Sodium-ion storage devices are highly desirable for large-scale energy storage applications owing to the wide availability of sodium resources and low cost.Transition metal nitrides(TMNs)are promising anode materials ...Sodium-ion storage devices are highly desirable for large-scale energy storage applications owing to the wide availability of sodium resources and low cost.Transition metal nitrides(TMNs)are promising anode materials for sodium-ion storage,while their detailed reaction mechanism remains unexplored.Herein,we synthesize the mesoporous Mo3N2 nanowires(Meso-Mo_(3)N_(2)-NWs).The sodium-ion storage mechanism of Mo3N2 is systematically investigated through in-situ XRD,ex-situ experimental characterizations and detailed kinetics analysis.Briefly,the Mo_(3)N_(2) undergoes a surface pseudocapacitive redox charge storage process.Benefiting from the rapid surface redox reaction,the Meso-Mo_(3)N_(2)-NWs anode delivers high specific capacity(282 m Ah g^(-1) at 0.1 A g^(-1)),excellent rate capability(87 m Ah g^(-1) at 16 A g^(-1))and long cycling stability(a capacity retention of 78.6%after 800 cycles at 1 A g^(-1)).The present work highlights that the surface pseudocapacitive sodium-ion storage mechanism enables to overcome the sluggish sodium-ion diffusion process,which opens a new direction to design and synthesize high-rate sodiumion storage materials.展开更多
The urea oxidization reaction(UOR)is an important anodic reaction in electro-catalytic energy conversion.However,the sluggish reaction kinetics and complex catalyst transformation in electrocatalysis require activity ...The urea oxidization reaction(UOR)is an important anodic reaction in electro-catalytic energy conversion.However,the sluggish reaction kinetics and complex catalyst transformation in electrocatalysis require activity improvement and better mechanistic understanding of the state-of-the-art Ni(OH)_(2) catalyst.Herein,by utilizing low-temperature argon(Ar)plasma processing,tooth-wheel Ni(OH)_(2) nanosheets self-supported on Ni foam(Ni(OH)_(2)-Ar)are demonstrated to have improved UOR activity compared to conventional Ni(OH)_(2).The theoretical assessment confirms that the edge has a smaller cation vacancy formation energy than the basal plane,consequently explaining the structural formation.Operando and quasi-operando methods are employed to investigate the dynamic evolution of the Ni(OH)_(2) film in UOR.The crucial dehydrogenation products of Ni(OH)_(5)O^(-)intermediates are identified to be stable on the etched edge and explain the enhanced UOR in the low potential region.In addition,the dynamic active sites are monitored to elucidate the reaction mechanism in different potential ranges.展开更多
The selection of the most suitable crystal structure for ions storage and the investigation of the corresponding reaction mechanism is still an ongoing challenge for the development of Mg-based batteries.In this artic...The selection of the most suitable crystal structure for ions storage and the investigation of the corresponding reaction mechanism is still an ongoing challenge for the development of Mg-based batteries.In this article,high flexible graphene network supporting different crystal structures of Nb2 O5(TTNb_(2)O_(5)@rGO and T-Nb_(2)O_(5)@rGO) are successfully synthesized by a spray-drying-assisted approach.The three-dimensional graphene framework provides high conductivity and avoids the aggregation of Nb2 O5 nanoparticles.When employed as electrode materials for energy storage applications,TT-Nb_(2)O_(5) delivers a higher discharge capacity of 129.5 mAh g^(-1), about twice that of T-Nb_(2)O_(5) for Mg-storage,whereas,T-Nb_(2)O_(5) delivers a much higher capacity(162 mAh g^(-1)) compared with TT-Nb_(2)O_(5)(129 mAh g^(-1)) for Li-storage.Detailed investigations reveal the Mg intercalation mechanism and lower Mg^(2+) migration barriers,faster Mg^(2+) diffusion kinetics of TT-Nb_(2)O_(5) as cathode material for Mg-storage,and the faster Li+ diffusion kinetics,shorter diffusion distance of T-Nb_(2)O_(5) as cathode material for Li-storage.Our work demonstrates that exploring the proper crystal structure of Nb2 O5 for different ions storage is necessary.展开更多
In this work,homogeneous Ni0.33Co0.67Se hollow nanoprisms were synthesized successfully in virtue of Kirkendall effect.It is the first time for bimetallic Ni-Co compounds Ni0.33Co0.67Se to be used in lithium-ion batte...In this work,homogeneous Ni0.33Co0.67Se hollow nanoprisms were synthesized successfully in virtue of Kirkendall effect.It is the first time for bimetallic Ni-Co compounds Ni0.33Co0.67Se to be used in lithium-ion batteries (LIBs).Impressively,the Ni0.33Co0.67Se hollow nanoprisms show superior specific capacity (1,575 mAh/g at the current density of 100 mA/g) and outstanding rate performance (850 mAh/g at 2,000 mA/g) as anode material for LIBs.This work proves the potential of bimetallic chalcogenide compounds as high performance anode materials for LIBs.展开更多
Rechargeable magnesium batteries are identified as a promising next-generation energy storage system,but their development is hindered by the anode−electrolyte−cathode incompatibilities and passivation of magnesium me...Rechargeable magnesium batteries are identified as a promising next-generation energy storage system,but their development is hindered by the anode−electrolyte−cathode incompatibilities and passivation of magnesium metal anode.To avoid or alleviate these problems,the exploitation of alternative anode materials is a promising choice.Herein,we present titanium pyrophosphate(TiP_(2)O_(7))as anode materials for magnesium-ion batteries(MIBs)and investigate the effect of the crystal phase on its magnesium storage performance.Compared with the me-tastable layered TiP_(2)O_(7),the thermodynamically stable cubic TiP_(2)O_(7) displays a better rate capability of 72 mAh g^(−1) at 5000 mA g^(−1).Moreover,cubic TiP_(2)O_(7) exhibits excellent cycling stability with the capacity of 60 mAh g^(−1) after 5000 cycles at 1000 mA g^(−1),which are better than pre-viously reported Ti-based anode materials for MIBs.In situ X-ray diffraction technology confirms the single-phase magnesiumion inter-calation/deintercalation reaction mechanism of cubic TiP_(2)O_(7) with a low volume change of 3.2%.In addition,the density functional theory calcu-lation results demonstrate that three-dimensional magnesiumion diffu-sion can be allowed in cubic TiP_(2)O_(7) with a low migration energy barrier of 0.62 eV.Our work demonstrates the promise of TiP_(2)O_(7) as high-rate and long-life anode materials for MIBs and may pave the way for further development of MIBs.展开更多
Molybdenum-based materials have stepped into the spotlight as promising electrodes for energy storage systems due to their abundant valence states,low cost,and high theoretical capacity.However,the performance of conv...Molybdenum-based materials have stepped into the spotlight as promising electrodes for energy storage systems due to their abundant valence states,low cost,and high theoretical capacity.However,the performance of conventional molybdenum-based electrode materials has been limited by slow diffusion dynamics and deficient thermodynamics.Applying defect engineering to molybdenum-based electrode materials is a viable method for overcoming these intrinsic limitations to realize superior electrochemical performance for energy storage.Herein,we systematically review recent progress in defect engineering for molybdenum-based electrode materials,including vacancy modulation,doping engineering,topochemical substitution,and amorphization.In particular,the essential optimization mechanisms of defect engineering in molybdenum-based electrode materials are pre-sented:accelerating ion diffusion,enhancing electron transfer,adjusting potential,and maintaining structural stability.We also discuss the existing challenges and future objectives for defect engineering in molybdenum-based electrode materials to realize high-energy and high-power energy storage devices.展开更多
镁离子电池由于具有高安全性、低成本等优点,近年来受到了广泛的关注.然而,镁离子缓慢的扩散动力学使其难以找到合适的具有良好电化学性能的正极材料.在此,我们设计并合成了一种新颖的柔性三维网络钒酸铁纳米片阵列/碳布(3D FeVO/CC)作...镁离子电池由于具有高安全性、低成本等优点,近年来受到了广泛的关注.然而,镁离子缓慢的扩散动力学使其难以找到合适的具有良好电化学性能的正极材料.在此,我们设计并合成了一种新颖的柔性三维网络钒酸铁纳米片阵列/碳布(3D FeVO/CC)作为镁离子电池的无粘结剂正极材料.与原始钒酸铁纳米片(FeVO)相比,结构改善的3D无粘结剂电极能够实现全面的电化学性能优化,包括高比容量(270 mA h g^(-1))和更长的循环寿命(超过5000次循环).这种可实现的高能量密度来源于电子和离子动力学的协同优化,而循环稳定性得益于稳固的分级结构.本文采用原位X射线衍射和拉曼技术对镁离子储存过程中FeVO单相反应机理进行了研究.此外,还组装了柔性镁离子全电池(3D FeVO/CC|MgNaTi(3)O_(7)),并展示出一定的应用潜力.本工作证明了3D FeVO/CC是一种有潜力的正极材料,可以满足高性能镁离子电池的要求,也为提高镁离子电池正极材料的电化学性能开辟了一条新的途径.展开更多
低成本、高容量金属氧化物/氢氧化物作为具有更高能量密度的锂离子电池的负极材料时具有显著优势.合理调控金属氧化物/氢氧化物的中空结构和无序的原子框架是提高其电化学性能的有效途径.本文提出了一种快速碱刻蚀方法,实现了非晶FeOOH...低成本、高容量金属氧化物/氢氧化物作为具有更高能量密度的锂离子电池的负极材料时具有显著优势.合理调控金属氧化物/氢氧化物的中空结构和无序的原子框架是提高其电化学性能的有效途径.本文提出了一种快速碱刻蚀方法,实现了非晶FeOOH分级纳米管的原位构筑.得益于增强的电子/离子动力学和对循环过程中的体积变化的有效缓冲,石墨烯修饰的非晶FeOOH分级纳米管展现出高倍率性能(在2000 mA g^−1的电流密度下容量可达~650 mA h g^−1)和优异的循环稳定性(循环1800次后容量仍保持在463 mA h g^−1),在目前报道的FeOOH基材料中处于领先水平.研究表明碱刻蚀过程中的选择性溶解-再生长机制,即FeVO4的溶解和FeOOH的原位成核再生长在非晶FeOOH分级纳米管的合成过程中具有重要作用.此外,这种选择性溶解-再生长机制是一种合成具有一维分级纳米结构的金属(例如Fe,Mn,Co和Cu)氧化物/羟基氧化物的普适方法.展开更多
Na_(3)(VO)_(2)(PO_(4))_(2)F(NVPOF)has been considered as one potential candidate for sodium-ion batteries because of its high operating voltage and theoretical capacity.However,the poor intrinsic electronic conductivi...Na_(3)(VO)_(2)(PO_(4))_(2)F(NVPOF)has been considered as one potential candidate for sodium-ion batteries because of its high operating voltage and theoretical capacity.However,the poor intrinsic electronic conductivity significantly restricts its widespread application.In response to this drawback,we adopt the optimization strategy of tuning the morphology and structure to boost the electrical conductivity and mitigate the capacity fading.In this paper,NVPOF microspheres with unique porous yolk-shell structure were fabricated via a facile one-step solvothermal method for the first time.By monitoring the morphological evolution with time-dependent experiments,the self-sacrifice and Ostwald ripening mechanism from rough spheres to yolk-shell structure was revealed.Benefited from the favorable interwoven nanosheets shell,inner cavity and porous core structure,the resulting NVPOF electrode exhibits superior rate capability of 63 m A h g^(-1)at 20 C as well as outstanding long-cycling performance with the capacity retention up to 92.1%over 1000 cycles at 5 C.展开更多
基金supported by the National Natural Science Foundation of China(51832004,51521001)the National Key Research and Development Program of China(2016YFA0202603)+2 种基金the Program of Introducing Talents of Discipline to Universities(B17034)the Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-003)the “Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen University。
文摘Sodium-ion storage devices are highly desirable for large-scale energy storage applications owing to the wide availability of sodium resources and low cost.Transition metal nitrides(TMNs)are promising anode materials for sodium-ion storage,while their detailed reaction mechanism remains unexplored.Herein,we synthesize the mesoporous Mo3N2 nanowires(Meso-Mo_(3)N_(2)-NWs).The sodium-ion storage mechanism of Mo3N2 is systematically investigated through in-situ XRD,ex-situ experimental characterizations and detailed kinetics analysis.Briefly,the Mo_(3)N_(2) undergoes a surface pseudocapacitive redox charge storage process.Benefiting from the rapid surface redox reaction,the Meso-Mo_(3)N_(2)-NWs anode delivers high specific capacity(282 m Ah g^(-1) at 0.1 A g^(-1)),excellent rate capability(87 m Ah g^(-1) at 16 A g^(-1))and long cycling stability(a capacity retention of 78.6%after 800 cycles at 1 A g^(-1)).The present work highlights that the surface pseudocapacitive sodium-ion storage mechanism enables to overcome the sluggish sodium-ion diffusion process,which opens a new direction to design and synthesize high-rate sodiumion storage materials.
基金the financial support from City University of Hong Kong Strategic Research Grant(SRG)(7005505)the National Natural Science Foundation of China(51601136 and 51604202)。
文摘The urea oxidization reaction(UOR)is an important anodic reaction in electro-catalytic energy conversion.However,the sluggish reaction kinetics and complex catalyst transformation in electrocatalysis require activity improvement and better mechanistic understanding of the state-of-the-art Ni(OH)_(2) catalyst.Herein,by utilizing low-temperature argon(Ar)plasma processing,tooth-wheel Ni(OH)_(2) nanosheets self-supported on Ni foam(Ni(OH)_(2)-Ar)are demonstrated to have improved UOR activity compared to conventional Ni(OH)_(2).The theoretical assessment confirms that the edge has a smaller cation vacancy formation energy than the basal plane,consequently explaining the structural formation.Operando and quasi-operando methods are employed to investigate the dynamic evolution of the Ni(OH)_(2) film in UOR.The crucial dehydrogenation products of Ni(OH)_(5)O^(-)intermediates are identified to be stable on the etched edge and explain the enhanced UOR in the low potential region.In addition,the dynamic active sites are monitored to elucidate the reaction mechanism in different potential ranges.
基金supported by the National Natural Science Foundation of China(51972259,51832004,51521001)the Fundamental Research Funds for the Central Universities(WUT:2020III043GX,2020III015GX)+2 种基金Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-003)the National Key Research and Development Program of China(2016YFA0202601)the Hubei Provincial Natural Science Foundation of China(2019CFB519)。
文摘The selection of the most suitable crystal structure for ions storage and the investigation of the corresponding reaction mechanism is still an ongoing challenge for the development of Mg-based batteries.In this article,high flexible graphene network supporting different crystal structures of Nb2 O5(TTNb_(2)O_(5)@rGO and T-Nb_(2)O_(5)@rGO) are successfully synthesized by a spray-drying-assisted approach.The three-dimensional graphene framework provides high conductivity and avoids the aggregation of Nb2 O5 nanoparticles.When employed as electrode materials for energy storage applications,TT-Nb_(2)O_(5) delivers a higher discharge capacity of 129.5 mAh g^(-1), about twice that of T-Nb_(2)O_(5) for Mg-storage,whereas,T-Nb_(2)O_(5) delivers a much higher capacity(162 mAh g^(-1)) compared with TT-Nb_(2)O_(5)(129 mAh g^(-1)) for Li-storage.Detailed investigations reveal the Mg intercalation mechanism and lower Mg^(2+) migration barriers,faster Mg^(2+) diffusion kinetics of TT-Nb_(2)O_(5) as cathode material for Mg-storage,and the faster Li+ diffusion kinetics,shorter diffusion distance of T-Nb_(2)O_(5) as cathode material for Li-storage.Our work demonstrates that exploring the proper crystal structure of Nb2 O5 for different ions storage is necessary.
基金supported by the National Key Research and Development Program of China(2020YFA0715000)the National Natural Science Foundation of China(521722315197225951832004)+3 种基金the Fundamental Research Funds for the Central Universities(WUT:2020Ⅲ043GX2020Ⅲ015GX)the support by MOE,Singapore Ministry of Education(Tier 1,A-8000186-01-00)the funding support from Singapore A*STAR CRF Awardthe scholarship support from China Scholarship Council(CSC)under No.202106950024。
基金the National Natural Science Foundation of China (Nos.51425204,51521001,and 51602239)the National Key R&D Program of China (No.2016YFA0202603)+2 种基金the Program of Introducing Talents of Discipline to Universities (No.B17034)the Yellow Crane Talent (Science & Technology) Program of Wuhan Citythe International Science & Technology Cooperation Program of China (No.2013DFA50840).
文摘In this work,homogeneous Ni0.33Co0.67Se hollow nanoprisms were synthesized successfully in virtue of Kirkendall effect.It is the first time for bimetallic Ni-Co compounds Ni0.33Co0.67Se to be used in lithium-ion batteries (LIBs).Impressively,the Ni0.33Co0.67Se hollow nanoprisms show superior specific capacity (1,575 mAh/g at the current density of 100 mA/g) and outstanding rate performance (850 mAh/g at 2,000 mA/g) as anode material for LIBs.This work proves the potential of bimetallic chalcogenide compounds as high performance anode materials for LIBs.
基金supported by the National Key Research and Development Program of China(2016YFA0202603 and 2016YFA0202601)the National Natural Science Fund for Distinguished Young Scholars(51425204)+1 种基金the National Natural Science Foundation of China(51832004,51602239 and 51672307)the International Science&Technology Cooperation Program of China(2013DFA50840)。
基金This study was supported by the National Natural Science Foundation of China(51832004,U1804253,and 51972259)Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-003).
文摘Rechargeable magnesium batteries are identified as a promising next-generation energy storage system,but their development is hindered by the anode−electrolyte−cathode incompatibilities and passivation of magnesium metal anode.To avoid or alleviate these problems,the exploitation of alternative anode materials is a promising choice.Herein,we present titanium pyrophosphate(TiP_(2)O_(7))as anode materials for magnesium-ion batteries(MIBs)and investigate the effect of the crystal phase on its magnesium storage performance.Compared with the me-tastable layered TiP_(2)O_(7),the thermodynamically stable cubic TiP_(2)O_(7) displays a better rate capability of 72 mAh g^(−1) at 5000 mA g^(−1).Moreover,cubic TiP_(2)O_(7) exhibits excellent cycling stability with the capacity of 60 mAh g^(−1) after 5000 cycles at 1000 mA g^(−1),which are better than pre-viously reported Ti-based anode materials for MIBs.In situ X-ray diffraction technology confirms the single-phase magnesiumion inter-calation/deintercalation reaction mechanism of cubic TiP_(2)O_(7) with a low volume change of 3.2%.In addition,the density functional theory calcu-lation results demonstrate that three-dimensional magnesiumion diffu-sion can be allowed in cubic TiP_(2)O_(7) with a low migration energy barrier of 0.62 eV.Our work demonstrates the promise of TiP_(2)O_(7) as high-rate and long-life anode materials for MIBs and may pave the way for further development of MIBs.
基金supported by the National Natural Science Foundation of China(51972259,52172231 and U1804253)Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-003)the Fundamental Research Funds for the Central Universities(WUT:2021III024GX,2021III001GL).
文摘Molybdenum-based materials have stepped into the spotlight as promising electrodes for energy storage systems due to their abundant valence states,low cost,and high theoretical capacity.However,the performance of conventional molybdenum-based electrode materials has been limited by slow diffusion dynamics and deficient thermodynamics.Applying defect engineering to molybdenum-based electrode materials is a viable method for overcoming these intrinsic limitations to realize superior electrochemical performance for energy storage.Herein,we systematically review recent progress in defect engineering for molybdenum-based electrode materials,including vacancy modulation,doping engineering,topochemical substitution,and amorphization.In particular,the essential optimization mechanisms of defect engineering in molybdenum-based electrode materials are pre-sented:accelerating ion diffusion,enhancing electron transfer,adjusting potential,and maintaining structural stability.We also discuss the existing challenges and future objectives for defect engineering in molybdenum-based electrode materials to realize high-energy and high-power energy storage devices.
基金supported by the National Key Research and Development Program of China(2020YFA0715000)the National Natural Science Foundation of China(51832004 and 51972259)+1 种基金the Natural Science Foundation of Hubei Province(2019CFA001)Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-003)。
文摘镁离子电池由于具有高安全性、低成本等优点,近年来受到了广泛的关注.然而,镁离子缓慢的扩散动力学使其难以找到合适的具有良好电化学性能的正极材料.在此,我们设计并合成了一种新颖的柔性三维网络钒酸铁纳米片阵列/碳布(3D FeVO/CC)作为镁离子电池的无粘结剂正极材料.与原始钒酸铁纳米片(FeVO)相比,结构改善的3D无粘结剂电极能够实现全面的电化学性能优化,包括高比容量(270 mA h g^(-1))和更长的循环寿命(超过5000次循环).这种可实现的高能量密度来源于电子和离子动力学的协同优化,而循环稳定性得益于稳固的分级结构.本文采用原位X射线衍射和拉曼技术对镁离子储存过程中FeVO单相反应机理进行了研究.此外,还组装了柔性镁离子全电池(3D FeVO/CC|MgNaTi(3)O_(7)),并展示出一定的应用潜力.本工作证明了3D FeVO/CC是一种有潜力的正极材料,可以满足高性能镁离子电池的要求,也为提高镁离子电池正极材料的电化学性能开辟了一条新的途径.
基金This work was supported by the National Key Research and Development Program of China(2017YFE0127600,2016YFA0202600)the Program of Introducing Talents of Discipline to Universities(B17034)+3 种基金the National Natural Science Foundation of China(51521001 and 51602239)the National Natural Science Fund for Distinguished Young Scholars(51425204)Hubei Provincial Natural Science Foundation(2016CFB267)the Fundamental Research Funds for the Central Universities(WUT:2017-YB-001).
文摘低成本、高容量金属氧化物/氢氧化物作为具有更高能量密度的锂离子电池的负极材料时具有显著优势.合理调控金属氧化物/氢氧化物的中空结构和无序的原子框架是提高其电化学性能的有效途径.本文提出了一种快速碱刻蚀方法,实现了非晶FeOOH分级纳米管的原位构筑.得益于增强的电子/离子动力学和对循环过程中的体积变化的有效缓冲,石墨烯修饰的非晶FeOOH分级纳米管展现出高倍率性能(在2000 mA g^−1的电流密度下容量可达~650 mA h g^−1)和优异的循环稳定性(循环1800次后容量仍保持在463 mA h g^−1),在目前报道的FeOOH基材料中处于领先水平.研究表明碱刻蚀过程中的选择性溶解-再生长机制,即FeVO4的溶解和FeOOH的原位成核再生长在非晶FeOOH分级纳米管的合成过程中具有重要作用.此外,这种选择性溶解-再生长机制是一种合成具有一维分级纳米结构的金属(例如Fe,Mn,Co和Cu)氧化物/羟基氧化物的普适方法.
基金financially supported by the National Natural Science Foundation of China(No.51972259)the Hubei Provincial Natural Science Foundation of China(No.2019CFB519)+1 种基金the Fundamental Research Funds for the Central Universities(No.WUT:2020Ⅲ015GX)the National innovation and entrepreneurship training program for Undergraduate(No.201910497011)。
文摘Na_(3)(VO)_(2)(PO_(4))_(2)F(NVPOF)has been considered as one potential candidate for sodium-ion batteries because of its high operating voltage and theoretical capacity.However,the poor intrinsic electronic conductivity significantly restricts its widespread application.In response to this drawback,we adopt the optimization strategy of tuning the morphology and structure to boost the electrical conductivity and mitigate the capacity fading.In this paper,NVPOF microspheres with unique porous yolk-shell structure were fabricated via a facile one-step solvothermal method for the first time.By monitoring the morphological evolution with time-dependent experiments,the self-sacrifice and Ostwald ripening mechanism from rough spheres to yolk-shell structure was revealed.Benefited from the favorable interwoven nanosheets shell,inner cavity and porous core structure,the resulting NVPOF electrode exhibits superior rate capability of 63 m A h g^(-1)at 20 C as well as outstanding long-cycling performance with the capacity retention up to 92.1%over 1000 cycles at 5 C.
