Sodium-ion batteries stand a chance of enabling fast charging ability and long lifespan while operating at low temperature(low-T).However,sluggish kinetics and aggravated dendrites present two major challenges for ano...Sodium-ion batteries stand a chance of enabling fast charging ability and long lifespan while operating at low temperature(low-T).However,sluggish kinetics and aggravated dendrites present two major challenges for anodes to achieve the goal at low-T.Herein,we propose an interlayer confined strategy for tailoring nitrogen terminals on Ti_(3)C_(2) MXene(Ti_(3)C_(2)-N_(funct)) to address these issues.The introduction of nitrogen terminals endows Ti_(3)C_(2)-N_(funct) with large interlayer space and charge redistribution,improved conductivity and sufficient adsorption sites for Na^(+),which improves the possibility of Ti_(3)C_(2) for accommodating more Na atoms,further enhancing the Na^(+) storage capability of Ti_(3)C_(2).As revealed,Ti_(3)C_(2)-N_(funct) not only possesses a lower Na-ion diffusion energy barrier and charge trans-fer activation energy,but also exhibits Na^(+)-solvent co-intercalation behavior to circumvent a high de-solvation energy barrier at low-T.Besides,the solid electrolyte interface dominated by inorganic com-pounds is more beneficial for the Na^(+)transfer at the electrode/electrolyte interface.Compared with of the unmodified sample,Ti_(3)C_(2)-Nfunct exhibits a twofold capacity(201 mAh g^(-1)),fast-charging ability(18 min at 80% capacity retention),and great superiority in cycle life(80.9%@5000 cycles)at -25℃.When coupling with Na_(3)V_(2)(PO_(4))_(2)F_(3) cathode,the Ti_(3)C_(2)-N_(funct)//NVPF exhibits high energy density and cycle stability at -25℃.展开更多
Lithium-sulfur(Li-S)batteries with high theoretical capacity and energy density need to solve problems such as the high decomposition energy barrier of Li2S and large volume change of sulfur in the charging process ca...Lithium-sulfur(Li-S)batteries with high theoretical capacity and energy density need to solve problems such as the high decomposition energy barrier of Li2S and large volume change of sulfur in the charging process caused by the shuttle effect before practical application.Herein,a green synthesis method is used to prepare polyacrylic acid(PAA)superabsorbent material,and then the pyrolyzed PAA(P/PAA)material is obtained as the positive electrode of Li-S battery.Density functional calculation reveals that the oxygen self-doping pyrolyzed polyacrylic acid(P/PAA)delivered stronger binding energy toward Li2S species in carbonyl C=O than that of graphite powder(GP)which are-1.58 eV and-1.02 eV,respectively.Coupled with the distribution of relaxation time analysis and the in-situ electrochemical impedance approach,it is further demonstrated that the designed P/PAA as sulfur host plays a physical/chemical adsorption dual function in maintaining the stability and rate performance of batteries.With an initial discharge capacity of 1258 mAh/g at 0.1 C and a minimal capacity decline of 0.05%per cycle even after 800 cycles at 0.5 C,the produced cathode demonstrated outstanding electrochemical performance.The average Coulombic efficiency is nearly 100%.The P/PAA electrodes may typically retain 96%of their capacity while declining on average only 0.033%per cycle after 130 cycles at 3 C.This effort provides a new method for the future development of heteroatomic self-doping superabsorbent with promising adsorption properties for polysulfides as cathode materials of Li-S batteries.展开更多
基金the National Natural Sci-ence Foundation of China(Grant Nos.21673064,51902072 and 22109033)Heilongjiang Touyan Team(Grant No.HITTY-20190033)+1 种基金Fundamental Research Funds for the Central Universities(Grant Nos.HIT.NSRIF.2019040 and 2019041)State Key Laboratory of Urban Water Resource and Environment(Harbin Institute of Technology)(Grant No.2020 DX11).
文摘Sodium-ion batteries stand a chance of enabling fast charging ability and long lifespan while operating at low temperature(low-T).However,sluggish kinetics and aggravated dendrites present two major challenges for anodes to achieve the goal at low-T.Herein,we propose an interlayer confined strategy for tailoring nitrogen terminals on Ti_(3)C_(2) MXene(Ti_(3)C_(2)-N_(funct)) to address these issues.The introduction of nitrogen terminals endows Ti_(3)C_(2)-N_(funct) with large interlayer space and charge redistribution,improved conductivity and sufficient adsorption sites for Na^(+),which improves the possibility of Ti_(3)C_(2) for accommodating more Na atoms,further enhancing the Na^(+) storage capability of Ti_(3)C_(2).As revealed,Ti_(3)C_(2)-N_(funct) not only possesses a lower Na-ion diffusion energy barrier and charge trans-fer activation energy,but also exhibits Na^(+)-solvent co-intercalation behavior to circumvent a high de-solvation energy barrier at low-T.Besides,the solid electrolyte interface dominated by inorganic com-pounds is more beneficial for the Na^(+)transfer at the electrode/electrolyte interface.Compared with of the unmodified sample,Ti_(3)C_(2)-Nfunct exhibits a twofold capacity(201 mAh g^(-1)),fast-charging ability(18 min at 80% capacity retention),and great superiority in cycle life(80.9%@5000 cycles)at -25℃.When coupling with Na_(3)V_(2)(PO_(4))_(2)F_(3) cathode,the Ti_(3)C_(2)-N_(funct)//NVPF exhibits high energy density and cycle stability at -25℃.
基金the financial support of the National Natural Science Foundation of China(Nos.22271106,21501175 and 2227518)the Natural Science Foundation of Fujian Province(No.2022Y0071)the Leading Project Foundation of Science Department of Fujian Province(No.2023H0045)。
文摘Lithium-sulfur(Li-S)batteries with high theoretical capacity and energy density need to solve problems such as the high decomposition energy barrier of Li2S and large volume change of sulfur in the charging process caused by the shuttle effect before practical application.Herein,a green synthesis method is used to prepare polyacrylic acid(PAA)superabsorbent material,and then the pyrolyzed PAA(P/PAA)material is obtained as the positive electrode of Li-S battery.Density functional calculation reveals that the oxygen self-doping pyrolyzed polyacrylic acid(P/PAA)delivered stronger binding energy toward Li2S species in carbonyl C=O than that of graphite powder(GP)which are-1.58 eV and-1.02 eV,respectively.Coupled with the distribution of relaxation time analysis and the in-situ electrochemical impedance approach,it is further demonstrated that the designed P/PAA as sulfur host plays a physical/chemical adsorption dual function in maintaining the stability and rate performance of batteries.With an initial discharge capacity of 1258 mAh/g at 0.1 C and a minimal capacity decline of 0.05%per cycle even after 800 cycles at 0.5 C,the produced cathode demonstrated outstanding electrochemical performance.The average Coulombic efficiency is nearly 100%.The P/PAA electrodes may typically retain 96%of their capacity while declining on average only 0.033%per cycle after 130 cycles at 3 C.This effort provides a new method for the future development of heteroatomic self-doping superabsorbent with promising adsorption properties for polysulfides as cathode materials of Li-S batteries.