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Anomalous metal segregation in lithium-rich material provides design rules for stable cathode in lithium-ion battery

Ruoqian Lin, Enyuan Hu, Mingjie Liu, Yi Wang, Hao Cheng, Jinpeng Wu, Jin-Cheng Zheng, Qin Wu, Seongmin Bak, Xiao Tong, Rui Zhang, Wanli Yang, Kristin A. Persson, Xiqian Yu (), Xiao-Qing Yang () and Huolin L. Xin ()
Additional contact information
Ruoqian Lin: Brookhaven National Laboratory
Enyuan Hu: Brookhaven National Laboratory
Mingjie Liu: Brookhaven National Laboratory
Yi Wang: Chinese Academy of Sciences
Hao Cheng: Xiamen University
Jinpeng Wu: Lawrence Berkeley National Laboratory
Jin-Cheng Zheng: Xiamen University
Qin Wu: Brookhaven National Laboratory
Seongmin Bak: Brookhaven National Laboratory
Xiao Tong: Brookhaven National Laboratory
Rui Zhang: University of California
Wanli Yang: Lawrence Berkeley National Laboratory
Kristin A. Persson: Lawrence Berkeley National Laboratory
Xiqian Yu: Chinese Academy of Sciences
Xiao-Qing Yang: Brookhaven National Laboratory
Huolin L. Xin: Brookhaven National Laboratory

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

Abstract: Abstract Despite the importance of studying the instability of delithiated cathode materials, it remains difficult to underpin the degradation mechanism of lithium-rich cathode materials due to the complication of combined chemical and structural evolutions. Herein, we use state-of-the-art electron microscopy tools, in conjunction with synchrotron X-ray techniques and first-principle calculations to study a 4d-element-containing compound, Li2Ru0.5Mn0.5O3. We find surprisingly, after cycling, ruthenium segregates out as metallic nanoclusters on the reconstructed surface. Our calculations show that the unexpected ruthenium metal segregation is due to its thermodynamic insolubility in the oxygen deprived surface. This insolubility can disrupt the reconstructed surface, which explains the formation of a porous structure in this material. This work reveals the importance of studying the thermodynamic stability of the reconstructed film on the cathode materials and offers a theoretical guidance for choosing manganese substituting elements in lithium-rich as well as stoichiometric layer-layer compounds for stabilizing the cathode surface.

Date: 2019
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DOI: 10.1038/s41467-019-09248-0

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