our Zn-graphite battery exhibits ultrafast rate capability(60 C,a discharge time of 44 s)and high energy/power densities(208 Wh·kg^(-1)at 214 W·kg^(-1);142 Wh·kg^(-1)at 8692 W·kg^(-1)),which holds great promise for large-scale energy storage.
基金financially supported by the National Natural Science Foundation of China(No.22179113)the Fundamental Research Funds for the Central Universities(Nos.20720230028 and 20720210045)+1 种基金the Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM)(No.HRTP-2022-19)the XMU Training Program of Innovation and Entrepreneurship for Undergraduates(No.2021Y1089)。
文摘Developing anode materials with high specific/volumetric capacities,high-rate capability,long-term cycles and low cost is significant for advanced sodium-ion storage.Herein,we report the hybrid TiO_(2)/graphite(TiO_(2)/G)anodes for fast(dis)charging sodium-ion storage.Taking advantage of the rapid pseudocapacitive surface-redox on anatase TiO_(2)nanoparticles(NPs)and fast[Na(diglyme)_(x)]^(+)co-intercalation into graphite,the hybrid anodes display excellent rate capabilities.Additionally,the TiO_(2)NPs are able to fill into the interspaces among graphite flakes and the graphite provides continuous electron pathways,which largely boosts the volumetric capacities and rate performance.
基金National Natural Science Foundation of China,Grant/Award Number:22309062Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2022A1515110052Jihua Laboratory,Grant/Award Numbers:X200191TL200,X220301XS220。
文摘The typical metal chloride-graphite intercalation compounds(MC-GICs)inherit intercalation capacity,high charge conductivity,and high tap density from graphite,and these are considered as one of the promising alternatives of graphite anode in rechargeable metal-ion batteries(MIBs).Notably,the special interlayer decoupling effects and the introduction of extra conversion capacity by metal chloride could greatly break the capacity limitation of graphite anodes and achieve higher energy density in MIBs.The optimization of both graphite host and metal chloride species with specific structures endows MC-GICs with design feasibility for different application requirements of different MIBs,such as several times the actual capacity compared to graphite anodes,rapid migration of large carriers,and other properties.Herein,a brief review has been provided with the latest understanding of conductivity characteristics and energy storage mechanisms of MC-GICs and their interesting performance features of full potential application in rechargeable MIBs.Based on the existing research of MC-GICs,necessary improvements and prospects in the near future have been put forward.
基金supported by the International Science & Technology Cooperation Program of China(2010DFB63680)the National Natural Science Foundation of China(21376220)Zhejiang Provincial Natural Science Foundation of China(LY16B060009,LY12B03008)~~
文摘Highly dispersed tungsten carbide（WC） nanoparticles（NPs） sandwiched between few-layer reduced graphene oxide（RGO） have been successfully synthesized by using thiourea as an anchoring and inducing reagent.The metatungstate ion,[H2W（12）O（40）]^6-,is assembled on thiourea-modified graphene oxide（GO） by an impregnation method.The WC NPs,with a mean diameter of 1.5 nm,are obtained through a process whereby ammonium metatungstate first turns to WS2,which then forms an intercalation compound with RGO before growing,in situ,to WC NPs.The Pt/WC-RGO electrocatalysts are fabricated by a microwave-assisted method.The intimate contacts between Pt,WC,and RGO are confirmed by X-ray diffraction,scanning electron microscope,transmission electron microscope,and Raman spectroscopy.For methanol oxidation,the Pt/WC-RGO electrocatalyst exhibited an electrochemical surface area value of 246.1 m^2/g Pt and a peak current density of1364.7 mA/mg Pt,which are,respectively,3.66 and 4.77 times greater than those of commercial Pt/C electrocatalyst（67.2 m^2/g Pt,286.0 mA/mg Pt）.The excellent CO-poisoning resistance and long-term stability of the electrocatalyst are also evidenced by CO stripping,chronoamperometry,and accelerated durability testing.Because Pt/WC-RGO has higher catalytic activity compared with that of commercial Pt/C,as a result of its intercalated structure and synergistic effect,less Pt will be required for the same performance,which in turn will reduce the cost of the fuel cell.The present method is facile,efficient,and scalable for mass production of the nanomaterials.
