The Dr Jekyll and Mr Hyde of lithium hydride in lithium dendrites and solid-electrolyte interphases

The Dr Jekyll and Mr Hyde of lithium hydride in lithium dendrites and solid-electrolyte interphases

Nano Energy

10.1016/j.nanoen.2025.111243

https://doi.org/10.1016/j.nanoen.2025.111243

Xiang Feng, Yuanjian Li, Jinming Wang, Lin Fu, Tianshuai Wang, Anjun Hu, Qiuming Peng, Zhi Wei Seh, Qianfan Zhang

13 June 2025

Feng, X., Li, Y., Wang, J., Fu, L., Wang, T., Hu, A., Peng, Q., Seh, Z. W., & Zhang, Q. (2025). The Dr Jekyll and Mr Hyde of lithium hydride in lithium dendrites and solid-electrolyte interphases. Nano Energy, 142, 111243. https://doi.org/10.1016/j.nanoen.2025.111243

Lithium (Li) hydride (LiH) is widely observed in both the solid electrolyte interphase (S-LiH) and Li dendrites (D-LiH) on Li metal anodes (LMAs). Although considerable research has been devoted to LiH, its role in the LMA remains controversial. In this work, we utilize theoretical calculations to disentangle the chemical components in the solid electrolyte interphase (SEI) and dendrites, systematically analyzing the physicochemical properties of each component. Our results exhibit fundamentally opposite roles for S-LiH and D-LiH: S-LiH enhances cycling stability and suppresses dendrite growth due to its electron-blocking capability, robust Li+ conductivity across crystal sizes, and its role as an active stabilizer at the Li/LiH interface. Conversely, D-LiH, with its electronic insulation and extreme brittleness, is identified as the primary cause of capacity decay and anode pulverization. Furthermore, by analyzing electrochemical windows, we explore the thermodynamic mechanisms underpinning the formation, transformation, and decomposition of SEI and dendrite components, providing theoretical explanations for experimental anomalies associated with LiH. Building on these insights, we propose strategies to optimize LiH management, harnessing the advantages of S-LiH while mitigating the adverse impacts of D-LiH. Overall, our work offers a deeper understanding of LiH, laying a foundation for advancing Li battery technologies.

Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0)

This research / project is supported by the Singapore National Research Foundation - NRF Investigatorship NRF-NRFI09-0002
Grant Reference no. : NRF-NRFI09-0002

This research / project is supported by the the Agency for Science, Technology and Research - Manufacturing, Trade, and Connectivity Programmatic Fund M23L9b0052
Grant Reference no. : M23L9b0052

https://oar.a-star.edu.sg/communities-collections/articles/23495

2211-2855

Institute of Materials Research and Engineering