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Revealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor.

ABSTRACT: Understanding the Li-ions conduction network and transport dynamics in polymer electrolyte is crucial for developing reliable all-solid-state batteries. In this work, advanced nano- X-ray computed tomography combined with Raman spectroscopy and solid state nuclear magnetic resonance are used to multi-scale qualitatively and quantitatively reveal ion conduction network of poly(ethylene) oxide (PEO)-based electrolyte (from atomic, nano to macroscopic level). With the clear mapping of the microstructural heterogeneities of the polymer segments, aluminium-oxo molecular clusters (AlOC) are used to reconstruct a high-efficient conducting network with high available Li-ions (76.7%) and continuous amorphous domains via the strong supramolecular interactions. Such superionic PEO conductor (PEO-LiTFSI-AlOC) exhibites a molten-like Li-ion conduction behaviour among the whole temperature range and delivers an ionic conductivity of 1.87 × 10^-4 S cm^-1 at 35 °Ϲ. This further endows Li electrochemical plating/stripping stability under 50 μA cm^-2 and 50 μAh cm^-2 over 2000 h. The as-built Li|PEO-LiTFSI-AlOC|LiFePO₄ full batteries show a high rate performance and a capacity retention more than 90% over 200 cycling at 250 μA cm^-2, even enabling a high-loading LiFePO₄ cathode of 16.8 mg cm^-2 with a specific capacity of 150 mAh g^-1 at 50 °Ϲ.

SUBMITTER: Fang CD

PROVIDER: S-EPMC11310194 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature

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Revealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor.

Fang Cheng-Dong CD Huang Ying Y Sun Yi-Fan YF Sun Peng-Fei PF Li Ke K Yao Shu-Yang SY Zhang Min-Yi MY Fang Wei-Hui WH Chen Jia-Jia JJ

Nature communications 20240808 1

Understanding the Li-ions conduction network and transport dynamics in polymer electrolyte is crucial for developing reliable all-solid-state batteries. In this work, advanced nano- X-ray computed tomography combined with Raman spectroscopy and solid state nuclear magnetic resonance are used to multi-scale qualitatively and quantitatively reveal ion conduction network of poly(ethylene) oxide (PEO)-based electrolyte (from atomic, nano to macroscopic level). With the clear mapping of the microstru ...[more]

PMID: 39117642

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Project description:The development of fast Li ion-conducting materials for use as solid electrolytes that provide sufficient electrochemical stability against electrode materials is paramount for the future of all-solid-state batteries. Advances on these fast ionic materials are dependent on building structure-ionic mobility-function relationships. Here, we exploit a series of multinuclear and multidimensional nuclear magnetic resonance (NMR) approaches, including 6Li and 31P magic angle spinning (MAS), in conjunction with density functional theory (DFT) to provide a detailed understanding of the local structure of the ultraphosphate Li3P5O14, a promising candidate for an oxide-based Li ion conductor that has been shown to be a highly conductive, energetically favorable, and electrochemically stable potential solid electrolyte. We have reported a comprehensive assignment of the ultraphosphate layer and layered Li6O16 26- chains through 31P and 6Li MAS NMR, respectively, in conjunction with DFT. The chemical shift anisotropy of the eight resonances with the lowest 31P chemical shift is significantly lower than that of the 12 remaining resonances, suggesting the phosphate bonding nature of these P sites being one that bridges to three other phosphate groups. We employed a number of complementary 6,7Li NMR techniques, including MAS variable-temperature line narrowing spectra, spin-alignment echo (SAE) NMR, and relaxometry, to quantify the lithium ion dynamics in Li3P5O14. Detailed analysis of the diffusion-induced spin-lattice relaxation data allowed for experimental verification of the three-dimensional Li diffusion previously proposed computationally. The 6Li NMR relaxation rates suggest sites Li1 and Li5 (the only five-coordinate Li site) are the most mobile and are adjacent to one another, both in the a-b plane (intralayer) and on the c-axis (interlayer). As shown in the 6Li-6Li exchange spectroscopy NMR spectra, sites Li1 and Li5 likely exchange with one another both between adjacent layered Li6O16 26- chains and through the center of the P12O36 12- rings forming the three-dimensional pathway. The understanding of the Li ion mobility pathways in high-performing solid electrolytes outlines a route for further development of such materials to improve their performance.

Dataset Information

Revealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor.

Publications

Revealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor.

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