Electron beam curing is demonstrated as a promising method for high speed,low cost and environmentally friendly battery electrode manufacturing.This work reports transfer of this process to pilot scale equipment and e...Electron beam curing is demonstrated as a promising method for high speed,low cost and environmentally friendly battery electrode manufacturing.This work reports transfer of this process to pilot scale equipment and evaluation of electrochemical performance in prototype 1.5 Ah pouch cells.Thick LiNi0.5Mn0.3Co0.2O2(NMC532)composite electrodes with an areal loading of 25 mg cm^-2(~4 mAh cm^-2)are successfully cured at a line speed of 500 feet per minute at 275 keV.Compared to the NMC532 cathode processed via a conventional coating method,the electron beam cured electrodes show higher capacity fade in the first 100 cycles,but similar fade rate afterwards.Further improvement strategies are proposed and discussed.This work demonstrates that electron beam curing is a promising method for manufacturing thick battery electrodes at high speeds and low capital/operation cost.展开更多
Design and development of novel electrode materials is one of several hot topics in studying Li ion battery. The CALPHAD(CALculation of PHAse Diagrams) approach enables calculation of stable and metastable phase equil...Design and development of novel electrode materials is one of several hot topics in studying Li ion battery. The CALPHAD(CALculation of PHAse Diagrams) approach enables calculation of stable and metastable phase equilibria,as well as thermodynamic properties for various materials,w hich has been applied to accelerate modern materials design in recent years. The traditional trial-and-error method is being replaced by the integration of CALPHAD with first-principles calculations,as well as empirical methods and key experiments. The CALPHAD approach and first-principles calculations have been proved to be a powerful tool in studying electrode materials, not only for calculation of phase equilibria and thermodynamic properties,but also for prediction of cell voltages in Li ion batteries,which allows for the design of future electrode materials with improved stability and efficiency. Examples of the cathode systems(Li-O,Li-Co-O and Li-Ni-O) and anode systems(Li-Sb and Li-Sn),which are studied by applying the CALPHAD approach and first-principles calculations,are presented.展开更多
Lithium–sulfur batteries are one of the attractive next-generation energy storage systems owing to theienvironmental friendliness,low cost,and high specific energy densities.However,the low electrical conductivity of...Lithium–sulfur batteries are one of the attractive next-generation energy storage systems owing to theienvironmental friendliness,low cost,and high specific energy densities.However,the low electrical conductivity of sulfur,shuttling of soluble intermediate polysulfides between electrodes,and low capacitretention have hampered their commercial use.To address these issues,we use a halloysitemodulated(H-M)separator in a lithium–sulfur battery to mitigate the shuttling problem.The H-M separator acts as a mutual Coulombic repulsion in lithium-sulfur batteries,thereby selectively permitting Lions and efficiently suppressing the transfer of undesired lithium polysulfides to the Li anode sideMoreover,the use of halloysite switches the surface of the separator from hydrophobic to hydrophilicconsequently improving the electrolyte wettability and adhesion between the separator and cathodeWhen sulfur-multi-walled carbon nanotube(S-MWCNT)composites are used as cathode active materialsa lithium–sulfur battery with an H-M separator exhibits first discharge and charge capacities of 1587 an1527 m Ah g-1,respectively.Moreover,there is a consistent capacity retention up to 100 cyclesAccordingly,our approach demonstrates an economical and easily accessible strategy for commercialization of lithium–sulfur batteries.展开更多
Progress in the research on phase transitions during Li＋ extraction/insertion processes in typical battery materials is summarized as examples to illustrate the significance of understanding phase transition phenomen...Progress in the research on phase transitions during Li＋ extraction/insertion processes in typical battery materials is summarized as examples to illustrate the significance of understanding phase transition phenomena in Li-ion batteries. Physical phenomena such as phase transitions （and resultant phase diagrams） are often observed in Li-ion battery research and already play an important role in promoting Li-ion battery technology. For example, the phase transitions during Li＋ insertion/extraction are highly relevant to the thermodynamics and kinetics of Li-ion batteries, and even physical characteristics such as specific energy, power density, volume variation, and safety-related properties.展开更多
Mechanical degradation, especially fractures in active particles in an electrode, is a major reason why the capacity of lithiumion batteries fades. This paper proposes a model that couples Li-ion diffusion, stress evo...Mechanical degradation, especially fractures in active particles in an electrode, is a major reason why the capacity of lithiumion batteries fades. This paper proposes a model that couples Li-ion diffusion, stress evolution, and damage mechanics to simulate the growth of central cracks in cathode particles（Li Mn_2 O_4） by an extended finite element method by considering the influence of multiple factors. The simulation shows that particles are likely to crack at a high discharge rate, when the particle radius is large, or when the initial central crack is longer. It also shows that the maximum principal tensile stress decreases and cracking becomes more difficult when the influence of crack surface diffusion is considered. The fracturing process occurs according to the following stages： no crack growth, stable crack growth, and unstable crack growth. Changing the charge/discharge strategy before unstable crack growth sets in is beneficial to prevent further capacity fading during electrochemical cycling.展开更多
Construction of a thickness‐independent electrode with high active material mass loading is crucial for the development of high energy rechargeable lithium battery.Herein,we fabricate an all‐in‐one integrated SnS2@...Construction of a thickness‐independent electrode with high active material mass loading is crucial for the development of high energy rechargeable lithium battery.Herein,we fabricate an all‐in‐one integrated SnS2@3D multichannel carbon matrix(SnS2@3DMCM)electrode with in‐situ growth of ultrathin SnS2 nanosheets inside the inner walls of three dimensional(3D)multichannels.The interconnected conductive carbon matrix derived from natural wood acts as an integrated porous current collector to avail the electrons transport and accommodate massive SnS2 nanosheets,while plenty of 3D aligned multichannels facilitate fast ions transport with electrode thickness‐independent even under high mass loading.As expected,the integrated SnS2@3DMCM electrode exhibits remarkable electrochemical lithium storage performance,such as exceptional high‐areal‐capacity of 6.4 mAh cm−2,high rate capability of 3 mAh cm−2 under current of 6.8 mAcm−2(10 C),and stable cycling performance of 6.8 mAcm−2 with a high mass loading of 7mg cm−2.The 3D integrated porous electrode constructing conveniently with the natural source paves new avenues towards future high‐performance lithium batteries.展开更多
Nanostructured organic tetralithium salts of 2,5-dihydroxyterephthalic acid （Li4C8H2O6） supported on graphene were prepared via a facile recrystallization method. The optimized composite with 75 wt.% Li4C8H2O6 was e...Nanostructured organic tetralithium salts of 2,5-dihydroxyterephthalic acid （Li4C8H2O6） supported on graphene were prepared via a facile recrystallization method. The optimized composite with 75 wt.% Li4C8H2O6 was evaluated as an anode with redox couples of Li4C8H2O6/Li6C8H2O6 and as a cathode with redox couples of Li4C8H2O6/Li2C8H2O6 for Li-ion batteries, exhibiting a high-rate capability （10 C） and long cycling life （1,000 cycles）. Moreover, in an all-organic symmetric Li-ion battery, this dual-function electrode retained capacities of 191 and 121 mA.h·g-1 after 100 and 500 cycles, respectively. Density functional theory calculations indicated the presence of covalent bonds between Li4CsH206 and graphene, which affected both the morphology and electronic structure of the composite. The special nanostructures, high electronic conductivity of graphene, and covalent-bond interaction between Li4C8H2O6 and graphene contributed to the superior electrochemical properties. Our results indicate that the combination of organic salt molecules with graphene is useful for obtaining high-performance organic batteries.展开更多
A novel lightweight three-dimensional （3D） composite anode for a fast-charging] discharging Li-ion battery （LIB） was fabricated entirely using one-dimensional （1D） nanomaterials, i.e., Cu nanowires （CuNWs） and...A novel lightweight three-dimensional （3D） composite anode for a fast-charging] discharging Li-ion battery （LIB） was fabricated entirely using one-dimensional （1D） nanomaterials, i.e., Cu nanowires （CuNWs） and multi-walled C nanotubes （MWCNTs）. Because of the excellent electrical conductivity, high-aspect ratio structures, and large surface areas of these nanomaterials, the CuNW-MWCNT composite （CNMC） with 3D structure provides significant advantages regarding the transport pathways for both electrons and ions. As an advanced binder-free anode, a CuNW-MWCNT composite film with a controllable thickness （~ 600 prn） exhibited a considerably low sheet resistance, and internal cell resistance. Furthermore, the random CuNW network with 3D structure acting as a rigid framework not only prevented MWCNT shrinkage and expansion due to aggregation and swelling but also minimized the effect of the volume change during the charge/discharge process. Both a half cell and a full cell of LIBs with the CNMC anode exhibited high specific capacities and Coulombic efficiendes, even at a high current. More importantly, we for the first time overcame the limitation of MWCNTs as anode materials for fast-charging]discharging LIBs （both half cells and full cells） by employing CuNWs, and the resulting anode can be applied to flexible LIBs. This innovative anode structure can lead to the development of ultrafast chargeable LIBs for electric vehides.展开更多
基金sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies Office (VTO) (Deputy Director: David Howell) Applied Battery Research subprogram (Program Manager: Peter Faguy)
文摘Electron beam curing is demonstrated as a promising method for high speed,low cost and environmentally friendly battery electrode manufacturing.This work reports transfer of this process to pilot scale equipment and evaluation of electrochemical performance in prototype 1.5 Ah pouch cells.Thick LiNi0.5Mn0.3Co0.2O2(NMC532)composite electrodes with an areal loading of 25 mg cm^-2(~4 mAh cm^-2)are successfully cured at a line speed of 500 feet per minute at 275 keV.Compared to the NMC532 cathode processed via a conventional coating method,the electron beam cured electrodes show higher capacity fade in the first 100 cycles,but similar fade rate afterwards.Further improvement strategies are proposed and discussed.This work demonstrates that electron beam curing is a promising method for manufacturing thick battery electrodes at high speeds and low capital/operation cost.
基金Sponsored by the National Natural Science Foundation of China(Grant Nos.51531009 and 51671219)Natural Science Foundation of Hunan Province(Grant No.2017JJ3409)the Deutsche Forschungsgemeinschaft(DFG)CH-1688/1-1 and Nachwuchsakademie Program
文摘Design and development of novel electrode materials is one of several hot topics in studying Li ion battery. The CALPHAD(CALculation of PHAse Diagrams) approach enables calculation of stable and metastable phase equilibria,as well as thermodynamic properties for various materials,w hich has been applied to accelerate modern materials design in recent years. The traditional trial-and-error method is being replaced by the integration of CALPHAD with first-principles calculations,as well as empirical methods and key experiments. The CALPHAD approach and first-principles calculations have been proved to be a powerful tool in studying electrode materials, not only for calculation of phase equilibria and thermodynamic properties,but also for prediction of cell voltages in Li ion batteries,which allows for the design of future electrode materials with improved stability and efficiency. Examples of the cathode systems(Li-O,Li-Co-O and Li-Ni-O) and anode systems(Li-Sb and Li-Sn),which are studied by applying the CALPHAD approach and first-principles calculations,are presented.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIP)(No.2018R1C1B6004689)the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(No.2020R1I1A306182111)the Electronics and Telecommunications Research Institute(ETRI)grant funded by the Korean government(21ZB1200,Development of ICT Materials,Components and Equipment Technologies)。
文摘Lithium–sulfur batteries are one of the attractive next-generation energy storage systems owing to theienvironmental friendliness,low cost,and high specific energy densities.However,the low electrical conductivity of sulfur,shuttling of soluble intermediate polysulfides between electrodes,and low capacitretention have hampered their commercial use.To address these issues,we use a halloysitemodulated(H-M)separator in a lithium–sulfur battery to mitigate the shuttling problem.The H-M separator acts as a mutual Coulombic repulsion in lithium-sulfur batteries,thereby selectively permitting Lions and efficiently suppressing the transfer of undesired lithium polysulfides to the Li anode sideMoreover,the use of halloysite switches the surface of the separator from hydrophobic to hydrophilicconsequently improving the electrolyte wettability and adhesion between the separator and cathodeWhen sulfur-multi-walled carbon nanotube(S-MWCNT)composites are used as cathode active materialsa lithium–sulfur battery with an H-M separator exhibits first discharge and charge capacities of 1587 an1527 m Ah g-1,respectively.Moreover,there is a consistent capacity retention up to 100 cyclesAccordingly,our approach demonstrates an economical and easily accessible strategy for commercialization of lithium–sulfur batteries.
基金supported by the National High Technology Research and Development Program of China(Grant No.2013AA050906)the National Natural Science Foundation of China(Grant Nos.51272175 and 21301127)
文摘Progress in the research on phase transitions during Li＋ extraction/insertion processes in typical battery materials is summarized as examples to illustrate the significance of understanding phase transition phenomena in Li-ion batteries. Physical phenomena such as phase transitions （and resultant phase diagrams） are often observed in Li-ion battery research and already play an important role in promoting Li-ion battery technology. For example, the phase transitions during Li＋ insertion/extraction are highly relevant to the thermodynamics and kinetics of Li-ion batteries, and even physical characteristics such as specific energy, power density, volume variation, and safety-related properties.
基金support of the National Natural Science Foundation of China (11472165 and 11332005)
文摘Mechanical degradation, especially fractures in active particles in an electrode, is a major reason why the capacity of lithiumion batteries fades. This paper proposes a model that couples Li-ion diffusion, stress evolution, and damage mechanics to simulate the growth of central cracks in cathode particles（Li Mn_2 O_4） by an extended finite element method by considering the influence of multiple factors. The simulation shows that particles are likely to crack at a high discharge rate, when the particle radius is large, or when the initial central crack is longer. It also shows that the maximum principal tensile stress decreases and cracking becomes more difficult when the influence of crack surface diffusion is considered. The fracturing process occurs according to the following stages： no crack growth, stable crack growth, and unstable crack growth. Changing the charge/discharge strategy before unstable crack growth sets in is beneficial to prevent further capacity fading during electrochemical cycling.
基金Innovation Program of Shanghai Municipal Education Commission,Grant/Award Number:2019‐01‐07‐00‐07‐E00015National Natural Science Foundation of China,Grant/Award Numbers:21875141,51671135,51971146+4 种基金Support of young teachers in Shanghai colleges and universities,Grant/Award Number:ZZslg18039Shanghai Outstanding Academic Leaders PlanProgram of Shanghai Subject Chief Scientist,Grant/Award Number:17XD1403000Shanghai Pujiang Program,Grant/Award Number:18PJ1409000Opening Project of State Key Laboratory of Advanced Chemical Power Sources,Grant/Award Number:SKL‐ACPS‐C‐23。
文摘Construction of a thickness‐independent electrode with high active material mass loading is crucial for the development of high energy rechargeable lithium battery.Herein,we fabricate an all‐in‐one integrated SnS2@3D multichannel carbon matrix(SnS2@3DMCM)electrode with in‐situ growth of ultrathin SnS2 nanosheets inside the inner walls of three dimensional(3D)multichannels.The interconnected conductive carbon matrix derived from natural wood acts as an integrated porous current collector to avail the electrons transport and accommodate massive SnS2 nanosheets,while plenty of 3D aligned multichannels facilitate fast ions transport with electrode thickness‐independent even under high mass loading.As expected,the integrated SnS2@3DMCM electrode exhibits remarkable electrochemical lithium storage performance,such as exceptional high‐areal‐capacity of 6.4 mAh cm−2,high rate capability of 3 mAh cm−2 under current of 6.8 mAcm−2(10 C),and stable cycling performance of 6.8 mAcm−2 with a high mass loading of 7mg cm−2.The 3D integrated porous electrode constructing conveniently with the natural source paves new avenues towards future high‐performance lithium batteries.
文摘Nanostructured organic tetralithium salts of 2,5-dihydroxyterephthalic acid （Li4C8H2O6） supported on graphene were prepared via a facile recrystallization method. The optimized composite with 75 wt.% Li4C8H2O6 was evaluated as an anode with redox couples of Li4C8H2O6/Li6C8H2O6 and as a cathode with redox couples of Li4C8H2O6/Li2C8H2O6 for Li-ion batteries, exhibiting a high-rate capability （10 C） and long cycling life （1,000 cycles）. Moreover, in an all-organic symmetric Li-ion battery, this dual-function electrode retained capacities of 191 and 121 mA.h·g-1 after 100 and 500 cycles, respectively. Density functional theory calculations indicated the presence of covalent bonds between Li4CsH206 and graphene, which affected both the morphology and electronic structure of the composite. The special nanostructures, high electronic conductivity of graphene, and covalent-bond interaction between Li4C8H2O6 and graphene contributed to the superior electrochemical properties. Our results indicate that the combination of organic salt molecules with graphene is useful for obtaining high-performance organic batteries.
文摘A novel lightweight three-dimensional （3D） composite anode for a fast-charging] discharging Li-ion battery （LIB） was fabricated entirely using one-dimensional （1D） nanomaterials, i.e., Cu nanowires （CuNWs） and multi-walled C nanotubes （MWCNTs）. Because of the excellent electrical conductivity, high-aspect ratio structures, and large surface areas of these nanomaterials, the CuNW-MWCNT composite （CNMC） with 3D structure provides significant advantages regarding the transport pathways for both electrons and ions. As an advanced binder-free anode, a CuNW-MWCNT composite film with a controllable thickness （~ 600 prn） exhibited a considerably low sheet resistance, and internal cell resistance. Furthermore, the random CuNW network with 3D structure acting as a rigid framework not only prevented MWCNT shrinkage and expansion due to aggregation and swelling but also minimized the effect of the volume change during the charge/discharge process. Both a half cell and a full cell of LIBs with the CNMC anode exhibited high specific capacities and Coulombic efficiendes, even at a high current. More importantly, we for the first time overcame the limitation of MWCNTs as anode materials for fast-charging]discharging LIBs （both half cells and full cells） by employing CuNWs, and the resulting anode can be applied to flexible LIBs. This innovative anode structure can lead to the development of ultrafast chargeable LIBs for electric vehides.
