Spinel LiMn2O4 is recognized as one of the most competitive cathode candidates for lithium-ion batteries ascribed to environmentally benign and rich sources.However,the wholesale application of LiMn2O4 is predominately plagued by its severe capacity degradation,mainly associated with the innate Jahn-Teller effect.Herein,single-crystalline LiMn2O4 with Eu3+doping is rationally designed to mitigate the detri-mental Jahn-Teller distortion by tuning the chemical environment of MnO6 octahedra and accommodat-ing localized electron,based on the unique aspheric flexible 4f electron orbit of rare-earth metal ions.Notably,the stretching of MnO6 octahedron stemmed from the Jahn-Teller effect in Eu-doped LiMn2O4 is effectively suppressed,confirmed by theoretical calculation.Meanwhile,the structural stability of the material has been significantly enhanced due to the robust Mn-O band coherency and weakened phase transition,proved by synchrotron radiation absorption spectrum and operando X-ray diffraction.The corresponding active cathode manifests superior long-cycle stability after 300 loops at 2C and dis-plays only a 0.011％capacity drop per cycle even at 5C.Given this,this modification tactic sheds new light on achieving superior long-cycle performances by suppressing distortion in various cathode materials.

Shu Zhang;Hongyi Chen;Jun Chen;Shouyi Yin;Yu Mei;Lianshan Ni;Andi Di;Wentao Deng;Guoqiang Zou;Hongshuai Hou;Xiaobo Ji

State Key Laboratory of Powder Metallurgy,College of Chemistry and Chemical Engineering,Central South University,Changsha 410083,Hunan,China;Department of Materials and Environmental Chemistry,Stockholm University,Stockholm 10691,Sweden

能源化学

[1]Shu Zhang;Hongyi Chen;Jun Chen;Shouyi Yin;Yu Mei;Lianshan Ni;Andi Di;Wentao Deng;Guoqiang Zou;Hongshuai Hou;Xiaobo Ji-.Mitigating the Jahn-Teller distortion driven by the spin-orbit coupling of lithium manganate cathode)[J].能源化学,2022(09):379-387

manganate,MnO6,accommodat,stemmed

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