Room temperature sodium-sulfur(Na-S)batteries,known for their high energy density and low cost,are one of the most promising next-generation energy storage systems.However,the polysulfide shuttling and uncontrollable ...Room temperature sodium-sulfur(Na-S)batteries,known for their high energy density and low cost,are one of the most promising next-generation energy storage systems.However,the polysulfide shuttling and uncontrollable Na dendrite growth as well as safety issues caused by the use of organic liquid electrolytes in Na-S cells,have severely hindered their commercialization.Solid-state electrolytes instead of liquid electrolytes are considered to be the most direct and effective solution to solve the above problems.However,its practical application is still greatly challenged due to the poor interfacial compatibility between the all-solid-state electrolytes and the anode/cathode,ionic conductivity,and the shuttle effect caused by the presence of liquid phase in the quasi-solid-state electrolytes.This paper presents a comprehensive review of solid-state Na-S batteries from the perspective of regulating interfacial compatibility and improving ionic conductivity as well as suppressing polysulfide shuttle.According to different components,solid-state electrolytes were divided into five categories:solid inorganic electrolytes,solid polymer electrolytes,polymer/inorganic solid hybrid electrolytes,gel polymer electrolytes,and liquid–solid inorganic hybrid electrolytes.Finally,the prospect of developing high performance solid-state electrolytes to improve the cycling stability of room temperature Na-S cells is envisaged.展开更多
This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and ...This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and status are investigated.A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio(72%S).In contrast,a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio(44%S).In carbonate ester electrolyte,only the sulfur trapped in porous structures is active via‘solid-solid’behavior during cycling.The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents.To improve the capacity of the sulfur-rich cathode,ether electrolyte with NaNO_(3) additive is explored to realize a‘solid-liquid’sulfur redox process and confine the shuttle effect of the dissolved polysulfides.As a result,the sulfur-rich cathode achieved high reversible capacity(483 mAh g^(−1)),corresponding to a specific energy of 362 Wh kg^(−1) after 200 cycles,shedding light on the use of ether electrolyte for high-loading sulfur cathode.展开更多
Room temperature sodium-sulfur(RT Na-S)batteries are gaining extensive attention as attractive alternatives for large-scale energy storage,due to low cost and high abundancy of sodium and sulfur in nature.However,the ...Room temperature sodium-sulfur(RT Na-S)batteries are gaining extensive attention as attractive alternatives for large-scale energy storage,due to low cost and high abundancy of sodium and sulfur in nature.However,the dilemmas regarding soluble polysulfides(Na_(2)Sn,4<n<8)and the inferior reaction kinetics limit their practical application.To address these issues,we report the activated porous carbon fibers(APCF)with small sulfur molecules(S2-4)confined in ultramicropores,to achieve a reversible single-step reaction in RT Na-S batteries.The mechanism is investigated by the in situ UV/vis spectroscopy,which demonstrates Na2S is the only product during the whole discharge process.Moreover,the hierarchical carbon structure can enhance areal sulfur loading without sacrificing the capacity due to thorough contact between electrolyte and sulfur electrode.As a consequence,the APCF electrode with 38 wt%sulfur(APCF-38S)delivers a high initial reversible specific capacity of 1412 mAh g^(-1) and 10.6mAh cm^(-2)(avg.areal sulfur loading:7.5 mg cm^(-2))at 0.1 C(1C=1675 mA g^(-1)),revealing high degree of sulfur utilization.This study provides a new strategy for the development of high areal capacity RT Na-S batteries.展开更多
Sluggish polysulfide redox kinetics,especially the high energy barrier of rate-determining short-chain polysulfide conversion and the high activation barrier of Na_(2)S decomposition during sulfur recovery,compromise ...Sluggish polysulfide redox kinetics,especially the high energy barrier of rate-determining short-chain polysulfide conversion and the high activation barrier of Na_(2)S decomposition during sulfur recovery,compromise the full potential of rechargeable Na-S electrochemistry.Herein we construct the hierarchical sandwich-structured carbon matrix with atomically dispersed Mn-N4 Lewis acidic sites,taking advantage of their bidirectional electrocatalytic behavior toward interface-mediated reversible sulfur redox.Experimental and theoretical results reveal that the spatial confinement and catalytic effects facilitated via strong Lewis acid-base electron interactions synergistically manipulate the low kinetically direct Na_(2)S_(4) to Na_(2)S conversion,and the formation of Mn-S bond minimizes the energy barrier of Na_(2)S electrochemical activation during battery recharging,thereby rendering a reversible and tunable polysulfide speciation pathway.Furthermore,the degradation of the Na-S cell is due to the depletion of metal anode rather than the loss of active sulfur species and/or aggregation of inactive dead sulfur.As expected,the S@Mn/NC cathode delivers outstanding rate capability and ultrahigh cycling stability.Simultaneously,a proof-of-concept pouch cell was also demonstrated capable of delivering an energy density up to 840 Wh kgcathode−1.The tunable sulfur redox electrochemistry invoked by the bidirectional monodispersed Mn catalytic hot spots facilitates the efficient polysulfide speciation for practical Na-S cells.展开更多
Rechargeable room temperature sodium–sulfur(RT Na–S)batteries are seriously limited by low sulfur utilization and sluggish electrochemical reaction activity of polysulfide intermediates.Herein,a 3D“branch-leaf”bio...Rechargeable room temperature sodium–sulfur(RT Na–S)batteries are seriously limited by low sulfur utilization and sluggish electrochemical reaction activity of polysulfide intermediates.Herein,a 3D“branch-leaf”biomimetic design proposed for high performance Na–S batteries,where the leaves constructed from Co nanoparticles on carbon nanofibers(CNF)are fully to expose the active sites of Co.The CNF network acts as conductive“branches”to ensure adequate electron and electrolyte supply for the Co leaves.As an effective electrocatalytic battery system,the 3D“branch-leaf”conductive network with abundant active sites and voids can effectively trap polysulfides and provide plentiful electron/ions pathways for electrochemical reaction.DFT calculation reveals that the Co nanoparticles can induce the formation of a unique Co–S–Na molecular layer on the Co surface,which can enable a fast reduction reaction of the polysulfides.Therefore,the prepared“branch-leaf”CNF-L@Co/S electrode exhibits a high initial specific capacity of 1201 mAh g^−1 at 0.1 C and superior rate performance.展开更多
Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,t...Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.展开更多
Rechargeable room-temperature sodium–sulfur(Na–S)and sodium–selenium(Na–Se)batteries are gaining extensive attention for potential large-scale energy storage applications owing to their low cost and high theoretic...Rechargeable room-temperature sodium–sulfur(Na–S)and sodium–selenium(Na–Se)batteries are gaining extensive attention for potential large-scale energy storage applications owing to their low cost and high theoretical energy density.Optimization of electrode materials and investigation of mechanisms are essential to achieve high energy density and long-term cycling stability of Na–S(Se)batteries.Herein,we provide a comprehensive review of the recent progress in Na–S(Se)batteries.We elucidate the Na storage mechanisms and improvement strategies for battery performance.In particular,we discuss the advances in the development of battery components,including high-performance sulfur cathodes,optimized electrolytes,advanced Na metal anodes and modified separators.Combined with current research achievements,this review outlines remaining challenges and clear research directions for the future development of practical high-performance Na–S(Se)batteries.展开更多
Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metalsulfur batteries.Motivated by a theoretical prediction,herein,we strategically propose nitrogenvacancy tantalum nit...Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metalsulfur batteries.Motivated by a theoretical prediction,herein,we strategically propose nitrogenvacancy tantalum nitride(Ta3N5-x)impregnated inside the interconnected nanopores of nitrogendecorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in roomtemperature sodium-sulfur batteries.Through a pore-constriction mechanism,the nitrogen vacancies are controllably constructed during the nucleation of Ta3N5-x.The defect manipulation on the local environment enables well-regulated Ta 5d-orbital energy level,not only modulating band structure toward enhanced intrinsic conductivity of Ta-based materials,but also promoting polysulfide stabilization and achieving bifunctional catalytic capability toward completely reversible polysulfide conversion.Moreover,the interconnected continuous Ta3N5-x-in-pore structure facilitates electron and sodium-ion transport and accommodates volume expansion of sulfur species while suppressing their shuttle behavior.Due to these attributes,the as-developed Ta3N5-x-based electrode achieves superior rate capability of 730 mAh g-1 at 3.35 A g-1,long-term cycling stability over 2000 cycles,and high areal capacity over 6 mAh cm-2 under high sulfur loading of 6.2 mg cm-2.This work not only presents a new sulfur electrocatalyst candidate for metal-sulfur batteries,but also sheds light on the controllable material design of defect structure in hopes of inspiring new ideas and directions for future research.展开更多
Sodium-sulfur(Na–S)batteries that utilize earth-abundant materials of Na and S have been one of the hottest topics in battery research.The low cost and high energy density make them promising candidates for next-gene...Sodium-sulfur(Na–S)batteries that utilize earth-abundant materials of Na and S have been one of the hottest topics in battery research.The low cost and high energy density make them promising candidates for next-generation storage technologies as required in the grid and renewable energy.In recent years,extensive efforts have been devoted to the diversity and functionalities of Na–S batteries,aiming to extend their potential applications across multiple temporal and spatial dimensions.Here,we summarize the unconventional designs for the functionalities of Na–S batteries such as flexible batteries,solid-state cells,flame resistance,and operation at extreme temperatures.By highlighting these design strategies that help to realize the functionalities,we hope this review offers a pathway to foster the bright future of Na–S batteries in diverse applications.展开更多
In 2011,a new class of 2D materials was discovered;after 2012,they began to be concerned;in 2017,the“gold rush”of the materials was triggered,and they are exactly MXenes.2D MXenes,a new class of transition metal car...In 2011,a new class of 2D materials was discovered;after 2012,they began to be concerned;in 2017,the“gold rush”of the materials was triggered,and they are exactly MXenes.2D MXenes,a new class of transition metal carbides,carbonitrides and nitrides,have become the star and cutting-edge research materials in the field of emerging batteries systems due to their unique 2D structure,abundant surface chemistry,and excellent physical and electrochemical properties.This review focuses on the MXene materials and summarizes the recent advancements in the synthesis techniques and properties,in addition to a detailed discussion on the electrochemical energy storage applications,including alkali-ion(Li^(+),Na^(+),K^(+))storage,lithium-sulfur(Li–S)batteries,sodiumsulfur(Na–S)batteries,and metal anode protection.Special attentions are given to the elaborate design of nano-micro structures of MXenes for the various roles as electrodes,multifunctional components,S hosts,modified separators,and metal anode protective layers.The paper ends with a prospective summary of the promising research directions in terms of synthesis,structure,properties,analysis,and production on MXene materials.展开更多
Promising room-temperature sodium-sulfur(RT Na-S)battery systems rely on purposely designed highperforming and low-cost electrode materials.Nevertheless,there are the challenges of irreversible dissolution and slow re...Promising room-temperature sodium-sulfur(RT Na-S)battery systems rely on purposely designed highperforming and low-cost electrode materials.Nevertheless,there are the challenges of irreversible dissolution and slow redox kinetics of NaPSs in the complete discharge of sulfur capacity.Herein,engineered CoMoO_(4)in reduced graphene oxide(CoMoO_(4)@rGO)is reported as a class of superior cathode hosts for RT Na-S batteries.The CoMoO_(4)@rGO matrix is designed to facilitate the reversible sodiation and desodiation of sulfur,considering the strong chemisorption between sulfur(and short-chain sodium sulfides)and CoMoO_(4),which alleviates the shuttle effect of sodium sulfides and accelerates the electrochemical reaction rate at RT.The obtained S/CoMoO_(4)@rGO cathode with~52%S loading exhibits a high capacity of520.1 mA h g^(-1)after 100 cycles at 0.1 A g^(-1).Moreover,an enhanced long-term performance at high current densities(212.2 mA h g^(-1)at 4 A g^(-1)over 1000 cycles)with high Coulombic efficiency(~100%)is also achieved.This work demonstrates a novel multifunctional additive for RT Na-S battery cathodes,which is expected to promote the long-waited development towards practical applications of RT Na-S batteries.展开更多
Room temperature sodium–sulfur(Na–S)batteries are severely hampered by dissolution of polysulfides into electrolytes.Herein,a facile approach is used to tune a biomass-derived carbon down to an ultrasmall 0.37 nm mi...Room temperature sodium–sulfur(Na–S)batteries are severely hampered by dissolution of polysulfides into electrolytes.Herein,a facile approach is used to tune a biomass-derived carbon down to an ultrasmall 0.37 nm microporous structure for the first time as a cathode in sodium–sulfur batteries.This produced an intact uniform Na2S membrane to greatly confine the dissolution of polysulfides while realizing a direct solid phase conversion for complete reduction of sulfur to Na2S,which delivers a sulfur loading of 1 mg cm−2(50 wt.%),an excellent rate capacity(933 mAh g^(−1)@0.1 A g^(−1)and 410 mAh g^(−1)@2Ag^(−1)),long cycle performance(0.036%per cycle decay at 1 A g^(−1)after 1500 cycles),and a high energy density for 373 Wh kg^(−1)(0.1 A g^(−1))based on whole electrode weight(active sulfur loading+carbon),ranking the best among all reported plain carbon cathode-based room temperature sodium–sulfur batteries in terms of the cycle life and rate capacity.It is proposed that the solid Na2S produced in the ultrasmall pores(0.37 nm)can be squeezed out to grow an intact membrane on the electrode surface covering the outlet of the pores and greatly depressing the dissolution effect of polysulfides for the long cycle life.This work provides a green chemistry to recycle wastes for sustainable energies and sheds light on design of a unique pore structure to effectively block the dissolution of polysulfides for high-performance sodium–sulfur batteries.展开更多
According to a statistic,approximately 6 trillion cigarettes are smoked each year all over the world,which produces approximately 1.2 million tons of discarded cigarette butts.The discarded cigarette filters are non-b...According to a statistic,approximately 6 trillion cigarettes are smoked each year all over the world,which produces approximately 1.2 million tons of discarded cigarette butts.The discarded cigarette filters are non-biodegradable,thus they produce a mass of waste disposal and cause environmental pollution is-sue.For the purpose of transforming waste into wealth and reducing environmental pollution,nitrogen and sulfur co-doped carbon nanofiber/carbon black(N,S-CNF/CB)composite derived from the discarded cigarette filters is employed to modify glass fiber(GF)separator for the first time in this study.N,S-CNF improves binding ability towards sodium polysulfides(SPSs)by chemisorption.Non-polar CB limits the dissolution of SPSs in the liquid electrolyte by physisorption.The experiment and density functional theory calculation results indicate that a RT-Na/S battery with a N,S-CNF/CB+GF separator exhibits good cycling stability and rate performance.After 100 cycles at a low current rate of 0.1 C,a RT-Na/S battery with a sulfur mass fraction of 71%delivers a discharge capacity of 703 mAh g^(−1).In addition,at a high current rate of 0.5 C,a discharge capacity of 527 mAh g^(−1) is still maintained after 900 cycles with a very low capacity fading rate of 0.035%per cycle.展开更多
基金support from the National Natural Science Foundations of China(No.52002358)high-level talent internationalization training project of Henan province,and scientific and technological activities of Henan province for scholars with overseas study experience(No.002004025).
文摘Room temperature sodium-sulfur(Na-S)batteries,known for their high energy density and low cost,are one of the most promising next-generation energy storage systems.However,the polysulfide shuttling and uncontrollable Na dendrite growth as well as safety issues caused by the use of organic liquid electrolytes in Na-S cells,have severely hindered their commercialization.Solid-state electrolytes instead of liquid electrolytes are considered to be the most direct and effective solution to solve the above problems.However,its practical application is still greatly challenged due to the poor interfacial compatibility between the all-solid-state electrolytes and the anode/cathode,ionic conductivity,and the shuttle effect caused by the presence of liquid phase in the quasi-solid-state electrolytes.This paper presents a comprehensive review of solid-state Na-S batteries from the perspective of regulating interfacial compatibility and improving ionic conductivity as well as suppressing polysulfide shuttle.According to different components,solid-state electrolytes were divided into five categories:solid inorganic electrolytes,solid polymer electrolytes,polymer/inorganic solid hybrid electrolytes,gel polymer electrolytes,and liquid–solid inorganic hybrid electrolytes.Finally,the prospect of developing high performance solid-state electrolytes to improve the cycling stability of room temperature Na-S cells is envisaged.
基金This research was supported by the Australian Research Council(ARC)(DE170100928,DP170101467)an Australian Renewable Energy Agency(ARENA)Project(G00849).The authors acknowledge the use of the facilities at the UOW Electron Microscopy Center(LE0882813 and LE0237478)and Dr.Tania Silver for critical reading of the manuscript.
文摘This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and status are investigated.A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio(72%S).In contrast,a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio(44%S).In carbonate ester electrolyte,only the sulfur trapped in porous structures is active via‘solid-solid’behavior during cycling.The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents.To improve the capacity of the sulfur-rich cathode,ether electrolyte with NaNO_(3) additive is explored to realize a‘solid-liquid’sulfur redox process and confine the shuttle effect of the dissolved polysulfides.As a result,the sulfur-rich cathode achieved high reversible capacity(483 mAh g^(−1)),corresponding to a specific energy of 362 Wh kg^(−1) after 200 cycles,shedding light on the use of ether electrolyte for high-loading sulfur cathode.
基金Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20170036National Natural Science Foundation of China,Grant/Award Numbers:51572129,51772154,51811530100+1 种基金the Materials Characterization Facility of Nanjing University of Science and Technology for XRD,SEM,and TEM experiments.This study was supported by National Natural Science Foundation of China(Nos.51572129,51772154,and 51811530100)Natural Science Foundation of Jiangsu Province(No.BK20170036).
文摘Room temperature sodium-sulfur(RT Na-S)batteries are gaining extensive attention as attractive alternatives for large-scale energy storage,due to low cost and high abundancy of sodium and sulfur in nature.However,the dilemmas regarding soluble polysulfides(Na_(2)Sn,4<n<8)and the inferior reaction kinetics limit their practical application.To address these issues,we report the activated porous carbon fibers(APCF)with small sulfur molecules(S2-4)confined in ultramicropores,to achieve a reversible single-step reaction in RT Na-S batteries.The mechanism is investigated by the in situ UV/vis spectroscopy,which demonstrates Na2S is the only product during the whole discharge process.Moreover,the hierarchical carbon structure can enhance areal sulfur loading without sacrificing the capacity due to thorough contact between electrolyte and sulfur electrode.As a consequence,the APCF electrode with 38 wt%sulfur(APCF-38S)delivers a high initial reversible specific capacity of 1412 mAh g^(-1) and 10.6mAh cm^(-2)(avg.areal sulfur loading:7.5 mg cm^(-2))at 0.1 C(1C=1675 mA g^(-1)),revealing high degree of sulfur utilization.This study provides a new strategy for the development of high areal capacity RT Na-S batteries.
基金financially supported by the Natural Scientific Foundation of China(grant nos.22109001 and 22208335)the Postdoctoral Fellowship Program of CPSF(grant no.GZB20230950)+2 种基金the Heilongjiang Postdoctoral Science Foundation(grant no.LBH-Z23187)the Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices,Soochow University(grant no.KJS2308)startup funds provided to H.Z.from the Harbin Institute of Technology.
文摘Sluggish polysulfide redox kinetics,especially the high energy barrier of rate-determining short-chain polysulfide conversion and the high activation barrier of Na_(2)S decomposition during sulfur recovery,compromise the full potential of rechargeable Na-S electrochemistry.Herein we construct the hierarchical sandwich-structured carbon matrix with atomically dispersed Mn-N4 Lewis acidic sites,taking advantage of their bidirectional electrocatalytic behavior toward interface-mediated reversible sulfur redox.Experimental and theoretical results reveal that the spatial confinement and catalytic effects facilitated via strong Lewis acid-base electron interactions synergistically manipulate the low kinetically direct Na_(2)S_(4) to Na_(2)S conversion,and the formation of Mn-S bond minimizes the energy barrier of Na_(2)S electrochemical activation during battery recharging,thereby rendering a reversible and tunable polysulfide speciation pathway.Furthermore,the degradation of the Na-S cell is due to the depletion of metal anode rather than the loss of active sulfur species and/or aggregation of inactive dead sulfur.As expected,the S@Mn/NC cathode delivers outstanding rate capability and ultrahigh cycling stability.Simultaneously,a proof-of-concept pouch cell was also demonstrated capable of delivering an energy density up to 840 Wh kgcathode−1.The tunable sulfur redox electrochemistry invoked by the bidirectional monodispersed Mn catalytic hot spots facilitates the efficient polysulfide speciation for practical Na-S cells.
基金This work is financially supported by Grants from the National Natural Science Foundation of China(No.21773188,21972111,U1530401)Natural Science Foundation of Chongqing(cstc2018jcyjAX0714).
文摘Rechargeable room temperature sodium–sulfur(RT Na–S)batteries are seriously limited by low sulfur utilization and sluggish electrochemical reaction activity of polysulfide intermediates.Herein,a 3D“branch-leaf”biomimetic design proposed for high performance Na–S batteries,where the leaves constructed from Co nanoparticles on carbon nanofibers(CNF)are fully to expose the active sites of Co.The CNF network acts as conductive“branches”to ensure adequate electron and electrolyte supply for the Co leaves.As an effective electrocatalytic battery system,the 3D“branch-leaf”conductive network with abundant active sites and voids can effectively trap polysulfides and provide plentiful electron/ions pathways for electrochemical reaction.DFT calculation reveals that the Co nanoparticles can induce the formation of a unique Co–S–Na molecular layer on the Co surface,which can enable a fast reduction reaction of the polysulfides.Therefore,the prepared“branch-leaf”CNF-L@Co/S electrode exhibits a high initial specific capacity of 1201 mAh g^−1 at 0.1 C and superior rate performance.
文摘Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.
基金financial support from the Australian Research Council(ARC)through the ARC Discovery projects(DP200101249,DP210101389)the ARC Research Hub for Integrated Energy Storage Solutions(IH180100020).
文摘Rechargeable room-temperature sodium–sulfur(Na–S)and sodium–selenium(Na–Se)batteries are gaining extensive attention for potential large-scale energy storage applications owing to their low cost and high theoretical energy density.Optimization of electrode materials and investigation of mechanisms are essential to achieve high energy density and long-term cycling stability of Na–S(Se)batteries.Herein,we provide a comprehensive review of the recent progress in Na–S(Se)batteries.We elucidate the Na storage mechanisms and improvement strategies for battery performance.In particular,we discuss the advances in the development of battery components,including high-performance sulfur cathodes,optimized electrolytes,advanced Na metal anodes and modified separators.Combined with current research achievements,this review outlines remaining challenges and clear research directions for the future development of practical high-performance Na–S(Se)batteries.
基金support from University of Waterloo,Waterloo Institute for Nanotechnology,and Natural Sciences and Engineering Research Council of Canada(NSERC).This work was also supported by the Outstanding Youth Project of Guangdong Natural Science Foundation(2021B1515020051)Department of Science and Technology of Guangdong Province(2019JC01L203 and 2020B0909030004)+1 种基金the Natural Science Foundation of Ningxia(2023AAC01003)the Foundation of State Key Laboratory of High Efficiency Utilization of Coal and Green Chemical Engineering(2022-K79).
文摘Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metalsulfur batteries.Motivated by a theoretical prediction,herein,we strategically propose nitrogenvacancy tantalum nitride(Ta3N5-x)impregnated inside the interconnected nanopores of nitrogendecorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in roomtemperature sodium-sulfur batteries.Through a pore-constriction mechanism,the nitrogen vacancies are controllably constructed during the nucleation of Ta3N5-x.The defect manipulation on the local environment enables well-regulated Ta 5d-orbital energy level,not only modulating band structure toward enhanced intrinsic conductivity of Ta-based materials,but also promoting polysulfide stabilization and achieving bifunctional catalytic capability toward completely reversible polysulfide conversion.Moreover,the interconnected continuous Ta3N5-x-in-pore structure facilitates electron and sodium-ion transport and accommodates volume expansion of sulfur species while suppressing their shuttle behavior.Due to these attributes,the as-developed Ta3N5-x-based electrode achieves superior rate capability of 730 mAh g-1 at 3.35 A g-1,long-term cycling stability over 2000 cycles,and high areal capacity over 6 mAh cm-2 under high sulfur loading of 6.2 mg cm-2.This work not only presents a new sulfur electrocatalyst candidate for metal-sulfur batteries,but also sheds light on the controllable material design of defect structure in hopes of inspiring new ideas and directions for future research.
基金supported by the National Natural Science Foundation of China(52172219 and 51872192)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(19KJA170001)+1 种基金the Fundamental Research Program of Shanxi Province(202103021223019)Science and Technology Major Project of Shanxi(No.202101030201022)
文摘Sodium-sulfur(Na–S)batteries that utilize earth-abundant materials of Na and S have been one of the hottest topics in battery research.The low cost and high energy density make them promising candidates for next-generation storage technologies as required in the grid and renewable energy.In recent years,extensive efforts have been devoted to the diversity and functionalities of Na–S batteries,aiming to extend their potential applications across multiple temporal and spatial dimensions.Here,we summarize the unconventional designs for the functionalities of Na–S batteries such as flexible batteries,solid-state cells,flame resistance,and operation at extreme temperatures.By highlighting these design strategies that help to realize the functionalities,we hope this review offers a pathway to foster the bright future of Na–S batteries in diverse applications.
基金support from the Liao Ning Revitalization Talents Program(No.XLYC1907144)Dalian Youth Science and Technology Star Project Support Program(No.2017RQ104).
文摘In 2011,a new class of 2D materials was discovered;after 2012,they began to be concerned;in 2017,the“gold rush”of the materials was triggered,and they are exactly MXenes.2D MXenes,a new class of transition metal carbides,carbonitrides and nitrides,have become the star and cutting-edge research materials in the field of emerging batteries systems due to their unique 2D structure,abundant surface chemistry,and excellent physical and electrochemical properties.This review focuses on the MXene materials and summarizes the recent advancements in the synthesis techniques and properties,in addition to a detailed discussion on the electrochemical energy storage applications,including alkali-ion(Li^(+),Na^(+),K^(+))storage,lithium-sulfur(Li–S)batteries,sodiumsulfur(Na–S)batteries,and metal anode protection.Special attentions are given to the elaborate design of nano-micro structures of MXenes for the various roles as electrodes,multifunctional components,S hosts,modified separators,and metal anode protective layers.The paper ends with a prospective summary of the promising research directions in terms of synthesis,structure,properties,analysis,and production on MXene materials.
基金the support of the National Natural Science Foundation of China(51971146,51971147,52171218 and 52271222)the Shanghai Municipal Science and Technology Commission(21010503100 and 20ZR1438400)+3 种基金the Innovation Program of Shanghai Municipal EducationCommission(No.2019-01-07-00-07-E00015)the Shanghai Rising-Star Program(20QA1407100 and Yangfan Special Project:23YF1428900)the support of the Advanced Research and Technology Innovation Centre(ARTIC,Project Number ADT-RP2/A0005947-32-00)for research conducted by John Wang’s group。
文摘Promising room-temperature sodium-sulfur(RT Na-S)battery systems rely on purposely designed highperforming and low-cost electrode materials.Nevertheless,there are the challenges of irreversible dissolution and slow redox kinetics of NaPSs in the complete discharge of sulfur capacity.Herein,engineered CoMoO_(4)in reduced graphene oxide(CoMoO_(4)@rGO)is reported as a class of superior cathode hosts for RT Na-S batteries.The CoMoO_(4)@rGO matrix is designed to facilitate the reversible sodiation and desodiation of sulfur,considering the strong chemisorption between sulfur(and short-chain sodium sulfides)and CoMoO_(4),which alleviates the shuttle effect of sodium sulfides and accelerates the electrochemical reaction rate at RT.The obtained S/CoMoO_(4)@rGO cathode with~52%S loading exhibits a high capacity of520.1 mA h g^(-1)after 100 cycles at 0.1 A g^(-1).Moreover,an enhanced long-term performance at high current densities(212.2 mA h g^(-1)at 4 A g^(-1)over 1000 cycles)with high Coulombic efficiency(~100%)is also achieved.This work demonstrates a novel multifunctional additive for RT Na-S battery cathodes,which is expected to promote the long-waited development towards practical applications of RT Na-S batteries.
基金financial support from Chongqing Postdoctoral Natural Science Foundation No.cstc2020jcyj-bsh0048State Key Laboratory of Silkworm Genome Biology,Suzhou Foreign Academician Workstation(SWY2021002)Collaborative Innovation Center of Water Treatment Technology and Material,and Innovation Platform for Academicians of Hainan Province
文摘Room temperature sodium–sulfur(Na–S)batteries are severely hampered by dissolution of polysulfides into electrolytes.Herein,a facile approach is used to tune a biomass-derived carbon down to an ultrasmall 0.37 nm microporous structure for the first time as a cathode in sodium–sulfur batteries.This produced an intact uniform Na2S membrane to greatly confine the dissolution of polysulfides while realizing a direct solid phase conversion for complete reduction of sulfur to Na2S,which delivers a sulfur loading of 1 mg cm−2(50 wt.%),an excellent rate capacity(933 mAh g^(−1)@0.1 A g^(−1)and 410 mAh g^(−1)@2Ag^(−1)),long cycle performance(0.036%per cycle decay at 1 A g^(−1)after 1500 cycles),and a high energy density for 373 Wh kg^(−1)(0.1 A g^(−1))based on whole electrode weight(active sulfur loading+carbon),ranking the best among all reported plain carbon cathode-based room temperature sodium–sulfur batteries in terms of the cycle life and rate capacity.It is proposed that the solid Na2S produced in the ultrasmall pores(0.37 nm)can be squeezed out to grow an intact membrane on the electrode surface covering the outlet of the pores and greatly depressing the dissolution effect of polysulfides for the long cycle life.This work provides a green chemistry to recycle wastes for sustainable energies and sheds light on design of a unique pore structure to effectively block the dissolution of polysulfides for high-performance sodium–sulfur batteries.
基金supported by the National Natural Science Foundation of China(Nos.51631004 and 52130101)the Basic Construction Fund in Jilin Province Budget for 2019(No.2019C042-8).
文摘According to a statistic,approximately 6 trillion cigarettes are smoked each year all over the world,which produces approximately 1.2 million tons of discarded cigarette butts.The discarded cigarette filters are non-biodegradable,thus they produce a mass of waste disposal and cause environmental pollution is-sue.For the purpose of transforming waste into wealth and reducing environmental pollution,nitrogen and sulfur co-doped carbon nanofiber/carbon black(N,S-CNF/CB)composite derived from the discarded cigarette filters is employed to modify glass fiber(GF)separator for the first time in this study.N,S-CNF improves binding ability towards sodium polysulfides(SPSs)by chemisorption.Non-polar CB limits the dissolution of SPSs in the liquid electrolyte by physisorption.The experiment and density functional theory calculation results indicate that a RT-Na/S battery with a N,S-CNF/CB+GF separator exhibits good cycling stability and rate performance.After 100 cycles at a low current rate of 0.1 C,a RT-Na/S battery with a sulfur mass fraction of 71%delivers a discharge capacity of 703 mAh g^(−1).In addition,at a high current rate of 0.5 C,a discharge capacity of 527 mAh g^(−1) is still maintained after 900 cycles with a very low capacity fading rate of 0.035%per cycle.