Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance betw...Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.展开更多
Attracted by high energy density and considerable conductivity of selenium(Se),Na-Se batteries have been deemed promising energy-storage systems.But,it still suffers from sluggish kinetic behaviors and similar“shuttl...Attracted by high energy density and considerable conductivity of selenium(Se),Na-Se batteries have been deemed promising energy-storage systems.But,it still suffers from sluggish kinetic behaviors and similar“shuttling effect”to S-electrodes.Herein,utilizing uniform hollow carbon spheres as precursors,Se-material is effectively loaded through vapor-infiltration method.Owing to the distribution of optimized pores,the content of microspores could be up to~60%(<2 nm),serving important roles for the physical confinement effect.Meanwhile,the rich oxygen-containing groups and N-elements could be noted,inducing the evolution of electron-moving behaviors.More significantly,assisted by the interfacial C-Se bonds and tiny Se distributions,Se electrodes are activated during cycling.Used as cathodes for Na-Se systems,the as-resulted samples display a capacity of 593.9 mA h g^(-1)after 100 cycles at the current density of 0.1 C.Even after 6000 cycles,the capacity could be still kept at about 225 mA h g^(-1)at 5.0 C.Supported by the detailed kinetic analysis,the designed microspores size induces the increasing redox reaction of nano Se,whilst the surface traits further render the enhancement of pseudo-capacitive contributions.Moreover,after cycling,the product Sex(x<4)in pores serves as the primary active material.Given this,the work is anticipated to provide an effective strategy for advanced electrodes for Na-Se systems.展开更多
Nanostructured metal phosphides are very attractive materials in energy storage and conversion,but their applications are severely limited by complicated preparation steps,harsh conditions and large excess of highly t...Nanostructured metal phosphides are very attractive materials in energy storage and conversion,but their applications are severely limited by complicated preparation steps,harsh conditions and large excess of highly toxic phosphorus source.Here we develop a highly efficient one-step method to synthesize Sn_(4)P_(3)nanostructure based on simultaneous reduction of SnCl_(4)and PCl_(3)on mechanically activated Na surface and in situ phosphorization.The low-toxic PCl3 displays a very high phosphorizing efficiency(100%).Furthermore,this simple method is powerful to control phosphide size.Ultrafine Sn_(4)P_(3)nanocrystals(<5 nm)supported on carbon sheets(Sn_(4)P_(3)/C)are obtained,which is due to the unique bottom-up surface-limited reaction.As the anode material for sodium/lithium ion batteries(SIBs/LIBs),the Sn_(4)P_(3)/C shows profound sodiation/lithiation extents,good phase-conversion reversibility,excellent rate performance and long cycling stability,retaining high capacities of 420 mAh/g for SIBs and 760 mAh/g for LIBs even after 400 cycles at 1.0 A/g.Combining simple and efficient preparation,low-toxic and high-efficiency phosphorus source and good control of nanosize,this method is very promising for low-cost and scalable preparation of high-performance Sn_(4)P_(3)anode.展开更多
Nanostructured aluminum recently delivers a variety of new applications of the earth-abundant Al resource due to the unique properties,but its controllable synthesis remains very challenging with harsh conditions and ...Nanostructured aluminum recently delivers a variety of new applications of the earth-abundant Al resource due to the unique properties,but its controllable synthesis remains very challenging with harsh conditions and spontaneously flammable precursors.Herein,a surface group directed method is developed to efficiently achieve low-temperature synthesis and selfassembly of zero-dimensional(0D)Al nanocrystals over one-dimensional(1D)carbon fibers(Al@CFs)through non-flammable AlCl3 reduction at 70°C.Theoretical calculations unveil surface‒OLi groups of carbon fibers exert efficient binding effect to AlCl3,which guides intimate adsorption and in-situ self-assembly of the generated Al nanocrystals.The distinctive 0D-over-1D Al@CFs provides long 1D conductive networks for electron transfer,ultrafine 0D Al nanocrystals for fast lithiation and excellent buffering effect for volume change,thus exhibiting high structure stability and superior lithium storage performance.This work paves the way for mild and controllable synthesis of Al-based nanomaterials for new high-value applications.展开更多
基金supported by the National Natural Science Foundation of Tianjin(No.20JCQNJC01280)the National Natural Science Foundation of China(No.21905201)+1 种基金the support of the scientifi c research project from China Three Gorges Corporation(No.202103406)supported by Tohoku University and JSPS KAKENHI(No.JP16J06828).
文摘Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.
基金financially supported by the National Natural Science Foundation of China(No.21973028,52004334)the outstanding youth science fund of Henan Normal University(No.2021JQ02),Natural Science Foundation of Hunan Province(2021JJ20073)+2 种基金National Key Research and Development Program of China(2018YFC1901601 and 2019YFC1907801)Scientific Research Fund of Hunan Provincial Education Department,grant number(20C0085)Collaborative Innovation Center for Clean and Efficient Utilization of Strategic Metal Mineral Resources,Foundation of State Key Laboratory of Mineral Processing(BGRIMM-KJSKL-2017-13)。
文摘Attracted by high energy density and considerable conductivity of selenium(Se),Na-Se batteries have been deemed promising energy-storage systems.But,it still suffers from sluggish kinetic behaviors and similar“shuttling effect”to S-electrodes.Herein,utilizing uniform hollow carbon spheres as precursors,Se-material is effectively loaded through vapor-infiltration method.Owing to the distribution of optimized pores,the content of microspores could be up to~60%(<2 nm),serving important roles for the physical confinement effect.Meanwhile,the rich oxygen-containing groups and N-elements could be noted,inducing the evolution of electron-moving behaviors.More significantly,assisted by the interfacial C-Se bonds and tiny Se distributions,Se electrodes are activated during cycling.Used as cathodes for Na-Se systems,the as-resulted samples display a capacity of 593.9 mA h g^(-1)after 100 cycles at the current density of 0.1 C.Even after 6000 cycles,the capacity could be still kept at about 225 mA h g^(-1)at 5.0 C.Supported by the detailed kinetic analysis,the designed microspores size induces the increasing redox reaction of nano Se,whilst the surface traits further render the enhancement of pseudo-capacitive contributions.Moreover,after cycling,the product Sex(x<4)in pores serves as the primary active material.Given this,the work is anticipated to provide an effective strategy for advanced electrodes for Na-Se systems.
基金support from the National Natural Science Foundation of China(Nos.51972075 and 51772059)the Natural Science Foundation of Heilongjiang Province(No.ZD2019E004)the Fundamental Research funds for the Central Universities.
文摘Nanostructured metal phosphides are very attractive materials in energy storage and conversion,but their applications are severely limited by complicated preparation steps,harsh conditions and large excess of highly toxic phosphorus source.Here we develop a highly efficient one-step method to synthesize Sn_(4)P_(3)nanostructure based on simultaneous reduction of SnCl_(4)and PCl_(3)on mechanically activated Na surface and in situ phosphorization.The low-toxic PCl3 displays a very high phosphorizing efficiency(100%).Furthermore,this simple method is powerful to control phosphide size.Ultrafine Sn_(4)P_(3)nanocrystals(<5 nm)supported on carbon sheets(Sn_(4)P_(3)/C)are obtained,which is due to the unique bottom-up surface-limited reaction.As the anode material for sodium/lithium ion batteries(SIBs/LIBs),the Sn_(4)P_(3)/C shows profound sodiation/lithiation extents,good phase-conversion reversibility,excellent rate performance and long cycling stability,retaining high capacities of 420 mAh/g for SIBs and 760 mAh/g for LIBs even after 400 cycles at 1.0 A/g.Combining simple and efficient preparation,low-toxic and high-efficiency phosphorus source and good control of nanosize,this method is very promising for low-cost and scalable preparation of high-performance Sn_(4)P_(3)anode.
基金The authors acknowledge the financial support from the National Natural Science Foundation of China(Nos.22101065 and 51972075)the Natural Science Foundation of Heilongjiang Province(No.YQ2021B001)+1 种基金the China Postdoctoral Science Foundation(No.2020M681075)the Fundamental Research Funds for the Central Universities.
文摘Nanostructured aluminum recently delivers a variety of new applications of the earth-abundant Al resource due to the unique properties,but its controllable synthesis remains very challenging with harsh conditions and spontaneously flammable precursors.Herein,a surface group directed method is developed to efficiently achieve low-temperature synthesis and selfassembly of zero-dimensional(0D)Al nanocrystals over one-dimensional(1D)carbon fibers(Al@CFs)through non-flammable AlCl3 reduction at 70°C.Theoretical calculations unveil surface‒OLi groups of carbon fibers exert efficient binding effect to AlCl3,which guides intimate adsorption and in-situ self-assembly of the generated Al nanocrystals.The distinctive 0D-over-1D Al@CFs provides long 1D conductive networks for electron transfer,ultrafine 0D Al nanocrystals for fast lithiation and excellent buffering effect for volume change,thus exhibiting high structure stability and superior lithium storage performance.This work paves the way for mild and controllable synthesis of Al-based nanomaterials for new high-value applications.
