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Topotactically transformable antiphase boundaries with enhanced ionic conductivity.

ABSTRACT: Engineering lattice defects have emerged as a promising approach to effectively modulate the functionality of devices. Particularly, antiphase boundaries (APBs) as planar defects have been considered major obstacles to optimizing the ionic conductivity of mixed ionic-electronic conductors (MIECs) in solid oxide fuel applications. Here our study identifies topotactically transformable APBs (tt-APBs) at the atomic level and demonstrates that they exhibit higher ionic conductivity at elevated temperatures as compared to perfect domains. In-situ observation at the atomic scale tracks dynamic oxygen migration across these tt-APBs, where the abundant interstitial sites between tetrahedrons facilitate the ionic migration. Furthermore, annealing in an oxidized atmosphere can lead to the formation of interstitial oxygen at these APBs. These pieces of evidence clearly clarify that the tt-APBs can contribute to oxygen conductivity as anion diffusion channels, while the topotactically non-transformable APBs cannot. The topotactic transformability opens the way of defect engineering strategies for improving ionic transportation in MIECs.

SUBMITTER: Xu K

PROVIDER: S-EPMC10651924 | biostudies-literature | 2023 Nov

REPOSITORIES: biostudies-literature

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Topotactically transformable antiphase boundaries with enhanced ionic conductivity.

Xu Kun K Hung Shih-Wei SW Si Wenlong W Wu Yongshun Y Huo Chuanrui C Yu Pu P Zhong Xiaoyan X Zhu Jing J

Nature communications 20231115 1

Engineering lattice defects have emerged as a promising approach to effectively modulate the functionality of devices. Particularly, antiphase boundaries (APBs) as planar defects have been considered major obstacles to optimizing the ionic conductivity of mixed ionic-electronic conductors (MIECs) in solid oxide fuel applications. Here our study identifies topotactically transformable APBs (tt-APBs) at the atomic level and demonstrates that they exhibit higher ionic conductivity at elevated tempe ...[more]

PMID: 37968326

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Project description:Solvent-free polymer-based electrolytes (SPEs) have gained significant attention to realize safer and flexible lithium-ion batteries. Among all polymers used for preparing SPEs electrolytes, poly(ethylene oxide), a biocompatible and biodegradable polymer, has been the most prevalent one mainly because of its high ionic conductivity in the molten state, the capability for the dissolution of a wide range of different lithium salts as well as its potential for the environmental health and safety. However, linear PEO is highly semicrystalline at room temperature and thus exhibits weak mechanical performance. Addition of nanoparticles enhances the mechanical strength and effectively decreases the crystallization of linear PEO, yet enhancement in mechanical performance often results in decreased ionic conductivity when compared to the neat linear PEO-based electrolytes; new strategies for decoupling ionic conductivity from mechanical reinforcement are urgently needed. Herein, we used lithium bis(trifluoromethane-sulfonyl)-imide (LiTFSI) salts dissolved in various nonlinear PEO architectures, including stars (4-arms and 8-arms) and hyperbranched matrices, and SiO2 nanoparticles (approximately equal to 50 nm diameter) as fillers. Compared to the linear PEO chains, the room temperature crystallinity was eliminated in the branched PEO architectures. The electrolytes with good dispersion of the nanoparticles in the nonlinear PEOs significantly enhanced ionic conductivity, specifically by approximately equal to 40% for 8-arm star, approximately equal to 28% for 4-arms star, and approximately equal to %16 for hyperbranched matrices, with respect to the composite electrolyte with the linear matrix. Additionally, the rheological results of the SPEs with branched architectures show more than three orders of magnitude enhancement in the low-frequency moduli compared to the neat linear PEO/Li systems. The obtained results demonstrate that the solvent-free composite electrolytes made of branched PEO architectures can be quite promising especially for irregularly shaped and environmentally benign battery applications suitable for medical implants, wearable devices, and stretchable electronics, which require biodegradability and biocompatibility.

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Topotactically transformable antiphase boundaries with enhanced ionic conductivity.

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Topotactically transformable antiphase boundaries with enhanced ionic conductivity.

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