Understanding and Designing Lithiophilic Alloyed Metal Anodes for Practical Metal Batteries.

Abstract

Lithiophilic alloyed metal anodes (LAMAs) are emerging as a transformative platform for enabling practical Li metal batteries. By harnessing alloy chemistry, LAMAs combine favorable Li nucleation and growth behavior, robust interfacial chemistry, and mechanical integrity, thereby mitigating the long-standing challenges of manufacturability and cycling stability that have hindered large-scale deployment of Li metal anodes. Nevertheless, a unifying framework that quantitatively defines lithiophilicity, the central design parameter of LAMAs, remains underdeveloped. This review establishes a descriptor-based paradigm to systematically elucidate lithiophilicity, bridging empirical observations with thermodynamic, kinetic, and electronic-structure descriptors, while also addressing the temporal stability of lithiophilic interfaces. Building upon these insights, we critically analyze state-of-the-art strategies for designing and fabricating LAMAs, including alloy-embedded architectures, interfacial engineering approaches, modified current collector substrates, Li-free anode concepts, and all-solid-state configurations. We conclude by outlining key research opportunities and design principles that couple materials chemistry, interfacial science, and scalable manufacturing, aiming to accelerate the rational development of LAMAs for high-energy, industrially viable Li metal batteries.