Fast interfacial kinetics derived from bicontinuous three-dimensional(3D)architecture is a strategic feature for achieving fast-charging lithium-ion batteries(LIBs).One of the main reasons is its large active surface ...Fast interfacial kinetics derived from bicontinuous three-dimensional(3D)architecture is a strategic feature for achieving fast-charging lithium-ion batteries(LIBs).One of the main reasons is its large active surface and short diffusion path.Yet,understanding of unusual electrochemical properties still remain great challenge due to its complexity.In this study,we proposed a nickel–tin compound(Ni_(3)Sn_(4))supported by 3D Nickel scaffolds as main frame because the Ni_(3)Sn_(4) clearly offers a higher reversible capacity and stable cycling performance than bare tin(Sn).In order to verify the role of Ni,atomic-scale simulation based on density functional theory systematically addressed to the reaction mechanism and structural evolution of Ni_(3)Sn_(4) during the lithiation process.Our findings are that Ni enables Ni_(3)Sn_(4) to possess higher mechanical stability in terms of reactive flow stress,subsequently lead to improve Li storage capability.This study elucidates an understanding of the lithiation mechanism of Ni_(3)Sn_(4) and provides a new perspective for the design of high-capacity and high-power 3D anodes for fast-charging LIBs.展开更多
High electrochemical stability and safety make Na+superionic conductor(NASICON)-class cathodes highly desirable for Na-ion batteries(SIBs).However,their practical capacity is limited,leading to low specific energy.Fur...High electrochemical stability and safety make Na+superionic conductor(NASICON)-class cathodes highly desirable for Na-ion batteries(SIBs).However,their practical capacity is limited,leading to low specific energy.Furthermore,the low electrical conductivity combined with a decline in capacity upon prolonged cycling(>1000 cycles)related to the loss of active material-carbon conducting contact regions contributes to moderate rate performance and cycling stability.The need for high specific energy cathodes that meet practical electrochemical requirements has prompted a search for new materials.Herein,we introduce a new carbon-coated Na_(3)VFe_(0.5)Ti_(0.5)(PO_(4))_(3)(NVFTP/C)material as a promising candidate in the NASICON family of cathodes for SIBs.With a high specific energy of∼457 Wh kg^(-1) and a high Na+insertion voltage of 3.0 V versus Na^(+)/Na,this cathode can undergo a reversible single-phase solid-solution and two-phase(de)sodiation evolution at 28 C(1 C=174.7 mAh g^(-1))for up to 10,000 cycles.This study highlights the potential of utilizing low-cost and highly efficient cathodes made from Earth-abundant and harmless materials(Fe and Ti)with enriched Na^(+)-storage properties in practical SIBs.展开更多
Aqueous zinc-ion batteries(ZIBs)are receiving a continuously increasing attention for mobile devices,especially for the flexible and wearable electronics,due to their non-toxicity,non-flammability,and low-cost feature...Aqueous zinc-ion batteries(ZIBs)are receiving a continuously increasing attention for mobile devices,especially for the flexible and wearable electronics,due to their non-toxicity,non-flammability,and low-cost features.Despite the significant progress in achieving higher capacities for electrode materials of ZIBs,to endow them with high flexibility and economic feasibility is,however,still a significant challenge remaining unsolved.Herein,we present a highly flexible composite film composed of carbon nanotube film and V_(2)O_(5)(CNTF@V_(2)O_(5))with high strength and high conductivity,which is prepared by simply impregnating a porous CNT film with an aqueous V_(2)O_(5)sol under vacuum.For this material,intimate incorporation between V_(2)O_(5)and CNTs has been achieved,successfully integrating the high zinc ion storage capability with high mechanical flexibility.As a result,this CNTF@V_(2)O_(5)film delivers a high capacity of 356.6 m Ah g^(-1)at 0.4 A g^(-1)and excellent cycling stability with 80.1%capacity retention after 500 cycles at 2.0 A g^(-1).The novel strategy and the outstanding battery performance presented in this work should shed light on the development of high-performance and flexible ZIBs.展开更多
Realizing a lithium sulfide(Li_(2)S)cathode with both high energy density and a long lifespan requires an innovative cathode design that maximizes electrochemical performance and resists electrode deterioration.Herein...Realizing a lithium sulfide(Li_(2)S)cathode with both high energy density and a long lifespan requires an innovative cathode design that maximizes electrochemical performance and resists electrode deterioration.Herein,a high-loading Li_(2)S-based cathode with micrometric Li_(2)S particles composed of two-dimensional graphene(Gr)and one-dimensional carbon nanotubes(CNTs)in a compact geometry is developed,and the role of CNTs in stable cycling of high-capacity Li–S batteries is emphasized.In a dimensionally combined carbon matrix,CNTs embedded within the Gr sheets create robust and sustainable electron diffusion pathways while suppressing the passivation of the active carbon surface.As a unique point,during the first charging process,the proposed cathode is fully activated through the direct conversion of Li_(2)S into S_(8) without inducing lithium polysulfide formation.The direct conversion of Li_(2)S into S_(8) in the composite cathode is ubiquitously investigated using the combined study of in situ Raman spectroscopy,in situ optical microscopy,and cryogenic transmission electron microscopy.The composite cathode demonstrates unprecedented electrochemical properties even with a high Li_(2)S loading of 10 mg cm^(–2);in particular,the practical and safe Li–S full cell coupled with a graphite anode shows ultra-long-term cycling stability over 800 cycles.展开更多
Fiber materials are promising for electrocatalysis applications due to their structural features including high surface area,controllable chemical compositions,and abundant composite forms.In the past decade,considera...Fiber materials are promising for electrocatalysis applications due to their structural features including high surface area,controllable chemical compositions,and abundant composite forms.In the past decade,considerable research efforts have been devoted to construct advanced fiber materials possessing conductive network(to facilitate efficient electron transport)and large specific surface area(to support massive catalytically active sites)to boost electrocatalysis performance.Herein,we focused on recent advances in fiber-based electrocatalyst with enhanced electrocatalytic activity.Moreover,the synthesis,structure,and properties of fiber materials and their applications in hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction are discussed.Finally,the research challenges and future prospects of fiber materials in electrocatalysis applications are proposed.展开更多
Black phosphorus(BP)is a rapidly up and coming star in two-dimensional(2D)materials.The unique characteristic of BP is its in-plane anisotropy.This characteristic of BP ignites a new type of 2D materials that have low...Black phosphorus(BP)is a rapidly up and coming star in two-dimensional(2D)materials.The unique characteristic of BP is its in-plane anisotropy.This characteristic of BP ignites a new type of 2D materials that have low-symmetry structures and in-plane anisotropic properties.On this basis,they offer richer and more unique low-dimensional physics compared to isotropic 2D materials,thus providing a fertile ground for novel applications including electronics,optoelectronics,molecular detection,thermoelectric,piezoelectric,and ferroelectric with respect to in-plane anisotropy.This article reviews the recent advance in characterization and applications of in-plane anisotropic 2D materials.展开更多
High-entropy alloys(HEAs)have been widely studied due to their unconventional compositions and unique physicochemical properties for various applications.Herein,for the first time,we propose a surface strain strategy ...High-entropy alloys(HEAs)have been widely studied due to their unconventional compositions and unique physicochemical properties for various applications.Herein,for the first time,we propose a surface strain strategy to tune the electrocatalytic activity of HEAs for methanol oxidation reaction(MOR).High-resolution aberration-corrected scanning transmission electron microscopy(STEM)and elemental mapping demonstrate both uniform atomic dispersion and the formation of a face-centered cubic(FCC)crystalline structure in Pt Fe Co Ni Cu HEAs.The HEAs obtained by heat treatment at 700℃(HEA-700)exhibit 0.94%compressive strain compared with that obtained at 400℃(HEA-400).As expected,the specific activity and mass activity of HEA-700 is higher than that of HEA-400 and most of the state-of-the-art catalysts.The enhanced MOR activity can be attributed to a shorter Pt–Pt bond distance in HEA-700 resulting from compressive strain.The nonprecious metal atoms in the core could generate compressive strain and down shift d-band centers via electron transfer to surface Pt layer.This work presents a new perspective for the design of high-performance HEAs electrocatalysts.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2021M3H4A1A02045967)(NRF-2021M3H4A1A02048137)supported by the Chung-Ang University Research Scholarship Grants in 2021。
文摘Fast interfacial kinetics derived from bicontinuous three-dimensional(3D)architecture is a strategic feature for achieving fast-charging lithium-ion batteries(LIBs).One of the main reasons is its large active surface and short diffusion path.Yet,understanding of unusual electrochemical properties still remain great challenge due to its complexity.In this study,we proposed a nickel–tin compound(Ni_(3)Sn_(4))supported by 3D Nickel scaffolds as main frame because the Ni_(3)Sn_(4) clearly offers a higher reversible capacity and stable cycling performance than bare tin(Sn).In order to verify the role of Ni,atomic-scale simulation based on density functional theory systematically addressed to the reaction mechanism and structural evolution of Ni_(3)Sn_(4) during the lithiation process.Our findings are that Ni enables Ni_(3)Sn_(4) to possess higher mechanical stability in terms of reactive flow stress,subsequently lead to improve Li storage capability.This study elucidates an understanding of the lithiation mechanism of Ni_(3)Sn_(4) and provides a new perspective for the design of high-capacity and high-power 3D anodes for fast-charging LIBs.
基金This work was supported by the National Research Foundation of Korea(NRF)Grant funded by the Korean government(MSIT)(NRF-2018R1A5A1025224 and NRF-2021R1A4A1052051)This work was also supported by the National Research Foundation of Korea Grant funded by the Korean Government Ministry of Education and Science Technology(NRF-2021R1I1A3060193).
文摘High electrochemical stability and safety make Na+superionic conductor(NASICON)-class cathodes highly desirable for Na-ion batteries(SIBs).However,their practical capacity is limited,leading to low specific energy.Furthermore,the low electrical conductivity combined with a decline in capacity upon prolonged cycling(>1000 cycles)related to the loss of active material-carbon conducting contact regions contributes to moderate rate performance and cycling stability.The need for high specific energy cathodes that meet practical electrochemical requirements has prompted a search for new materials.Herein,we introduce a new carbon-coated Na_(3)VFe_(0.5)Ti_(0.5)(PO_(4))_(3)(NVFTP/C)material as a promising candidate in the NASICON family of cathodes for SIBs.With a high specific energy of∼457 Wh kg^(-1) and a high Na+insertion voltage of 3.0 V versus Na^(+)/Na,this cathode can undergo a reversible single-phase solid-solution and two-phase(de)sodiation evolution at 28 C(1 C=174.7 mAh g^(-1))for up to 10,000 cycles.This study highlights the potential of utilizing low-cost and highly efficient cathodes made from Earth-abundant and harmless materials(Fe and Ti)with enriched Na^(+)-storage properties in practical SIBs.
基金supported by the National Natural Science Foundation of China(No.51072130,51502045 and 21905202)the Australian Research Council(ARC)through Discovery Project(No.DP200100365)the Discovery Early Career Researcher Award(DECRA,No.DE170100871)program。
文摘Aqueous zinc-ion batteries(ZIBs)are receiving a continuously increasing attention for mobile devices,especially for the flexible and wearable electronics,due to their non-toxicity,non-flammability,and low-cost features.Despite the significant progress in achieving higher capacities for electrode materials of ZIBs,to endow them with high flexibility and economic feasibility is,however,still a significant challenge remaining unsolved.Herein,we present a highly flexible composite film composed of carbon nanotube film and V_(2)O_(5)(CNTF@V_(2)O_(5))with high strength and high conductivity,which is prepared by simply impregnating a porous CNT film with an aqueous V_(2)O_(5)sol under vacuum.For this material,intimate incorporation between V_(2)O_(5)and CNTs has been achieved,successfully integrating the high zinc ion storage capability with high mechanical flexibility.As a result,this CNTF@V_(2)O_(5)film delivers a high capacity of 356.6 m Ah g^(-1)at 0.4 A g^(-1)and excellent cycling stability with 80.1%capacity retention after 500 cycles at 2.0 A g^(-1).The novel strategy and the outstanding battery performance presented in this work should shed light on the development of high-performance and flexible ZIBs.
基金Korea Institute of Energy Technology Evaluation and Planning,Grant/Award Number:20214000000320Samsung Research Funding&Incubation Center of Samsung Electronics,Grant/Award Number:SRFC-MA1901-06。
文摘Realizing a lithium sulfide(Li_(2)S)cathode with both high energy density and a long lifespan requires an innovative cathode design that maximizes electrochemical performance and resists electrode deterioration.Herein,a high-loading Li_(2)S-based cathode with micrometric Li_(2)S particles composed of two-dimensional graphene(Gr)and one-dimensional carbon nanotubes(CNTs)in a compact geometry is developed,and the role of CNTs in stable cycling of high-capacity Li–S batteries is emphasized.In a dimensionally combined carbon matrix,CNTs embedded within the Gr sheets create robust and sustainable electron diffusion pathways while suppressing the passivation of the active carbon surface.As a unique point,during the first charging process,the proposed cathode is fully activated through the direct conversion of Li_(2)S into S_(8) without inducing lithium polysulfide formation.The direct conversion of Li_(2)S into S_(8) in the composite cathode is ubiquitously investigated using the combined study of in situ Raman spectroscopy,in situ optical microscopy,and cryogenic transmission electron microscopy.The composite cathode demonstrates unprecedented electrochemical properties even with a high Li_(2)S loading of 10 mg cm^(–2);in particular,the practical and safe Li–S full cell coupled with a graphite anode shows ultra-long-term cycling stability over 800 cycles.
基金The funding has been received from Fundamental Research Funds for the Central Universities with Grant no.2232021A-02Shanghai Committee of Science and Technology,China with Grant No.21ZR1480000National Natural Science Foundation of China with Grant Nos.52122312,52172291.
文摘Fiber materials are promising for electrocatalysis applications due to their structural features including high surface area,controllable chemical compositions,and abundant composite forms.In the past decade,considerable research efforts have been devoted to construct advanced fiber materials possessing conductive network(to facilitate efficient electron transport)and large specific surface area(to support massive catalytically active sites)to boost electrocatalysis performance.Herein,we focused on recent advances in fiber-based electrocatalyst with enhanced electrocatalytic activity.Moreover,the synthesis,structure,and properties of fiber materials and their applications in hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction are discussed.Finally,the research challenges and future prospects of fiber materials in electrocatalysis applications are proposed.
基金This work was supported by the National Natural Science Foundation of China(Grant No.21825103 and 51727809)the National Basic Research Foundation of China(Grant No.2015CB932600)the Project Funded by China Postdoctoral Science Foundation(Grant No.2017M610474,2016M600589,and 2017T100552).
文摘Black phosphorus(BP)is a rapidly up and coming star in two-dimensional(2D)materials.The unique characteristic of BP is its in-plane anisotropy.This characteristic of BP ignites a new type of 2D materials that have low-symmetry structures and in-plane anisotropic properties.On this basis,they offer richer and more unique low-dimensional physics compared to isotropic 2D materials,thus providing a fertile ground for novel applications including electronics,optoelectronics,molecular detection,thermoelectric,piezoelectric,and ferroelectric with respect to in-plane anisotropy.This article reviews the recent advance in characterization and applications of in-plane anisotropic 2D materials.
基金supported by the National Natural Science Foundation of China (51402100, 21573066, 21825201, 22002039, and 21522305)the Scientific Research Foundation of Hunan Provincial Education Department (19C0054)+2 种基金the Postgraduate Scientific Research Innovation Project of Hunan Province (CX20200441)the Australian Research Council (CE 140100012)the Australian National Fabrication Facility | UOW Electron Microscopy Centre, and Compute Canada, Natural Sciences and Engineering Research Council of Canada (NSERC), University of Toronto
文摘High-entropy alloys(HEAs)have been widely studied due to their unconventional compositions and unique physicochemical properties for various applications.Herein,for the first time,we propose a surface strain strategy to tune the electrocatalytic activity of HEAs for methanol oxidation reaction(MOR).High-resolution aberration-corrected scanning transmission electron microscopy(STEM)and elemental mapping demonstrate both uniform atomic dispersion and the formation of a face-centered cubic(FCC)crystalline structure in Pt Fe Co Ni Cu HEAs.The HEAs obtained by heat treatment at 700℃(HEA-700)exhibit 0.94%compressive strain compared with that obtained at 400℃(HEA-400).As expected,the specific activity and mass activity of HEA-700 is higher than that of HEA-400 and most of the state-of-the-art catalysts.The enhanced MOR activity can be attributed to a shorter Pt–Pt bond distance in HEA-700 resulting from compressive strain.The nonprecious metal atoms in the core could generate compressive strain and down shift d-band centers via electron transfer to surface Pt layer.This work presents a new perspective for the design of high-performance HEAs electrocatalysts.