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Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium
Ahu Shao1, Helin Wang1, Min Zhang1
1State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, PR China.
Nature Communications
|May 3, 2025
Summary
Anode-free lithium batteries achieve high energy density using a novel sacrificial layer on the separator. This stabilizes interfaces, replenishes lithium inventory, and enhances performance in large-capacity cells.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Anode-free lithium batteries offer high energy density but suffer from interfacial issues like lithium loss and cathode degradation.
- Limited lithium-ion (Li+) reversibility and parasitic reactions hinder practical application of these advanced batteries.
Purpose of the Study:
- To develop a multiscale interfacial stabilization strategy for Ah-class anode-free pouch cells.
- To improve lithium inventory management and cathode interface stability for high-voltage operation.
Main Methods:
- Integration of a polyolefin separator with a lithium sulfide (Li2S@C) sacrificial layer for prelithiation.
- In-situ electrochemical impedance spectroscopy (EIS) and operando X-ray diffraction (XRD) for real-time interface analysis.
- Assembly and testing of 1.22 Ah pouch cells using LiNi0.8Co0.1Mn0.1O2 cathodes and Ag-modified Cu foil.
Main Results:
- The Li2S@C|PE separator effectively replenished Li+ inventory and stabilized the cathode interface up to 4.5 V.
- Accelerated Li+ diffusion kinetics and stabilized phase evolution were observed in the cathode.
- Achieved gravimetric and volumetric energy densities of 450 Wh kg-1 and 1355 Wh L-1 in a 1.22 Ah pouch cell.
Conclusions:
- The proposed prelithiation protocol using a sacrificial layer offers a viable solution for interfacial stabilization in anode-free lithium batteries.
- Demonstrated upscaling potential and generic applicability for securing interfacial chemistries in lithium metal batteries.
- This method enhances energy density and cycle life, paving the way for practical high-energy storage solutions.
