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

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

Research output: Journal PublicationArticlepeer-review

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.

Original languageEnglish
JournalAdvanced Materials
DOIs
Publication statusAccepted/In press - 2025

Keywords

  • fluid dynamics
  • lean electrolyte
  • pore-throat ratio
  • porous electrode materials
  • ultrahigh-energy Li batteries

ASJC Scopus subject areas

  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering

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