Fully Lithiated Li<sub><i>x</i></sub>TiO<sub>2-δ</sub> Layer Coated Separator for Securing a Lithium-less Anode in an Ester-Based Electrolyte.
basic_science · Level V
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- Record sourced from PubMed, PMID 40455585.
- Also identified by DOI 10.1021/acsnano.5c03410.
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Abstract
Ester-based electrolytes, known for their cost-effectiveness and wide voltage windows, face compatibility challenges with lithium metal (Li<sup>0</sup>), leading to irreversible decomposition and dendrite growth, which impede their application in high-energy-density lithium metal batteries (LMBs). This work develops an electrochemical prelithiation strategy to obtain a fully lithiated Li<sub><i>x</i></sub>TiO<sub>2-δ</sub> coated polypropylene (PP) separator with oxygen vacancies, preventing the depletion of limited Li<sup>0</sup> resources while promoting uniform Li<sup>0</sup> plating. Moreover, the dense closest packing structure of Li<sub><i>x</i></sub>TiO<sub>2-δ</sub> can reduce the contact area and side reaction between Li<sup>0</sup> and ester-based electrolytes, stabilizing the solid electrolyte interface (SEI) on Li<sup>0</sup>. Symmetric Li cells operating under 1.0 mA cm<sup>-2</sup> and 1.0 mA h cm<sup>-2</sup> demonstrate a long cycle life exceeding 5000 h. Full cells with NMC811 cathodes (4.3 mA h cm<sup>-2</sup> areal capacity) and Li anodes (40 μm, N/P ratio ≈ 1.9) maintain 90% capacity retention after 100 cycles with an average Coulombic efficiency (CE<sub>avg</sub>) exceeding 99.85%. The anode-free Cu|NMC811 cells also show a CE<sub>avg</sub> of 98.36% after 60 cycles. This work provides a cost-effective strategy to enhance the safety, cycling stability, and energy density of next-generation LMBs.