Modulating Local Structure of Amorphous Oxyhalide to Achieve High-Rate and Ultra-Stable All-Solid-State Lithium Battery.
basic_science · Level V
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- Record sourced from PubMed, PMID 42438333.
- Also identified by DOI 10.1002/adma.74138.
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Abstract
Halides-based all-solid-state lithium batteries (ASSLBs) attract great attention because of their wide electrochemical window and fine processibility. However, low ionic conductivity of halides and solid-solid interface incompatibility result in inferior rate capability and poor cycling stability. Herein, we modulate local structure (short-range-structure disorder degree, coordination diversity, and so forth) via a synergistic anion-cation strategy to achieve amorphous solid electrolyte 1.6Li<sub>2</sub>O-TaCl<sub>5</sub>-0.3MgF<sub>2</sub> (LTOC-M) with a high ionic conductivity (11.15 mS cm<sup>-1</sup>) and favorable interfacial compatibility. F incorporation at Cl/O sites strengthens Ta─F bonding and Li-F interactions, enhancing long-term cycling stability, while Mg incorporation modulates the local cationic environment, increases coordination diversity, and facilitates Li<sup>+</sup> transport within the amorphous matrix. ASSLBs with LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> or LiCoO<sub>2</sub> demonstrate superhigh rate capability and long-term cycling stability (LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>:92.29%@4000cycles@5C; LiCoO<sub>2</sub>:80.85%@5000cycles@10C). When paired with Li-rich Li<sub>1.2</sub>Mn<sub>0.54</sub>Ni<sub>0.13</sub>Co<sub>0.13</sub>O<sub>2</sub>, the cell delivers a high initial capacity of 270.38 mAh g<sup>-1</sup> with a cycling stability (92.75%@120cycles@0.2C). Moreover, Li-In| Li<sub>6</sub>PS<sub>5</sub>Cl-LTOC-M|LiCoO<sub>2</sub> delivers a high discharge capacity of 128.80 mAh g<sup>-1</sup> at -20°C and demonstrates a cycling stability (96.62%@550cycles@0.2C), and the battery functions even at -75°C for over 400 h. The proposed strategy effectively enhances high-rate performance, long-term cycling stability and low-temperature performance of halides-based ASSLBs, accelerating their practical application.