Although it has been proven that porous,heteroatomic,and defective structures improve Na storage performance,they also severely affect the initial Coulombic efficiency(ICE)due to the huge irreversible capacity in the ...Although it has been proven that porous,heteroatomic,and defective structures improve Na storage performance,they also severely affect the initial Coulombic efficiency(ICE)due to the huge irreversible capacity in the first cycle,which always limits the practical application of carbon anodes in commercial Na-ion batteries(NIBs).Here,we show the successful synthesis of nanocrystalline cellulose and the derivative hard carbons.A series of treatments including acid hydrolysis,hydrothermal carbonization,and hightemperature pyrolysis help tune the pores,heteroatoms,and defects to achieve an optimized balance between superior ICE and reversible capacity of up to 90.4%and 314 mAh g^(−1).This study highlights that tailoring the electrode microstructure could be an important strategy in the future design of carbonaceous anode materials for high-performance Na-ion batteries.展开更多
Layered oxides are one of the most prom ising cathode materials for sodium ion batteries (NIBs), however, the relatively low working voltage hinders the increase of energy density thus limiting the application scenari...Layered oxides are one of the most prom ising cathode materials for sodium ion batteries (NIBs), however, the relatively low working voltage hinders the increase of energy density thus limiting the application scenarios of NIBs. Here we prepared and investigated a series of Sn^4+ substituted NaO.67NiO.33M na67-xSnxO2 (x = 0.10, 0.20, 0.30, 0.33) and found that Sn-substitution can induce three effects: promoting O3-stack formation, sm oothing the voltage profile and increasing the working voltage to -3.6 V. This study would enrich the knowledge of Sn-substitution and give guide to the better design of high-voltage cathode materials for NIBs.展开更多
Na-ion batteries(NIBs)are regarding as the optimum complement for Li-ion batteries along with the rapid development of stationary energy storage systems.In order to meet the commercial demands of cathodes for NIBs,O3-...Na-ion batteries(NIBs)are regarding as the optimum complement for Li-ion batteries along with the rapid development of stationary energy storage systems.In order to meet the commercial demands of cathodes for NIBs,O3-type Cu containing layered oxide Na_(0.9)0Cu_(0.22)Fe_(0.30)Mn_(0.48O_(2))with good comprehensive performance and low-cost element components is very promising for the practical use.However,only part of the Cu^(3+)/Cu^(2+)redox couple participated in the redox reaction,thus impairing the specific capacity of the cathode materials.Herein,Mg2+-doped O3-Na0.90Mg0.08Cu0.22Fe0.30Mn0.40O_(2)layered oxide without Mn3+was synthesized successfully,which exhibited improved reversible specific capacity of 118 mAh/g in the voltage range of 2.4-4.0 V at 0.2 C,corresponding to the intercalation/deintercalation of 0.47 Na+(0.1 more than that of Na_(0.9)0Cu_(0.22)Fe_(0.30)Mn_(0.48O_(2))).This work demonstrates an important strategy to obtain advanced layered oxide cathodes for NIBs.展开更多
The anionic redox reaction(ARR)is a promising charge contributor to improve the reversible capacity of layeredoxide cathodes for Na-ion batteries;however,some practical bottlenecks still need to be eliminated,includin...The anionic redox reaction(ARR)is a promising charge contributor to improve the reversible capacity of layeredoxide cathodes for Na-ion batteries;however,some practical bottlenecks still need to be eliminated,including a low capacity retention,large voltage hysteresis,and low rate capability.Herein,we proposed a high-Na content honeycomb-ordered cathode,P2–Na_(5/6)[Li_(1/6)Cu_(1/6)Mn_(2/3)]O_(2)(P2-NLCMO),with combined cationic/anionic redox.Neutron powder diffraction and X-ray diffraction of P2-NLCMO suggested P2-type stacking with rarely found P6322 symmetry.In addition,advanced spectroscopy techniques and density functional theory calculations confirmed the synergistic stabilizing relationship between the Li/Cu dual honeycomb centers,achieving fully active Cu^(3+)/Cu^(2+) redox and stabilized ARR with interactively suppressed local distortion.With a meticulously regulated charge/discharge protocol,both the cycling and rate capability of P2-NLCMO were significantly.展开更多
Na-ion batteries(NIBs)have received significant interest as potential candidates for large-scale energy storage owing to the widespread distribution of sodium and superior low-temperature performance.However,their com...Na-ion batteries(NIBs)have received significant interest as potential candidates for large-scale energy storage owing to the widespread distribution of sodium and superior low-temperature performance.However,their commercial application is usually hindered by the high production cost and inadequate performance for electrode materials,particularly for cathodes.Na_(3)(VOPO_(4))_(2)F(NVOPF)has been recognized as one of the most promising cathodes for high-energy NIBs owing to the high working voltage and energy density.Here,we report a facile highly efficient room-temperature solution protocol for large-scale synthesis of NVOPF cathode for NIBs.By simply regulating pH,NVOPF can be obtained,which delivered a discharge capacity of 120.2 mAh g^(-1) at 0.1 C and 72%capacity retention over 8000 cycles at 25 C.Besides,the kilogram-level NVOPF products have been synthesized,and 26650 cylindrical cells were fabricated,which exhibit excellent cycling stabilities,remarkable lowtemperature performance with comparable safety features.We hope our findings could provide insights on the industrial application of NVOPF in NIBs.展开更多
Electrochemical energy storage technologies have a profound influence on daily life,and their development heavily relies on innovations in materials science.Recently,high-entropy materials have attracted increasing re...Electrochemical energy storage technologies have a profound influence on daily life,and their development heavily relies on innovations in materials science.Recently,high-entropy materials have attracted increasing research interest worldwide.In this perspective,we start with the early development of high-entropy materials and the calculation of the configurational entropy.Then,we summarize the recent progress in material design and application using the high-entropy strategy,espe-cially highlighting rechargeable battery materials.Finally,we discuss the potential directions for the future development of high-entropy energy materials.展开更多
基金Natural Science Foundation of Beijing Municipality,Grant/Award Number:2212022Science and Technology Facilities Council,Grant/Award Number:ST/R006873/1+3 种基金China Postdoctoral Science Foundation,Grant/Award Number:2021M693367National Natural Science Foundation of China,Grant/Award Numbers:51725206,51861165201,52072403,52122214Engineering and Physical Sciences Research Council,Grant/Award Numbers:EP/R021554/2,EP/S018204/2Chinese Academy of Sciences,Grant/Award Numbers:2020006,XDA21070500。
文摘Although it has been proven that porous,heteroatomic,and defective structures improve Na storage performance,they also severely affect the initial Coulombic efficiency(ICE)due to the huge irreversible capacity in the first cycle,which always limits the practical application of carbon anodes in commercial Na-ion batteries(NIBs).Here,we show the successful synthesis of nanocrystalline cellulose and the derivative hard carbons.A series of treatments including acid hydrolysis,hydrothermal carbonization,and hightemperature pyrolysis help tune the pores,heteroatoms,and defects to achieve an optimized balance between superior ICE and reversible capacity of up to 90.4%and 314 mAh g^(−1).This study highlights that tailoring the electrode microstructure could be an important strategy in the future design of carbonaceous anode materials for high-performance Na-ion batteries.
基金supported financially by the Funding from the Science and Technology Project of the State Grid Corporation of China (No. DG71-16-027, research on key technology of low-strain layered oxides for long-life Na-ion batteries)
文摘Layered oxides are one of the most prom ising cathode materials for sodium ion batteries (NIBs), however, the relatively low working voltage hinders the increase of energy density thus limiting the application scenarios of NIBs. Here we prepared and investigated a series of Sn^4+ substituted NaO.67NiO.33M na67-xSnxO2 (x = 0.10, 0.20, 0.30, 0.33) and found that Sn-substitution can induce three effects: promoting O3-stack formation, sm oothing the voltage profile and increasing the working voltage to -3.6 V. This study would enrich the knowledge of Sn-substitution and give guide to the better design of high-voltage cathode materials for NIBs.
基金supported by the National Natural Science Foundation of China(Grant Nos.51725206,52122214,and 52072403)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA21070500)+1 种基金Youth Innovation Promotion Association of the Chinese Academy of Sciences(Grant No.2020006)Beijing Municipal Natural Science Foundation,China(Grant No.2212022)。
文摘Na-ion batteries(NIBs)are regarding as the optimum complement for Li-ion batteries along with the rapid development of stationary energy storage systems.In order to meet the commercial demands of cathodes for NIBs,O3-type Cu containing layered oxide Na_(0.9)0Cu_(0.22)Fe_(0.30)Mn_(0.48O_(2))with good comprehensive performance and low-cost element components is very promising for the practical use.However,only part of the Cu^(3+)/Cu^(2+)redox couple participated in the redox reaction,thus impairing the specific capacity of the cathode materials.Herein,Mg2+-doped O3-Na0.90Mg0.08Cu0.22Fe0.30Mn0.40O_(2)layered oxide without Mn3+was synthesized successfully,which exhibited improved reversible specific capacity of 118 mAh/g in the voltage range of 2.4-4.0 V at 0.2 C,corresponding to the intercalation/deintercalation of 0.47 Na+(0.1 more than that of Na_(0.9)0Cu_(0.22)Fe_(0.30)Mn_(0.48O_(2))).This work demonstrates an important strategy to obtain advanced layered oxide cathodes for NIBs.
基金supported by the National Natural Science Foundation(NSFC)of China(52002394)Young Elite Scientists Sponsorship Program by CAST(2022QNRC001)Youth Innovation Promotion Association of the Chinese Academy of Sciences(2020006).
文摘The anionic redox reaction(ARR)is a promising charge contributor to improve the reversible capacity of layeredoxide cathodes for Na-ion batteries;however,some practical bottlenecks still need to be eliminated,including a low capacity retention,large voltage hysteresis,and low rate capability.Herein,we proposed a high-Na content honeycomb-ordered cathode,P2–Na_(5/6)[Li_(1/6)Cu_(1/6)Mn_(2/3)]O_(2)(P2-NLCMO),with combined cationic/anionic redox.Neutron powder diffraction and X-ray diffraction of P2-NLCMO suggested P2-type stacking with rarely found P6322 symmetry.In addition,advanced spectroscopy techniques and density functional theory calculations confirmed the synergistic stabilizing relationship between the Li/Cu dual honeycomb centers,achieving fully active Cu^(3+)/Cu^(2+) redox and stabilized ARR with interactively suppressed local distortion.With a meticulously regulated charge/discharge protocol,both the cycling and rate capability of P2-NLCMO were significantly.
基金This work was supported by the National Natural Science Foundation(NSFC)of China(51725206,52122214,and 52072403)Beijing Natural Science Foundation(2222078)+4 种基金the Science and Technology Project of Inner Mongolia(2021GG0162)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21070500)Youth Innovation Promotion Association of the Chinese Academy of Sciences(2020006)Beijing Municipal Natural Science Foundation(2212022)Innovation Academy for Green Manufacture,CAS(IAGM2020C07).
文摘Na-ion batteries(NIBs)have received significant interest as potential candidates for large-scale energy storage owing to the widespread distribution of sodium and superior low-temperature performance.However,their commercial application is usually hindered by the high production cost and inadequate performance for electrode materials,particularly for cathodes.Na_(3)(VOPO_(4))_(2)F(NVOPF)has been recognized as one of the most promising cathodes for high-energy NIBs owing to the high working voltage and energy density.Here,we report a facile highly efficient room-temperature solution protocol for large-scale synthesis of NVOPF cathode for NIBs.By simply regulating pH,NVOPF can be obtained,which delivered a discharge capacity of 120.2 mAh g^(-1) at 0.1 C and 72%capacity retention over 8000 cycles at 25 C.Besides,the kilogram-level NVOPF products have been synthesized,and 26650 cylindrical cells were fabricated,which exhibit excellent cycling stabilities,remarkable lowtemperature performance with comparable safety features.We hope our findings could provide insights on the industrial application of NVOPF in NIBs.
基金supported by the National Key R&D Program of China(2022YFB3807800)the National Natural Science Foundation of China(52122214 and 52202332)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2020006).
文摘Electrochemical energy storage technologies have a profound influence on daily life,and their development heavily relies on innovations in materials science.Recently,high-entropy materials have attracted increasing research interest worldwide.In this perspective,we start with the early development of high-entropy materials and the calculation of the configurational entropy.Then,we summarize the recent progress in material design and application using the high-entropy strategy,espe-cially highlighting rechargeable battery materials.Finally,we discuss the potential directions for the future development of high-entropy energy materials.
