Rechargeable lithium-oxygen(Li-O2)batteries have appeal to enormous attention because they demonstrate higher energy density than the state-of-the-art Li-ion batteries.Whereas,their practical application is impeded by...Rechargeable lithium-oxygen(Li-O2)batteries have appeal to enormous attention because they demonstrate higher energy density than the state-of-the-art Li-ion batteries.Whereas,their practical application is impeded by several challenging problems,such as the low energy round trip efficiencies and the insufficient cycle life,due to the cathode passivation caused by the accumulation of discharge products.Developing efficient catalyst for oxygen reduction and evolution reactions is effective to reduce the overpotentials in Li-O2cells.In our work,we report a Co3O4modified Ag/g-C3N4nanocomposite as a bifunctional cathode catalyst for Li-O2cells.The g-C3N4substrate prevents the accumulation of Ag and Co3O4nanoparticles and the presence of Ag NPs improves the surface area of g-C3N4and electronic conductivity,significantly improving the oxygen reduction/evolution capabilities of Co3O4.Due to a synergetic effect,the Ag/g-C3N4/Co3O4nanocomposite demonstrates a higher catalytic activity than each individual constituent of Co3O4or Ag/g-C3N4for the ORR/OER on as catalysts in Li-O2cells.As a result,the Ag/gC3N4/Co3O4composite shows impressive electrochemical performance in a Li-O2battery,including high discharge capacity,small gap between charge and discharge potential,and high cycling stability.展开更多
Solid-state electrolytes are critical for the development of next-generation high-energy and high-safety rechargeable batteries.Among all the candidates,sodium(Na)superionic conductors(NASICONs)are highly promising be...Solid-state electrolytes are critical for the development of next-generation high-energy and high-safety rechargeable batteries.Among all the candidates,sodium(Na)superionic conductors(NASICONs)are highly promising because of their evident advantages in high ionic conductivity and high chemical/electrochemical stability.The concept of NASICONs was proposed by Hong and Goodenough et al.in 1976 by reporting the synthesis and characterization of Na1+xZr2(SixP3−x)O12(0≤x≤3),which has attracted tremendous attention on the NASICONs-type solid-state electrolytes.In this review,we are committed to describing the development history of NASICONs-type solid-state electrolytes and elucidating the contribution of Goodenough as a tribute to him.We summarize the correlations and differences between lithium-based and sodium-based NASICONs electrolytes,such as their preparation methods,structures,ionic conductivities,and the mechanisms of ion transportation.Critical challenges of NASICONs-structured electrolytes are discussed,and several research directions are proposed to tackle the obstacles toward practical applications.展开更多
According to the reports of"Top Ten Emerging Technologies in Chemistry 2022"released by the International Union of Pure and Applied Chemistry,sodium-ion battery(SIB)technology is identified as a crucial emer...According to the reports of"Top Ten Emerging Technologies in Chemistry 2022"released by the International Union of Pure and Applied Chemistry,sodium-ion battery(SIB)technology is identified as a crucial emerging technology,indicating its promising development for future energy-storage applications[1].In practical applications,commercialized lithium-ion batteries(LIBs)with lithium cobalt oxide and ternary oxide as cathode materials have assumed a dominant position[2].However,these cathode materials of LIBs are highly dependent on expensive cobalt and nickel,rendering them less sustainable for grid-scale energy storage.Conversely,cathode materials in SIBs appear more sustainable due to their lower dependence on cobalt.Furthermore,the strategic importance of reducing over-dependence on lithium resources cannot be overstated.Hence,SIB technology can serve as one of the potential solutions to mitigate this issue[3].展开更多
Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challen...Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challenged by its low conductivity and drastic volume variation during the Li uptake/release process. Tremendous efforts have been made on shrinking the particle size of Si into nanoscale so that the volume variation could be accommodated. However, the bare nano-Si material would still pulverize upon (de)lithiation. Moreover, it shows an excessive surface area to invite unlimited growth of solid electrolyte interface that hinders the transportation of charge carriers, and an increased interparticle resistance. As a result, the Si nanoparticles gradually lose their electrical contact during the cycling process, which accounts for poor thermodynamic stability and sluggish kinetics of the anode reaction versus Li. To address these problems and improve the Li storage performance of nano-Si anode, proper structural design should be applied on the Si anode. In this perspective, we will briefly review some strategies for improving the electrochemistry versus Li of nano-Si materials and their derivatives, and show opinions on the optimal design of nanostructured Si anode for advanced LIBs.展开更多
The development of new sodium ion battery （SIB） cathodes with satisfactory performance requires an in-depth understanding of their structure-function relationships, to rationally design better electrode materials. I...The development of new sodium ion battery （SIB） cathodes with satisfactory performance requires an in-depth understanding of their structure-function relationships, to rationally design better electrode materials. In this work highly ordered, honeycomb-layered Na3Ni2SbO6 was prepared to elucidate the structural evolution and Na~ kinetics during electrochemical desodiation/sodiation processes. Structural analysis involving in situ synchrotron X-ray diffraction （XRD） experiments, electrochemical performance measurements, and electrochemical characterization （galvanostatic intermittent titration technique, GITT） methods were used to obtain new insights into the reaction mechanism controlling the （de）intercalation of sodium into the host NaB-xNi2SbO6 structure. Two phase transitions occur （initial O＇3 phase → intermediate P＇3 phase→final O1 phase） upon Na^＋ extraction; the partial irreversible O＇3-P＇3 phase transition is responsible for the insufficient cycling stability. The fast Na^＋ mobility （average 10^-12 cm^2·s^-1） in the interlayer, high equilibrium voltage （3.27 V）, and low voltage polarization （50 mV） establish the linkage between kinetic advantage and a good rate performance of the cathode. These new findings provide deep insight into the reaction mechanism operating in the honeycomb cathode; the present approach could be also extended to investigate other materials for SIBs.展开更多
Rechargeable batteries based on solid-state electrolytes are of great interest and importance for the next-generation energy storage due to their high energy output and improved safety.For building the solid-state bat...Rechargeable batteries based on solid-state electrolytes are of great interest and importance for the next-generation energy storage due to their high energy output and improved safety.For building the solid-state batteries,Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)represents a promising candidate as it features high chemical stability against air exposure and a high Na^(+)conductivity.NZSP pellets were usually calcined at a high temperature,and the high volatility of Na and P elements easily led to the formation of impurity phase.In this work,the effects of calcination temperature and stoichiometry on the phase purity and ionic conductivity of the NZSP electrolyte were studied.At an elevated sintering temperature,the NZSP electrolyte showed a high ionic conductivity owing to decreased porosity,and the highest ionic conductivity at 30℃was observed to be 2.75×10^(-5)S·cm^(-1)with an activation energy of 0.41 eV.For the stoichiometry,the introduction of 5 mol%excessive P results in formation of more Na_(3)PO_(4) and glass-like phase at the grain boundary,which caused the blurred grain boundary and reduced grain barrier,and effectively suppressed Na dendrite growth,then accounted for improved cycling performance of a Na‖Na symmetric cell.Our work provided insights on reasonable design and preparation of NZSP electrolyte towards practical realization of solid-state Na-metal batteries.展开更多
As we know,Prof John B.Goodenough discovered almost all the commercial cathode materials,LiCoO_(2),LiMn_(2)O_(4),and LiFePO_(4),for lithium-ion batteries(LIBs).Nowadays,LIBs have been extensively used in our daily lif...As we know,Prof John B.Goodenough discovered almost all the commercial cathode materials,LiCoO_(2),LiMn_(2)O_(4),and LiFePO_(4),for lithium-ion batteries(LIBs).Nowadays,LIBs have been extensively used in our daily life,which provide power for mobile phones,laptop computers,electric vehicles,energy storage systems,and so forth.The discovery of LIBs is believed as one of the most important inventions in the 20th century.Expectedly,he won the Nobel prize in chemistry in 2019 together with M.Stanley Whittingham and Akira Yoshino.Their pioneering contributions have created a rechargeable world for our modern society.展开更多
基金the financial support from National Natural Science Foundation of China(Grant no.51472070,51872071)China Postdoctoral Science Foundation(Grant no.172731)。
文摘Rechargeable lithium-oxygen(Li-O2)batteries have appeal to enormous attention because they demonstrate higher energy density than the state-of-the-art Li-ion batteries.Whereas,their practical application is impeded by several challenging problems,such as the low energy round trip efficiencies and the insufficient cycle life,due to the cathode passivation caused by the accumulation of discharge products.Developing efficient catalyst for oxygen reduction and evolution reactions is effective to reduce the overpotentials in Li-O2cells.In our work,we report a Co3O4modified Ag/g-C3N4nanocomposite as a bifunctional cathode catalyst for Li-O2cells.The g-C3N4substrate prevents the accumulation of Ag and Co3O4nanoparticles and the presence of Ag NPs improves the surface area of g-C3N4and electronic conductivity,significantly improving the oxygen reduction/evolution capabilities of Co3O4.Due to a synergetic effect,the Ag/g-C3N4/Co3O4nanocomposite demonstrates a higher catalytic activity than each individual constituent of Co3O4or Ag/g-C3N4for the ORR/OER on as catalysts in Li-O2cells.As a result,the Ag/gC3N4/Co3O4composite shows impressive electrochemical performance in a Li-O2battery,including high discharge capacity,small gap between charge and discharge potential,and high cycling stability.
基金National Key Research and Development Program of China,Grant/Award Number:2020YFA0715000National Natural Science Foundation of China,Grant/Award Numbers:51902238,52127816,52172234Fundamental Research Funds for the Central Universities,Grant/Award Numbers:WUT:2020IVA069,2020IVB043,2021IVA020B。
文摘Solid-state electrolytes are critical for the development of next-generation high-energy and high-safety rechargeable batteries.Among all the candidates,sodium(Na)superionic conductors(NASICONs)are highly promising because of their evident advantages in high ionic conductivity and high chemical/electrochemical stability.The concept of NASICONs was proposed by Hong and Goodenough et al.in 1976 by reporting the synthesis and characterization of Na1+xZr2(SixP3−x)O12(0≤x≤3),which has attracted tremendous attention on the NASICONs-type solid-state electrolytes.In this review,we are committed to describing the development history of NASICONs-type solid-state electrolytes and elucidating the contribution of Goodenough as a tribute to him.We summarize the correlations and differences between lithium-based and sodium-based NASICONs electrolytes,such as their preparation methods,structures,ionic conductivities,and the mechanisms of ion transportation.Critical challenges of NASICONs-structured electrolytes are discussed,and several research directions are proposed to tackle the obstacles toward practical applications.
基金supported by the National Key R&D Program of China(2023YFE0202000)the National Natural Science Foundation of China(52173246)Double-Thousand Talents Plan of Jiangxi Province(jxsq2023102005)。
文摘According to the reports of"Top Ten Emerging Technologies in Chemistry 2022"released by the International Union of Pure and Applied Chemistry,sodium-ion battery(SIB)technology is identified as a crucial emerging technology,indicating its promising development for future energy-storage applications[1].In practical applications,commercialized lithium-ion batteries(LIBs)with lithium cobalt oxide and ternary oxide as cathode materials have assumed a dominant position[2].However,these cathode materials of LIBs are highly dependent on expensive cobalt and nickel,rendering them less sustainable for grid-scale energy storage.Conversely,cathode materials in SIBs appear more sustainable due to their lower dependence on cobalt.Furthermore,the strategic importance of reducing over-dependence on lithium resources cannot be overstated.Hence,SIB technology can serve as one of the potential solutions to mitigate this issue[3].
基金the financial support of this work by the National Natural Science Foundation of China (No.21773078)the Fundamental Research Funds for the Central Universities of China (Nos.2662015PY163 and 2662017JC025).
文摘Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challenged by its low conductivity and drastic volume variation during the Li uptake/release process. Tremendous efforts have been made on shrinking the particle size of Si into nanoscale so that the volume variation could be accommodated. However, the bare nano-Si material would still pulverize upon (de)lithiation. Moreover, it shows an excessive surface area to invite unlimited growth of solid electrolyte interface that hinders the transportation of charge carriers, and an increased interparticle resistance. As a result, the Si nanoparticles gradually lose their electrical contact during the cycling process, which accounts for poor thermodynamic stability and sluggish kinetics of the anode reaction versus Li. To address these problems and improve the Li storage performance of nano-Si anode, proper structural design should be applied on the Si anode. In this perspective, we will briefly review some strategies for improving the electrochemistry versus Li of nano-Si materials and their derivatives, and show opinions on the optimal design of nanostructured Si anode for advanced LIBs.
文摘The development of new sodium ion battery （SIB） cathodes with satisfactory performance requires an in-depth understanding of their structure-function relationships, to rationally design better electrode materials. In this work highly ordered, honeycomb-layered Na3Ni2SbO6 was prepared to elucidate the structural evolution and Na~ kinetics during electrochemical desodiation/sodiation processes. Structural analysis involving in situ synchrotron X-ray diffraction （XRD） experiments, electrochemical performance measurements, and electrochemical characterization （galvanostatic intermittent titration technique, GITT） methods were used to obtain new insights into the reaction mechanism controlling the （de）intercalation of sodium into the host NaB-xNi2SbO6 structure. Two phase transitions occur （initial O＇3 phase → intermediate P＇3 phase→final O1 phase） upon Na^＋ extraction; the partial irreversible O＇3-P＇3 phase transition is responsible for the insufficient cycling stability. The fast Na^＋ mobility （average 10^-12 cm^2·s^-1） in the interlayer, high equilibrium voltage （3.27 V）, and low voltage polarization （50 mV） establish the linkage between kinetic advantage and a good rate performance of the cathode. These new findings provide deep insight into the reaction mechanism operating in the honeycomb cathode; the present approach could be also extended to investigate other materials for SIBs.
基金financially supported by the National Natural Science Foundation of China(Nos.51902238 and 52172234)the Fundamental Research Funds for the Central Universities(Nos.2020IVA069,2020IVB043 and 2021IVA020B)
文摘Rechargeable batteries based on solid-state electrolytes are of great interest and importance for the next-generation energy storage due to their high energy output and improved safety.For building the solid-state batteries,Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)represents a promising candidate as it features high chemical stability against air exposure and a high Na^(+)conductivity.NZSP pellets were usually calcined at a high temperature,and the high volatility of Na and P elements easily led to the formation of impurity phase.In this work,the effects of calcination temperature and stoichiometry on the phase purity and ionic conductivity of the NZSP electrolyte were studied.At an elevated sintering temperature,the NZSP electrolyte showed a high ionic conductivity owing to decreased porosity,and the highest ionic conductivity at 30℃was observed to be 2.75×10^(-5)S·cm^(-1)with an activation energy of 0.41 eV.For the stoichiometry,the introduction of 5 mol%excessive P results in formation of more Na_(3)PO_(4) and glass-like phase at the grain boundary,which caused the blurred grain boundary and reduced grain barrier,and effectively suppressed Na dendrite growth,then accounted for improved cycling performance of a Na‖Na symmetric cell.Our work provided insights on reasonable design and preparation of NZSP electrolyte towards practical realization of solid-state Na-metal batteries.
文摘As we know,Prof John B.Goodenough discovered almost all the commercial cathode materials,LiCoO_(2),LiMn_(2)O_(4),and LiFePO_(4),for lithium-ion batteries(LIBs).Nowadays,LIBs have been extensively used in our daily life,which provide power for mobile phones,laptop computers,electric vehicles,energy storage systems,and so forth.The discovery of LIBs is believed as one of the most important inventions in the 20th century.Expectedly,he won the Nobel prize in chemistry in 2019 together with M.Stanley Whittingham and Akira Yoshino.Their pioneering contributions have created a rechargeable world for our modern society.
