Self-Regulatory Lean-Electrolyte Flow for Building 600Wh Kg−1-Level Rechargeable Lithium Batteries

Shi, Zhepu; Hao, Peng; He, Yangcai; Zhang, Yibin; Hu, Shoulei; Shen, Yanbin; Gu, Qingwen; Zhang, Ling; Chen, George Zheng; Hu, Di; Liu, Zhaoping; Qiu, Bao

Abstract

Reducing excess electrolytes offers a promising approach to improve the specific energy of electrochemical energy storage devices. However, using lean electrolytes presents a significant challenge for porous electrode materials due to heterogeneous wetting. The spontaneous wetting of nano- or meso-pores within particles, though seldom discussed, adversely affects wetting under lean electrolyte conditions. Herein, this undesired wetting behavior is mitigated by enlarging the pore-throat ratio, enabling Li-rich layered oxide to function effectively at very low electrolyte/capacity (E/C) ratio of 1.4 g Ah−1. The resulting pouch cell achieves 606 Wh kg−1 and retains 80% capacity (75% energy) after 70 cycles. Through imaging techniques and molecular dynamics simulations, it is demonstrated that the pore-throat ratio effectively determines the permeability of electrolyte within particles. By elucidating pore-relating mechanisms, this work unveils promising potential of manipulating pore structures in porous electrode materials, an approach that can be applied to improve the specific energy of other devices including semi-solid-state lithium batteries.

Citation

Shi, Z., Hao, P., He, Y., Zhang, Y., Hu, S., Shen, Y., Gu, Q., Zhang, L., Chen, G. Z., Hu, D., Liu, Z., & Qiu, B. (2025). Self-Regulatory Lean-Electrolyte Flow for Building 600Wh Kg−1-Level Rechargeable Lithium Batteries. Advanced Materials, https://doi.org/10.1002/adma.202419377

• Journal Article Type: Article
• Acceptance Date: Jan 19, 2025
• Online Publication Date: Jan 28, 2025
• Publication Date: Jan 28, 2025
• Deposit Date: Jan 31, 2025
• Publicly Available Date: Jan 29, 2026
• Journal: Advanced Materials
• Print ISSN: 0935-9648
• Electronic ISSN: 1521-4095
• Publisher: Wiley
• Peer Reviewed: Peer Reviewed
• DOI: https://doi.org/10.1002/adma.202419377
• Keywords: ultrahigh-energy Li batteries; porous electrode materials; pore-throat ratio; fluid dynamics; lean electrolyte
• Public URL: https://nottingham-repository.worktribe.com/output/44692110
• Publisher URL: https://advanced.onlinelibrary.wiley.com/doi/10.1002/adma.202419377