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

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.

SUBMITTER: Sun S

PROVIDER: S-EPMC10589268 | biostudies-literature | 2023 Oct

REPOSITORIES: biostudies-literature

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

Sun Shuo S Han Zhen Z Liu Wei W Xia Qiuying Q Xue Liang L Lei Xincheng X Zhai Teng T Su Dong D Xia Hui H

Nature communications 20231020 1

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 undesirabl ...[more]

PMID: 37863930

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Project description:Alkali ion intercalation is fundamental to battery technologies for a wide spectrum of potential applications that permeate our modern lifestyle, including portable electronics, electric vehicles, and the electric grid. In spite of its importance, the Nernstian nature of the charge transfer process describing lithiation of carbon has not been described previously. Here we use the ultrathin few-layer graphene (FLG) with micron-sized grains as a powerful platform for exploring intercalation and co-intercalation mechanisms of alkali ions with high versatility. Using voltammetric and chronoamperometric methods and bolstered by density functional theory (DFT) calculations, we show the kinetically facile co-intercalation of Li+ and K+ within an ultrathin FLG electrode. While changes in the solution concentration of Li+ lead to a displacement of the staging voltammetric signature with characteristic slopes ca. 54-58 mV per decade, modification of the K+/Li+ ratio in the electrolyte leads to distinct shifts in the voltammetric peaks for (de)intercalation, with a changing slope as low as ca. 30 mV per decade. Bulk ion diffusion coefficients in the carbon host, as measured using the potentiometric intermittent titration technique (PITT) were similarly sensitive to solution composition. DFT results showed that co-intercalation of Li+ and K+ within the same layer in FLG can form thermodynamically favorable systems. Calculated binding energies for co-intercalation systems increased with respect to the area of Li+-only domains and decreased with respect to the concentration of -K-Li- phases. While previous studies of co-intercalation on a graphitic anode typically focus on co-intercalation of solvents and one particular alkali ion, this is to the best of our knowledge the first study elucidating the intercalation behavior of two monovalent alkali ions. This study establishes ultrathin graphitic electrodes as an enabling electroanalytical platform to uncover thermodynamic and kinetic processes of ion intercalation with high versatility.

Dataset Information

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

Publications

Lattice pinning in MoO<sub>3</sub> via coherent interface with stabilized Li<sup>+</sup> intercalation.

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