Aqueous ammonium batteries(AAIBs)gain extensive attention because of their merits,such as costeffectiveness,eco-friendliness,and safety.Nevertheless,the limited research on electrode materials impedes their further de...Aqueous ammonium batteries(AAIBs)gain extensive attention because of their merits,such as costeffectiveness,eco-friendliness,and safety.Nevertheless,the limited research on electrode materials impedes their further development.Here,we prepare Cu_(x)O(x=1,2)materials and apply them as cathode materials for AAIBs.The electrodes have a high discharge-specific capacity and a long and stable charge-discharge plateau.In accordance with density functional theory,the mechanism of NH_(4)^(+)storage involves the reversible formation and breaking of hydrogen bonds.Simultaneously,CuO contributes additional electrons and facilitates the rearrangement of internal electrons,thereby enhancing the storage performance of NH_(4)^(+).To further improve the chemical reaction kinetics and address the limited cycle stability of CuO,a compositematerial composed of CuO and carbon(CuO/C)is developed.The findings demonstrate that CuO/C exhibits superior rate capability,with an initial discharge-specific capacity reaching 1851 mAh g^(-1)(0.1 A g^(-1))and improved reversible cycle performance(113 mAh g^(-1)after 400cycles).This study investigates the application of CuO as the cathode material in AAIBs and presents new opportunities for future industrial development.展开更多
To tackle energy crisis and achieve sustainable development, aqueous rechargeable zinc ion batteries have gained widespread attention in large-scale energy storage for their low cost, high safety, high theoretical cap...To tackle energy crisis and achieve sustainable development, aqueous rechargeable zinc ion batteries have gained widespread attention in large-scale energy storage for their low cost, high safety, high theoretical capacity, and environmental compatibility in recent years. However, zinc anode in aqueous zinc ion batteries is still facing several challenges such as dendrite growth and side reactions(e.g., hydrogen evolution), which cause poor reversibility and the failure of batteries. To address these issues, interfacial modification of Zn anodes has received great attention by tuning the interaction between the anode and the electrolyte. Herein, we present recent advances in the interfacial modification of zinc anode in this review. Besides, the challenges of reported approaches of interfacial modification are also discussed.Finally, we provide an outlook for the exploration of novel zinc anode for aqueous zinc ion batteries.We hope that this review will be helpful in designing and fabricating dendrite-free and hydrogenevolution-free Zn anodes and promoting the practical application of aqueous rechargeable zinc ion batteries.展开更多
Ni-rich cathodes exhibit appealing properties,such as high capacity density,low cost,and prominent energy density.However,the inferior ionic conductivity and bulk structural degradation become bottlenecks for Ni-rich ...Ni-rich cathodes exhibit appealing properties,such as high capacity density,low cost,and prominent energy density.However,the inferior ionic conductivity and bulk structural degradation become bottlenecks for Ni-rich cathodes and severely limit their commercial utilization.Traditional coating and doping methods suffer fatal drawbacks in functioning as a unit and cannot radically promote material performance to meet the needs of Li-ion batteries(LIBs).Herein,we successfully devised an ingenious and facile synthetic method to establish Ni-rich oxides with a La_(2)Zr_(2)O_(7) coating and Zr doping.The coating layer improves the ion diffusion kinetics and enhances Li-ion transportation while Zr doping effectively suppresses the phase transition of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode.Owing to the synergetic effect of Zr doping and La_(2)Zr_(2)O_(7) coating,the modified material shows prominent initial discharge capacity of 184.7 m Ah g^(-1) at 5℃ and maintains 177.5 m Ah g^(-1) after 100 cycles at 1℃.Overall,the proposed feasible electrode design method can have a far-reaching impact on further fabrication of advanced cathodes for high-performance LIBs.展开更多
The synthesis of layered oxide cathode materials by the traditional high-temperature ceramic method usually requires calcination and annealing at temperatures in the range of 700-1000℃,with high energy consumption an...The synthesis of layered oxide cathode materials by the traditional high-temperature ceramic method usually requires calcination and annealing at temperatures in the range of 700-1000℃,with high energy consumption and serious cation mixing problems.Herein,we present a novel hydrothermalLi^(+)/H^(+)exchange method for the preparation of layered oxide cathodes at temperatures as low as 200℃.In contrast to the widely reported Li^(+)/Na^(+)exchange method using sodium-containing:precursors,layered oxide cathodes can be directly synthesized by hydrothermal reaction between commercial hydroxide precursors and LiOH·H2O.The reaction pathway consists of two steps.(1)The hydroxyl oxide intermediate is obtained by oxidizing the hydroxide precursor.(2)The layered oxide product is obtained by theLi^(+)/H^(+)exchange reaction of the hydroxyl oxide with Li+in solution.Through studying the time-resolved structural evolution,we reveal that the mechanism of material formation duringLi^(+)/H^(+)ion exchange is in situ crystallization,and the ion exchange process is accompanied by lattice distortion caused by internal diffusion of ions.These findings not only provide valuable insights into theLi^(+)/H^(+)exchange process,but also provide a new paradigm for the lowtemperature synthesis of advanced cathode materials.展开更多
Ion exchange is a promising synthetic method for alleviating severe cation mixing in traditional layered oxide materials for lithium-ion batteries,leading to enhanced structural stability.However,the underlying mechan...Ion exchange is a promising synthetic method for alleviating severe cation mixing in traditional layered oxide materials for lithium-ion batteries,leading to enhanced structural stability.However,the underlying mechanisms of ion exchange are still not fully understood.Such a fundamental study of the ion-exchange mechanism is needed for achieving the controllable synthesis of layered oxides with a stable structure.Herein,we thoroughly unearth the underlying mechanism that triggers the ion exchange of Ni-rich materials in aqueous solutions by examining time-resolved structural evolution combined with theoretical calculations.Our results reveal that the reaction pathway of ion exchange can be divided into two steps:protonation and lithiation.The proton is the key to achieving charge balance in the ion exchange process,as revealed by X-ray adsorption spectroscopy and inductive coupled plasma analysis.In addition,the intermediate product shows high lattice distortion during ion exchange,but it ends up with a most stable product with high lattice energy.Such apparent discrepancies in lattice energy between materials before and after ion exchange emphasize the importance of synthetic design in structural stability.This work provides new insights into the ion-exchange synthesis of Ni-rich oxide materials,which advances the development of cathode materials for high-performance lithium-ion batteries.展开更多
Lithium-ion batteries(LIBs)represent the most promising choice for meeting the ever-growing demand of society for various electric applications,such as electric transportation,portable electronics,and grid storage.Nic...Lithium-ion batteries(LIBs)represent the most promising choice for meeting the ever-growing demand of society for various electric applications,such as electric transportation,portable electronics,and grid storage.Nickel-rich layered oxides have largely replaced LiCoO_(2)in commercial batteries because of their low cost,high energy density,and good reliability.Traditional nickel-based oxide particles,usually called polycrystal materials,are composed of microsized primary particles.However,polycrystal particles tend to suffer from pulverization and severe side reactions along grain boundaries during cycling.These phenomena accelerate cell degradation.Single-crystal materials,which exhibit robust mechanical strength and a high surface area,have great potential to address the challenges that hinder their polycrystal counterparts.A comprehensive understanding of the growing body of research related to single-crystal materials is imperative to improve the performance of cathodes in LIBs.This review highlights origins,recent developments,challenges,and opportunities for single-crystal layered oxide cathodes.The synthesis science behind single-crystal materials and comparative studies between single-crystal and polycrystal materials are discussed in detail.Industrial techniques and facilities are also reviewed in combination with our group’s experiences in single-crystal research.Future development should focus on facile production with strong control of the particle size and distribution,structural defects,and impurities to fully reap the benefits of single-crystal materials.展开更多
基金financially supported by the National Natural Scientific Foundation of China(Nos.52371211 and 52171200)Changsha Special Project(No.kh2301006)the Natural Science Foundation of Shandong Province(No.ZR2024QB185)
文摘Aqueous ammonium batteries(AAIBs)gain extensive attention because of their merits,such as costeffectiveness,eco-friendliness,and safety.Nevertheless,the limited research on electrode materials impedes their further development.Here,we prepare Cu_(x)O(x=1,2)materials and apply them as cathode materials for AAIBs.The electrodes have a high discharge-specific capacity and a long and stable charge-discharge plateau.In accordance with density functional theory,the mechanism of NH_(4)^(+)storage involves the reversible formation and breaking of hydrogen bonds.Simultaneously,CuO contributes additional electrons and facilitates the rearrangement of internal electrons,thereby enhancing the storage performance of NH_(4)^(+).To further improve the chemical reaction kinetics and address the limited cycle stability of CuO,a compositematerial composed of CuO and carbon(CuO/C)is developed.The findings demonstrate that CuO/C exhibits superior rate capability,with an initial discharge-specific capacity reaching 1851 mAh g^(-1)(0.1 A g^(-1))and improved reversible cycle performance(113 mAh g^(-1)after 400cycles).This study investigates the application of CuO as the cathode material in AAIBs and presents new opportunities for future industrial development.
基金financial support from the National Natural Science Foundation of China (52272261 and 52104300)。
文摘To tackle energy crisis and achieve sustainable development, aqueous rechargeable zinc ion batteries have gained widespread attention in large-scale energy storage for their low cost, high safety, high theoretical capacity, and environmental compatibility in recent years. However, zinc anode in aqueous zinc ion batteries is still facing several challenges such as dendrite growth and side reactions(e.g., hydrogen evolution), which cause poor reversibility and the failure of batteries. To address these issues, interfacial modification of Zn anodes has received great attention by tuning the interaction between the anode and the electrolyte. Herein, we present recent advances in the interfacial modification of zinc anode in this review. Besides, the challenges of reported approaches of interfacial modification are also discussed.Finally, we provide an outlook for the exploration of novel zinc anode for aqueous zinc ion batteries.We hope that this review will be helpful in designing and fabricating dendrite-free and hydrogenevolution-free Zn anodes and promoting the practical application of aqueous rechargeable zinc ion batteries.
基金supported by the National Natural Science Foundation of China(Grant No.51974368)the Fundamental Research Funds for the Central Universities of Central South University(2019zzts251)。
文摘Ni-rich cathodes exhibit appealing properties,such as high capacity density,low cost,and prominent energy density.However,the inferior ionic conductivity and bulk structural degradation become bottlenecks for Ni-rich cathodes and severely limit their commercial utilization.Traditional coating and doping methods suffer fatal drawbacks in functioning as a unit and cannot radically promote material performance to meet the needs of Li-ion batteries(LIBs).Herein,we successfully devised an ingenious and facile synthetic method to establish Ni-rich oxides with a La_(2)Zr_(2)O_(7) coating and Zr doping.The coating layer improves the ion diffusion kinetics and enhances Li-ion transportation while Zr doping effectively suppresses the phase transition of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode.Owing to the synergetic effect of Zr doping and La_(2)Zr_(2)O_(7) coating,the modified material shows prominent initial discharge capacity of 184.7 m Ah g^(-1) at 5℃ and maintains 177.5 m Ah g^(-1) after 100 cycles at 1℃.Overall,the proposed feasible electrode design method can have a far-reaching impact on further fabrication of advanced cathodes for high-performance LIBs.
基金financially supported by the National Natural Science Foundation of China(No.51974368)supported by the Beamlines MCD-A and MCD-B(Soochow Beamline for Energy Materials)at NSRL。
文摘The synthesis of layered oxide cathode materials by the traditional high-temperature ceramic method usually requires calcination and annealing at temperatures in the range of 700-1000℃,with high energy consumption and serious cation mixing problems.Herein,we present a novel hydrothermalLi^(+)/H^(+)exchange method for the preparation of layered oxide cathodes at temperatures as low as 200℃.In contrast to the widely reported Li^(+)/Na^(+)exchange method using sodium-containing:precursors,layered oxide cathodes can be directly synthesized by hydrothermal reaction between commercial hydroxide precursors and LiOH·H2O.The reaction pathway consists of two steps.(1)The hydroxyl oxide intermediate is obtained by oxidizing the hydroxide precursor.(2)The layered oxide product is obtained by theLi^(+)/H^(+)exchange reaction of the hydroxyl oxide with Li+in solution.Through studying the time-resolved structural evolution,we reveal that the mechanism of material formation duringLi^(+)/H^(+)ion exchange is in situ crystallization,and the ion exchange process is accompanied by lattice distortion caused by internal diffusion of ions.These findings not only provide valuable insights into theLi^(+)/H^(+)exchange process,but also provide a new paradigm for the lowtemperature synthesis of advanced cathode materials.
基金This work was supported by the National Natural Science Foundation of China(Grant No.51974368)This work was supported in part by the High Performance Computing Center of Central South UniversityThis work was supported by the Beamlines 1W1B-XAFS at BSRF.
文摘Ion exchange is a promising synthetic method for alleviating severe cation mixing in traditional layered oxide materials for lithium-ion batteries,leading to enhanced structural stability.However,the underlying mechanisms of ion exchange are still not fully understood.Such a fundamental study of the ion-exchange mechanism is needed for achieving the controllable synthesis of layered oxides with a stable structure.Herein,we thoroughly unearth the underlying mechanism that triggers the ion exchange of Ni-rich materials in aqueous solutions by examining time-resolved structural evolution combined with theoretical calculations.Our results reveal that the reaction pathway of ion exchange can be divided into two steps:protonation and lithiation.The proton is the key to achieving charge balance in the ion exchange process,as revealed by X-ray adsorption spectroscopy and inductive coupled plasma analysis.In addition,the intermediate product shows high lattice distortion during ion exchange,but it ends up with a most stable product with high lattice energy.Such apparent discrepancies in lattice energy between materials before and after ion exchange emphasize the importance of synthetic design in structural stability.This work provides new insights into the ion-exchange synthesis of Ni-rich oxide materials,which advances the development of cathode materials for high-performance lithium-ion batteries.
基金the National Natural Science Foundation of China(Grant Nos.51974368 and 51774333).
文摘Lithium-ion batteries(LIBs)represent the most promising choice for meeting the ever-growing demand of society for various electric applications,such as electric transportation,portable electronics,and grid storage.Nickel-rich layered oxides have largely replaced LiCoO_(2)in commercial batteries because of their low cost,high energy density,and good reliability.Traditional nickel-based oxide particles,usually called polycrystal materials,are composed of microsized primary particles.However,polycrystal particles tend to suffer from pulverization and severe side reactions along grain boundaries during cycling.These phenomena accelerate cell degradation.Single-crystal materials,which exhibit robust mechanical strength and a high surface area,have great potential to address the challenges that hinder their polycrystal counterparts.A comprehensive understanding of the growing body of research related to single-crystal materials is imperative to improve the performance of cathodes in LIBs.This review highlights origins,recent developments,challenges,and opportunities for single-crystal layered oxide cathodes.The synthesis science behind single-crystal materials and comparative studies between single-crystal and polycrystal materials are discussed in detail.Industrial techniques and facilities are also reviewed in combination with our group’s experiences in single-crystal research.Future development should focus on facile production with strong control of the particle size and distribution,structural defects,and impurities to fully reap the benefits of single-crystal materials.
