High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions wit...High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.展开更多
Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuin...Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuing higher energy density,of which application has been challenged due to the unstable interface caused by the non-uniform electrodeposition as well as high chemical activity.Operating at higher temperature can be recommended to uniform electrodeposition of Li metal.Nevertheless,the intrinsic side-reaction between Li metal anode and electrolyte is inevitably aggravated and thus fosters the failure of Li metal anode rapidly with uneven electrodeposition.Here,a kind of temperature-tolerated ionic liquid(1-methyl-3-ethylimidazole bis(fluorosulfo nyl)imide/lithium bis(trifluoromethylsulfo nyl)imide,EF/LT)based electrolyte that matrixed with poly(vinylidene fluoride-hexafluoropropylene) was designed to maintain the interfacial stabilization of Li metal due to the weak interfacial reaction and uniform electrodeposition at high temperature of 80℃.It is the matter that the 660-h cycle with lower polarization is achieved with EF/LT-based electrolyte at temperature of 80 ℃ and the full cell embraces outstanding cyclic performance,without capacity fading within 100 cycles.Delighting,a door for practical application of Li metal anode for higher energy density as the carbon neutrality progresses in the blooming human society has been opened gradually.展开更多
Nickel-rich LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathode material has been widely concerned due to its high voltage,high specific capacity and excellent rate performance,which is considered as one of the most promi...Nickel-rich LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathode material has been widely concerned due to its high voltage,high specific capacity and excellent rate performance,which is considered as one of the most promising cathode materials for the next generation of high-energy-density solid-state lithium batteries.However,serious electro-chemo-mechanical degradation of Nickel-rich cathode during cycling,especially at a high voltage(over 4.5 V),constrains their large-scale application.Here,using the multiphysical simulation,highly-conductive polymer matrix with spontaneous stress-buffering effect was uncovered theoretically for reinforcing the electrochemical performance of composited NCM81 1 cathode through the visualization of uniform concentration distribution of Li-ion coupled with improved stress field inside NCM811 cathode.Thereupon,polyacrylonitrile(PAN) and soft polyvinylidene fluoride(PVDF) were selected as the polymer matrix to fabricate the composited NCM811 cathode(PVDFPAN@NCM811) for improving the electrochemical performance of the solid-state NMC811|Li full cells,which can maintain high capacity over 146.2 mA h g^(-1)after 200 cycles at a high voltage of 4.5 V.Suggestively,designing a multifunctional polymer matrix with high ionic conductivity and mechanical property can buffer the stress and maintain the integrity of the structure,which can be regarded as the door-opening avenue to realize the high electrochemical performance of Ni-rich cathode for solidstate batteries.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22102212 and 22479067).
文摘High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.
基金financially supported by the Natural Science Foundation of Hunan Province(2020JJ5653)the National Natural Science Foundation of China(21875282,22102212)+1 种基金the National University of Defense Technology Scientific Research Project(ZK20-44)financial support from the Ministry of Science and Higher Education of the Russian Federation(075-15-2022-1150)。
文摘Embracing ultrahigh theoretical capacity of 3860 mA h g^(-1)and the lowest reduction potential of-3.04 V(versus standard hydrogen electrode),lithium(Li) is considered as the "holy grail" material for pursuing higher energy density,of which application has been challenged due to the unstable interface caused by the non-uniform electrodeposition as well as high chemical activity.Operating at higher temperature can be recommended to uniform electrodeposition of Li metal.Nevertheless,the intrinsic side-reaction between Li metal anode and electrolyte is inevitably aggravated and thus fosters the failure of Li metal anode rapidly with uneven electrodeposition.Here,a kind of temperature-tolerated ionic liquid(1-methyl-3-ethylimidazole bis(fluorosulfo nyl)imide/lithium bis(trifluoromethylsulfo nyl)imide,EF/LT)based electrolyte that matrixed with poly(vinylidene fluoride-hexafluoropropylene) was designed to maintain the interfacial stabilization of Li metal due to the weak interfacial reaction and uniform electrodeposition at high temperature of 80℃.It is the matter that the 660-h cycle with lower polarization is achieved with EF/LT-based electrolyte at temperature of 80 ℃ and the full cell embraces outstanding cyclic performance,without capacity fading within 100 cycles.Delighting,a door for practical application of Li metal anode for higher energy density as the carbon neutrality progresses in the blooming human society has been opened gradually.
基金financially supported by the Natural Science Foundation of Hunan Province(2020JJ5653)the National Natural Science Foundation of China(21875282,22102212)+1 种基金the Ministry of Science and Higher Education of the Russian Federation(07515-2022-1150)the National University of Defense Technology Scientific Research Project(ZK20-44)。
文摘Nickel-rich LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811) cathode material has been widely concerned due to its high voltage,high specific capacity and excellent rate performance,which is considered as one of the most promising cathode materials for the next generation of high-energy-density solid-state lithium batteries.However,serious electro-chemo-mechanical degradation of Nickel-rich cathode during cycling,especially at a high voltage(over 4.5 V),constrains their large-scale application.Here,using the multiphysical simulation,highly-conductive polymer matrix with spontaneous stress-buffering effect was uncovered theoretically for reinforcing the electrochemical performance of composited NCM81 1 cathode through the visualization of uniform concentration distribution of Li-ion coupled with improved stress field inside NCM811 cathode.Thereupon,polyacrylonitrile(PAN) and soft polyvinylidene fluoride(PVDF) were selected as the polymer matrix to fabricate the composited NCM811 cathode(PVDFPAN@NCM811) for improving the electrochemical performance of the solid-state NMC811|Li full cells,which can maintain high capacity over 146.2 mA h g^(-1)after 200 cycles at a high voltage of 4.5 V.Suggestively,designing a multifunctional polymer matrix with high ionic conductivity and mechanical property can buffer the stress and maintain the integrity of the structure,which can be regarded as the door-opening avenue to realize the high electrochemical performance of Ni-rich cathode for solidstate batteries.
