Lithophilic metal–ceramic Achieving high durability in lithium-metal batteries via lithophilic metal-ceramic interface engineering

Abstract

Highly reactive lithium (Li) requires precise control of nucleation and growth, necessitating stable processing techniques for the fabrication of Li-metal batteries. This study proposes a novel strategy to mitigate Li dendrite formation using a dual-layer protective coating composed of a ceramic (Al₂O₃) and lithophilic metal (Au) fabricated via a solvent-free transfer printing process. The dual-layer structure consists of a Au layer positioned between Al₂O₃ and Li metal, where the Al₂O₃ layer suppresses dendrite growth and promotes uniform Li-ion flux. Meanwhile, the Au layer functions as a seed for Li deposition, reducing the nucleation overpotential of Li deposition through the Au-Li alloy formation, thus enabling uniform Li deposition. Using synchrotron-based operando X-ray computed tomography (CT), we directly visualized and analyzed the Li growth mechanisms within the Al₂O₃@Au dual-layer structure, confirming its role in facilitating uniform Li deposition and effectively preventing dendrite formation. This structural synergy resulted in superior battery performance. the Al₂O₃@Au dual-layer demonstrated outstanding performance in NCM811/Li cells (2.6 mAh cm^⁻2), achieving a capacity retention rate of over 85 % and Coulombic efficiency exceeding 99.8 % after 150 cycles. This study offers a scalable and practical approach to stabilizing Li metal anodes, thus paving the way for next-generation batteries.