Single crystallization is an important strategy to resolve intergranular cracks and unnecessary side reactions with electrolytes in layered transition metal oxide cathodes LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811).Due t...Single crystallization is an important strategy to resolve intergranular cracks and unnecessary side reactions with electrolytes in layered transition metal oxide cathodes LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811).Due to the limitations of high-temperature sintering and multi-step calcination,single crystal NMC811 generally shows irregular particles with a size of 2-3μm.However,the prolonged Li-ion diffusion pathway and the stress generated by the uneven de-/intercalation sluggish Li-ion diffusion kinetics,what is more,cause structural damage such as intragranular cracks.A slow Li extraction rate or particle size reduction will ameliorate the structural damage and improve the cycling stability.As the most promising cathodes for next-generation power batteries,NMC811 required fast charge performance and cycle stability.Particle size reduction appears to be the displacement option.Nanonization is an effective strategy to mitigate intragranular cracks of single crystal NMC811.However,the serious aggregation and increased specific surface area become new challenges.In this article,we synthesized monodisperse nanoscale single crystal NMC811 by molten salt method and modified the surface by LiNbO3 coating.The electrochemical performance shows that nanoscale single crystal NMC811 has faster kinetic and higher capacity retention,so the strategy of combining nanonization and surface coating is an alternative way to prepare high specific capacity and cycle stable single crystal NMC811.展开更多
LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)is an attractive material for high-energy-density Li-ion batteries in electric vehicles.However,it suffers from rapid capacity fading.Previous studies have shown that tuning the ...LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)is an attractive material for high-energy-density Li-ion batteries in electric vehicles.However,it suffers from rapid capacity fading.Previous studies have shown that tuning the positive electrode material via atomic layer deposition(ALD)can enhance the electrochemical performance of the material.In this article,we introduce a novel coating method using gaseous precursors in an ALD reactor,where an AlO_(x)layer is deposited directly on the surface of the NMC811 precursor,followed by lithiation.The AlO_(x)coating is applied to the NMC811 powder substrate by exposing it to gas-phase precursors,using a conventional ALD and simplified ALD(chemical vapor deposition-like)method.It is observed that the novel methods lead to the incorporation of Al as a dopant within the bulk of NMC811,rather than forming a conformal AlO_(x)coating,after the final lithiation step.The optimized procedures result in positive electrode materials with higher capacity and enhanced cycling stability in both half-cell and full-cell configurations.Doping or coating was shown to mitigate transition metal dissolution,reduce side reactions between the active material and electrolyte,and improve structural stability.展开更多
This work made use of the Aalto University Otanano-Nanomicroscopy Center and RAMI infrastructures.Financial support from Business Finland NextGenBat[grant number 211849]is greatly acknowledged.The tomography experimen...This work made use of the Aalto University Otanano-Nanomicroscopy Center and RAMI infrastructures.Financial support from Business Finland NextGenBat[grant number 211849]is greatly acknowledged.The tomography experiment was performed at the beamline ID16B of the European Synchrotron Radiation Facility(ESRF),Grenoble,France,in the frame of proposal CH-6644.The patent titled“Stabilized Positive Electrode Material to Enable High Energy and Power Density Lithium-Ion Batteries”(IPD3173)is pertinent to this manuscript.It was filed by Zahra Ahaliabadeh and Tanja Kallio,and the patent rights are held by Aalto University.展开更多
The undesired side reactions at electrode/electrolyte interface as well as the irreversible phase evolution during electrochemical cycling significantly affect the cyclic performances of nickel-rich NMCs electrode mat...The undesired side reactions at electrode/electrolyte interface as well as the irreversible phase evolution during electrochemical cycling significantly affect the cyclic performances of nickel-rich NMCs electrode materials.Electrolyte optimization is an effective approach to suppress such an adverse side reaction,thereby enhancing the electrochemical properties.Herein,a novel boron-based film forming additive,tris(2,2,2-trifluoroethyl)borate(TTFEB),has been introduced to regulate the interphasial chemistry of LiNi0.8Mn0.1Co0.1O2(NMC811)cathode to improve its long-term cyclability and rate properties.The results of multi-model diagnostic study reveal that formation lithium fluoride(LiF)-rich and boron(B)containing cathode electrolyte interphase(CEI)not only stabilizes cathode surface,but also prevents electrolyte decomposition.Moreover,homogenously distributed B containing species serves as a skeleton to form more uniform and denser CEI,reducing the interphasial resistance.Remarkably,the Li/NMC811 cell with the TTFEB additive delivers an exceptional cycling stability with a high-capacity retention of 72.8%after 350 electrochemical cycles at a 1 C current rate,which is significantly higher than that of the cell cycled in the conventional electrolyte(59.7%).These findings provide a feasible pathway for improving the electrochemical performance of Ni-rich NMCs cathode by regulating the interphasial chemistry.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.52022088,51971245,51772262,U20A20336,21935009)Natural Science Foundation of Hebei Province(Nos.F2021203097,B2020203037)China Postdoctoral Science Foundation(No.2021M702756)。
文摘Single crystallization is an important strategy to resolve intergranular cracks and unnecessary side reactions with electrolytes in layered transition metal oxide cathodes LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811).Due to the limitations of high-temperature sintering and multi-step calcination,single crystal NMC811 generally shows irregular particles with a size of 2-3μm.However,the prolonged Li-ion diffusion pathway and the stress generated by the uneven de-/intercalation sluggish Li-ion diffusion kinetics,what is more,cause structural damage such as intragranular cracks.A slow Li extraction rate or particle size reduction will ameliorate the structural damage and improve the cycling stability.As the most promising cathodes for next-generation power batteries,NMC811 required fast charge performance and cycle stability.Particle size reduction appears to be the displacement option.Nanonization is an effective strategy to mitigate intragranular cracks of single crystal NMC811.However,the serious aggregation and increased specific surface area become new challenges.In this article,we synthesized monodisperse nanoscale single crystal NMC811 by molten salt method and modified the surface by LiNbO3 coating.The electrochemical performance shows that nanoscale single crystal NMC811 has faster kinetic and higher capacity retention,so the strategy of combining nanonization and surface coating is an alternative way to prepare high specific capacity and cycle stable single crystal NMC811.
基金the European Union,the SOLiD project(grant agreement no.101069505),for the financial support。
文摘LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)is an attractive material for high-energy-density Li-ion batteries in electric vehicles.However,it suffers from rapid capacity fading.Previous studies have shown that tuning the positive electrode material via atomic layer deposition(ALD)can enhance the electrochemical performance of the material.In this article,we introduce a novel coating method using gaseous precursors in an ALD reactor,where an AlO_(x)layer is deposited directly on the surface of the NMC811 precursor,followed by lithiation.The AlO_(x)coating is applied to the NMC811 powder substrate by exposing it to gas-phase precursors,using a conventional ALD and simplified ALD(chemical vapor deposition-like)method.It is observed that the novel methods lead to the incorporation of Al as a dopant within the bulk of NMC811,rather than forming a conformal AlO_(x)coating,after the final lithiation step.The optimized procedures result in positive electrode materials with higher capacity and enhanced cycling stability in both half-cell and full-cell configurations.Doping or coating was shown to mitigate transition metal dissolution,reduce side reactions between the active material and electrolyte,and improve structural stability.
基金Financial support from Business Finland NextGenBat[grant number 211849]is greatly acknowledged.
文摘This work made use of the Aalto University Otanano-Nanomicroscopy Center and RAMI infrastructures.Financial support from Business Finland NextGenBat[grant number 211849]is greatly acknowledged.The tomography experiment was performed at the beamline ID16B of the European Synchrotron Radiation Facility(ESRF),Grenoble,France,in the frame of proposal CH-6644.The patent titled“Stabilized Positive Electrode Material to Enable High Energy and Power Density Lithium-Ion Batteries”(IPD3173)is pertinent to this manuscript.It was filed by Zahra Ahaliabadeh and Tanja Kallio,and the patent rights are held by Aalto University.
基金supported by the National Natural Science Foundation of China(Grant No.22209106).
文摘The undesired side reactions at electrode/electrolyte interface as well as the irreversible phase evolution during electrochemical cycling significantly affect the cyclic performances of nickel-rich NMCs electrode materials.Electrolyte optimization is an effective approach to suppress such an adverse side reaction,thereby enhancing the electrochemical properties.Herein,a novel boron-based film forming additive,tris(2,2,2-trifluoroethyl)borate(TTFEB),has been introduced to regulate the interphasial chemistry of LiNi0.8Mn0.1Co0.1O2(NMC811)cathode to improve its long-term cyclability and rate properties.The results of multi-model diagnostic study reveal that formation lithium fluoride(LiF)-rich and boron(B)containing cathode electrolyte interphase(CEI)not only stabilizes cathode surface,but also prevents electrolyte decomposition.Moreover,homogenously distributed B containing species serves as a skeleton to form more uniform and denser CEI,reducing the interphasial resistance.Remarkably,the Li/NMC811 cell with the TTFEB additive delivers an exceptional cycling stability with a high-capacity retention of 72.8%after 350 electrochemical cycles at a 1 C current rate,which is significantly higher than that of the cell cycled in the conventional electrolyte(59.7%).These findings provide a feasible pathway for improving the electrochemical performance of Ni-rich NMCs cathode by regulating the interphasial chemistry.
