Recently, the team led by Professor Ruqiang Zou and Associate Researcher Lei Gao from the School of Advanced Materials (SAM) at Peking University Shenzhen Graduate School, in collaboration with Southern University of Science and Technology and Shenzhen Eacomp Technology Co., Ltd., published a research paper titled “Dynamic Control of Lithium Dendrite Growth with Sequential Guiding and Limiting in All-Solid-State Batteries” in the top-tier international journal Science Advances (DOI: 10.1126/sciadv.adw9590). The study innovatively proposes and implements a “guiding + limiting” strategy for the dynamic regulation of lithium dendrites, achieving effective channeling and self-limiting growth of lithium dendrites through structural design of the solid-state electrolyte layer.
All-solid-state lithium metal batteries are considered a key development direction for next-generation energy storage systems due to their superior safety and higher theoretical energy density. However, during battery cycling, lithium dendrites easily form at the anode interface, and their continuous growth may penetrate the electrolyte, causing short circuits and safety hazards, which limits the large-scale application of all-solid-state lithium metal batteries. Conventional wisdom suggests that high-mechanical-strength solid-state electrolytes can effectively suppress lithium dendrite growth. However, experimental studies show that even high-modulus electrolytes (e.g., Li7La3Zr2O12, 51–62 GPa) can be penetrated by lithium dendrites at low current densities. This is primarily due to microscopic defects such as grain boundaries and pores within the solid-state electrolyte, which provide potential growth paths for lithium dendrites. Although techniques like densification sintering or interface coating can optimize these defects, they are difficult to eliminate entirely, indicating that completely suppressing lithium dendrite growth is nearly impossible.
To address this challenge, the research team adopted a novel approach, proposing a “guiding its nature to control its form” strategy—rather than attempting to fully suppress lithium dendrites, they guide their orderly growth and achieve self-limitation at critical locations. The team designed a hierarchical structure layer composed of coarse and fine particles as a stable interface layer covering the surface of solid-state electrolytes prone to reacting with lithium metal (e.g., Li2ZrCl6 or Li10GeP2S12). The coarse particles provide mechanical rigidity to hinder dendrite penetration, while the fine particles fill gaps to maintain good interfacial contact and ensure lithium-ion transport. This hierarchical structure not only spatially guides the lithium dendrite growth path but also leverages the stress generated from local reactions between lithium dendrites and solid-state electrolytes like Li2ZrCl6 to induce a “self-limiting effect,” forming a self-limiting region at the interface that restricts further dendrite growth. This achieves dynamic regulation of lithium dendrites, significantly enhancing interface stability and battery cycle life.
Experimental results demonstrate that this strategy significantly improves the cycling stability of symmetric batteries and is compatible with various mainstream cathode materials (e.g., LiFePO4, LiCoO2, LiNi0.8Mn0.1Co0.1O2). Through experimental characterization and phase-field simulations, the study further validated the controlled distribution, guided growth, and self-limiting process of lithium dendrites within the hierarchical structure, revealing the force-electrochemical coupling regulation mechanism in this electrolyte structure. Additionally, the strategy exhibits excellent versatility. This has been validated in multiple solid-state electrolyte systems, demonstrating its broad application potential as a universal interface engineering approach.
Figure 1. Schematic of the solid-state electrolyte structure design and lithium dendrite regulation mechanism
Professor Ruqiang Zou and Associate Researcher Lei Gao from School of Advanced Materials at Peking University, Research Professor Songbai Han from Southern University of Science and Technology, and Dr. Yunxing Zuo from Shenzhen Eacomp Technology Co., Ltd. are the co-corresponding authors of this paper. Doctoral student Longbang Di from the SAM and Zongji Huang from Shenzhen Eacomp Technology Co., Ltd. are the co-first authors. Associate Professor Jiaxin Zheng from the SAM made significant contributions to the theoretical calculations of this work. The research was supported by the National Natural Science Foundation of China and the National Key Research and Development Program.
Link to the paper: https://www.science.org/doi/10.1126/sciadv.adw9590
