Multidimensional synergistic gradient architectures for lithium-metal anodes: Design philosophy, dynamic interfacial engineering, and scalable applications

Abstract

Lithium-metal anodes (LMAs) are central to next-generation high-energy batteries but are plagued by dendritic growth, interfacial instability, and volume fluctuations. This review introduces multidimensional synergistic gradient architectures as a novel strategy, offering a comprehensive solution to reconcile the conflicting requirements of lithiophilicity, mechanical durability, and effective ion transport. In contrast to previous reviews that have predominantly emphasized isolated gradient characteristics, we pioneer a systematic framework that integrates chemical composition gradients, mechanical property gradients, and ion-transport gradients across atomic, micro-, and macroscales. Each gradient type is analyzed to elucidate its mechanistic influence on lithium nucleation, suppression of dendritic formation, and stabilization of the interfaces, with particular attention given to their synergistic interactions. Crucially, we unveil the dynamic evolution of gradient interfaces throughout the cycling process, leveraging operando characterization to expose degradation pathways such as lithium-ion depletion and interfacial delamination. By merging the principles of rational design, dynamic interfacial engineering, and practical scalability, this review offers transformative insights aimed at propelling LMAs from experimental innovations to commercial applications. We outline a strategic roadmap for the development of safe and high-performance energy storage systems, underscoring the potential for LMAs to revolutionize the battery landscape.