Lattice pinning in MoO3 via coherent interface with stabilized Li+ intercalation

Shuo Sun, Zhen Han, Wei Liu, Qiuying Xia, Liang Xue, Xincheng Lei, Teng Zhai (), Dong Su () and Hui Xia ()
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Shuo Sun: Nanjing University of Science and Technology
Zhen Han: Institute of Physics, Chinese Academy of Sciences
Wei Liu: Nanjing University of Science and Technology
Qiuying Xia: Nanjing University of Science and Technology
Liang Xue: Nanjing University of Science and Technology
Xincheng Lei: Institute of Physics, Chinese Academy of Sciences
Teng Zhai: Nanjing University of Science and Technology
Dong Su: Institute of Physics, Chinese Academy of Sciences
Hui Xia: Nanjing University of Science and Technology

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Large lattice expansion/contraction with Li+ intercalation/deintercalation of electrode active materials results in severe structural degradation to electrodes and can negatively impact the cycle life of solid-state lithium-based batteries. In case of the layered orthorhombic MoO3 (α-MoO3), its large lattice variation along the b axis during Li+ insertion/extraction induces irreversible phase transition and structural degradation, leading to undesirable cycle life. Herein, we propose a lattice pinning strategy to construct a coherent interface between α-MoO3 and η-Mo4O11 with epitaxial intergrowth structure. Owing to the minimal lattice change of η-Mo4O11 during Li+ insertion/extraction, η-Mo4O11 domains serve as pin centers that can effectively suppress the lattice expansion of α-MoO3, evidenced by the noticeably decreased lattice expansion from about 16% to 2% along the b direction. The designed α-MoO3/η-Mo4O11 intergrown heterostructure enables robust structural stability during cycling (about 81% capacity retention after 3000 cycles at a specific current of 2 A g−1 and 298 ± 2 K) by harnessing the merits of epitaxial stabilization and the pinning effect. Finally, benefiting from the stable positive electrode–solid electrolyte interface, a highly durable and flexible all-solid-state thin-film lithium microbattery is further demonstrated. This work advances the fundamental understanding of the unstable structure evolution for α-MoO3, and may offer a rational strategy to develop highly stable electrode materials for advanced batteries.

Date: 2023
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DOI: 10.1038/s41467-023-42335-x

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