Improving the oxygen redox reversibility of Li-rich battery cathode materials via Coulombic repulsive interactions strategy

Li, Qingyuan; Ning, De; Wong, Deniz; An, Ke; Tang, Yuxin; Zhou, Dong; Schuck, Götz; Chen, Zhenhua; Zhang, Nian; Liu, Xiangfeng

doi:10.1038/s41467-022-28793-9

Improving the oxygen redox reversibility of Li-rich battery cathode materials via Coulombic repulsive interactions strategy

Journal Article · Wed Mar 02 00:00:00 EST 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-022-28793-9· OSTI ID:1903918

^[1]; Ning, De ^[2]; Wong, Deniz ^[3]; ^[4]; Tang, Yuxin ^[5]; Zhou, Dong ^[3]; Schuck, Götz ^[3]; Chen, Zhenhua ^[6]; ^[6]; ^[7]

University of Chinese Academy of Sciences, Shenzhan(China); OSTI
Helmholtz-Zentrum Berlin für Materialien und Energie, Berlin (Germany); Chinese Academy of Sciences (CAS), Shenzhen (China)
Helmholtz-Zentrum Berlin für Materialien und Energie, Berlin (Germany)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Fuzhou University (China)
University of Chinese Academy of Sciences, Shanghai (China)
University of Chinese Academy of Sciences, Beijing (China)

The oxygen redox reaction in lithium-rich layered oxide battery cathode materials generates extra capacity at high cell voltages (i.e., >4.5 V). However, the irreversible oxygen release causes transition metal (TM) dissolution, migration and cell voltage decay. To circumvent these issues, we introduce a strategy for tuning the Coulombic interactions in a model Li-rich positive electrode active material, i.e., Li_1.2Mn_0.6Ni_0.2O₂. In particular, we tune the Coulombic repulsive interactions to obtain an adaptable crystal structure that enables the reversible distortion of TMO₆ octahedron and mitigates TM dissolution and migration. Moreover, this strategy hinders the irreversible release of oxygen and other parasitic reactions (e.g., electrolyte decomposition) commonly occurring at high voltages. When tested in non-aqueous coin cell configuration, the modified Li-rich cathode material, combined with a Li metal anode, enables a stable cell discharge capacity of about 240 mAh g^-1 for 120 cycles at 50 mA g^-1and a slower voltage decay compared to the unmodified Li_1.2Mn_0.6Ni_0.2O₂.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Central Universities; Chinese Academy of Sciences; National Natural Science Foundation of China; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1903918

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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