Designing a Stable Alloy Interlayer on Li Metal Anodes for Fast Charging of All-Solid-State Li Metal Batteries

The deposition of a thin LixSny alloy layer by plasma vapor deposition (PVD) on the surface of a Li foil is reported. The formation of a Li-rich alloy is confirmed by the volume expansion (up to 380%) of the layer and by the disappearance of metallic Sn peaks in the X-ray diffractogram. The layer has a much higher hardness than bare Li and can withstand aggressive cycling at 1C. Post-mortem scanning electron microscope observations revealed that the alloy layer remains intact even after fast cycling for hundreds of cycles. A concept of double modification by adding a thin ceramic/polymer layer deposited by a doctor blade on top of the LixSny layer was also reported to be efficient to reach long-term stability for 500 cycles at C/3. Finally, a post-treatment after Sn deposition consisting of a plasma cleaning of the LixSny alloy layer led to a strong improvement in the cycling performance at 1C. The surface is smoother and less oxidized after this treatment. The combination of a Li-rich alloy interlayer, the increase in hardness at the electrolyte/Li interface, and the absence of dissolution of the layer during cycling at high C-rates are reasons for such an improvement in electrochemical performance.