Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique ...Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.展开更多
Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully syn...Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.展开更多
Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising...Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising potential in balancing structural stability and enhancing reaction kinetics.However,their controlled synthesis mechanisms remain elusive.Herein,a substrate interface engineering strategy is developed to achieve controllable synthesis of mesocrystalline and polycrystalline NiCo_(2)O_(4) nanorods.Remarkably,mesocrystalline NiCo_(2)O_(4) exhibits a high capacity retention rate of 85.7% after 500 cycles at 2 A/g,attributed to its porous structure facilitating Li^(+) transport kinetics and unique stress-buffering effect validated by ex-situ TEM.Theoretical calculations and interfacial chemical analysis reveal that substratecrystal surface engineering regulates the nucleation-growth pathways:Acid-treated nickel foam enables epitaxial growth via lattice matching,acting as a low-interfacial-energy template to reduce nucleation barriers and promote low-temperature oriented crystallization.In contrast,carbon cloth requires hightemperature thermal activation to overcome surface diffusion barriers induced by elevated interfacial energy.This substrate-driven crystallization kinetic modulation overcomes the limitations of random nucleation in conventional hydrothermal synthesis.The established substrate-crystal interfacial interaction model not only clarifies the kinetic essence of crystal orientation regulation but also provides a universal theoretical framework for lattice-matching design and mesostructural optimization of advanced electrode materials.展开更多
基金supported by the National Nature Science Foundation of China(Nos.52202335 and 52171227)Natural Science Foundation of Jiangsu Province(No.BK20221137)National Key R&D Program of China(2024YFE0108500).
文摘Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.
基金financially supported by the National Natural Science Foundation of China (52272209)
文摘Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.
基金financially supported by the National Nature Science Foundation of China (No.52401273)Science and Technology Department of Henan (Nos.242102241007,252102320178 and 252102321067)Training Program for Young Backbone Teachers in Higher Education Institutions in Henan Province (No.2024GGJS101)。
文摘Structural instability and sluggish lithium-ion(Li+) kinetics of spinel NiCo_(2)O_(4) anodes severely hinder their applications in high-energy-density lithium-ion batteries.Mesocrystalline structures exhibit promising potential in balancing structural stability and enhancing reaction kinetics.However,their controlled synthesis mechanisms remain elusive.Herein,a substrate interface engineering strategy is developed to achieve controllable synthesis of mesocrystalline and polycrystalline NiCo_(2)O_(4) nanorods.Remarkably,mesocrystalline NiCo_(2)O_(4) exhibits a high capacity retention rate of 85.7% after 500 cycles at 2 A/g,attributed to its porous structure facilitating Li^(+) transport kinetics and unique stress-buffering effect validated by ex-situ TEM.Theoretical calculations and interfacial chemical analysis reveal that substratecrystal surface engineering regulates the nucleation-growth pathways:Acid-treated nickel foam enables epitaxial growth via lattice matching,acting as a low-interfacial-energy template to reduce nucleation barriers and promote low-temperature oriented crystallization.In contrast,carbon cloth requires hightemperature thermal activation to overcome surface diffusion barriers induced by elevated interfacial energy.This substrate-driven crystallization kinetic modulation overcomes the limitations of random nucleation in conventional hydrothermal synthesis.The established substrate-crystal interfacial interaction model not only clarifies the kinetic essence of crystal orientation regulation but also provides a universal theoretical framework for lattice-matching design and mesostructural optimization of advanced electrode materials.
