Correlation between manganese dissolution and dynamic phase stability in spinel-based lithium-ion battery

Tongchao Liu, Alvin Dai, Jun Lu (), Yifei Yuan, Yinguo Xiao, Lei Yu, Matthew Li, Jihyeon Gim, Lu Ma, Jiajie Liu, Chun Zhan, Luxi Li, Jiaxin Zheng, Yang Ren, Tianpin Wu, Reza Shahbazian-Yassar, Jianguo Wen, Feng Pan () and Khalil Amine ()
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Tongchao Liu: Shenzhen Graduate School
Alvin Dai: Argonne National Laboratory
Jun Lu: Argonne National Laboratory
Yifei Yuan: Argonne National Laboratory
Yinguo Xiao: Shenzhen Graduate School
Lei Yu: Argonne National Laboratory
Matthew Li: Argonne National Laboratory
Jihyeon Gim: Argonne National Laboratory
Lu Ma: Argonne National Laboratory
Jiajie Liu: Shenzhen Graduate School
Chun Zhan: Argonne National Laboratory
Luxi Li: Argonne National Laboratory
Jiaxin Zheng: Shenzhen Graduate School
Yang Ren: Argonne National Laboratory
Tianpin Wu: Argonne National Laboratory
Reza Shahbazian-Yassar: University of Illinois at Chicago
Jianguo Wen: Argonne National Laboratory
Feng Pan: Shenzhen Graduate School
Khalil Amine: Argonne National Laboratory

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract Historically long accepted to be the singular root cause of capacity fading, transition metal dissolution has been reported to severely degrade the anode. However, its impact on the cathode behavior remains poorly understood. Here we show the correlation between capacity fading and phase/surface stability of an LiMn2O4 cathode. It is revealed that a combination of structural transformation and transition metal dissolution dominates the cathode capacity fading. LiMn2O4 exhibits irreversible phase transitions driven by manganese(III) disproportionation and Jahn-Teller distortion, which in conjunction with particle cracks results in serious manganese dissolution. Meanwhile, fast manganese dissolution in turn triggers irreversible structural evolution, and as such, forms a detrimental cycle constantly consuming active cathode components. Furthermore, lithium-rich LiMn2O4 with lithium/manganese disorder and surface reconstruction could effectively suppress the irreversible phase transition and manganese dissolution. These findings close the loop of understanding capacity fading mechanisms and allow for development of longer life batteries.

Date: 2019
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DOI: 10.1038/s41467-019-12626-3

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