Nickel(Ni)-rich layered materials have attracted considerable interests as promising cathode materials for lithium ion batteries(LIBs)owing to their higher capacities and lower cost.Nevertheless,Mn-rich cathode materi...Nickel(Ni)-rich layered materials have attracted considerable interests as promising cathode materials for lithium ion batteries(LIBs)owing to their higher capacities and lower cost.Nevertheless,Mn-rich cathode materials usually suffer from poor cyclability caused by the unavoidable side-reactions between Ni^4+ions on the surface a nd electrolytes.The design of gradient concentration(GC)particles with Ni-rich inside and Mn-rich outside is proved to be an efficient way to address the issue.Herein,a series of LiNi0.6Co0.2Mn0.2O2(LNCM 622)materials with different GCs(the atomic ratio of Ni/Mn decreasing from the core to the outer layer)have been successfully synthesized via rationally designed co-precipitation process.Experimental results demonstrate that the GC of LNCM 622 materials plays an important role in their microstructure and electrochemical properties.The as-prepared GC3.5 cathode material with optimal GC can provide a shorter pathway for lithium-ion diffusion and stabilize the near-surface region,and finally achieve excellent electrochemical performances,delivering a discharge capacity over 176 mAh·g^-1 at 0.2 C rate and exhibiting capacity retention up to 94%after 100 cycles at 1 C.T h e rationally-designed co-precipitation process for fabricating the Ni-rich layered cathode materials with gradient composition lays a solid foundation for the preparation of high-performance cathode materials for LIBs.展开更多
High energy density lithium-ion batteries using Ni-rich cathode(such as LiNi0.6Co0.2Mn0.2O2) suffer from severe capacity decay.P-toluenesulfonyl fluoride(pTSF) has been investigated as a novel film-forming electrolyte...High energy density lithium-ion batteries using Ni-rich cathode(such as LiNi0.6Co0.2Mn0.2O2) suffer from severe capacity decay.P-toluenesulfonyl fluoride(pTSF) has been investigated as a novel film-forming electrolyte additive to enhance the cycling performances of graphite/LiNi0.6Co0.2Mn0.2O2 pouch cell.In comparison with the baseline electrolyte,a small dose of pTSF can significantly improve the cyclic stability of the cell.Theoretical calculations together with experimental results indicate that pTSF would be oxidized and reduced to construct protective interphase film on the surfaces of LiNi0.6Co0.2Mn0.2O2 cathode and graphite anode,respectively.These S-containing surface films derived from pTSF effectively mitigate the decomposition of electrolyte,reduce the interphasial impedance,as well as prevent the dissolution of transition metal ions from Ni-rich cathode upon cycling at high voltage.This finding is beneficial for the practical application of high energy density graphite/LiNi0.6Co0.2Mn0.2O2 cells.展开更多
基金the financial support of the National Natural Science Foundation of China(Grant Nos.91834301,91534102 and 21271058)Science and Technology Project of Anhui Province(Nos.201903a05020021 and 17030901067).
文摘Nickel(Ni)-rich layered materials have attracted considerable interests as promising cathode materials for lithium ion batteries(LIBs)owing to their higher capacities and lower cost.Nevertheless,Mn-rich cathode materials usually suffer from poor cyclability caused by the unavoidable side-reactions between Ni^4+ions on the surface a nd electrolytes.The design of gradient concentration(GC)particles with Ni-rich inside and Mn-rich outside is proved to be an efficient way to address the issue.Herein,a series of LiNi0.6Co0.2Mn0.2O2(LNCM 622)materials with different GCs(the atomic ratio of Ni/Mn decreasing from the core to the outer layer)have been successfully synthesized via rationally designed co-precipitation process.Experimental results demonstrate that the GC of LNCM 622 materials plays an important role in their microstructure and electrochemical properties.The as-prepared GC3.5 cathode material with optimal GC can provide a shorter pathway for lithium-ion diffusion and stabilize the near-surface region,and finally achieve excellent electrochemical performances,delivering a discharge capacity over 176 mAh·g^-1 at 0.2 C rate and exhibiting capacity retention up to 94%after 100 cycles at 1 C.T h e rationally-designed co-precipitation process for fabricating the Ni-rich layered cathode materials with gradient composition lays a solid foundation for the preparation of high-performance cathode materials for LIBs.
基金supported by the National Natural Science Foundation of China (21573080)the Guangdong Program for Support of Distinguished Young Scholar (2017B030306013)the Science and Technology Planning Project of Guangdong Province (2017B090901020)。
文摘High energy density lithium-ion batteries using Ni-rich cathode(such as LiNi0.6Co0.2Mn0.2O2) suffer from severe capacity decay.P-toluenesulfonyl fluoride(pTSF) has been investigated as a novel film-forming electrolyte additive to enhance the cycling performances of graphite/LiNi0.6Co0.2Mn0.2O2 pouch cell.In comparison with the baseline electrolyte,a small dose of pTSF can significantly improve the cyclic stability of the cell.Theoretical calculations together with experimental results indicate that pTSF would be oxidized and reduced to construct protective interphase film on the surfaces of LiNi0.6Co0.2Mn0.2O2 cathode and graphite anode,respectively.These S-containing surface films derived from pTSF effectively mitigate the decomposition of electrolyte,reduce the interphasial impedance,as well as prevent the dissolution of transition metal ions from Ni-rich cathode upon cycling at high voltage.This finding is beneficial for the practical application of high energy density graphite/LiNi0.6Co0.2Mn0.2O2 cells.