DOI: 10.1002/adma.74644 ISSN: 0935-9648

Quantifying the Correlation Between Capacity Utilization and Electrolyte Dosage for Ultrahigh‐Energy‐Density 769 Wh Kg −1 Rechargeable Lithium Metal Batteries

Shuo Zhang, Yuyang Lu, Chong Yan, Xiangbiao Liao, Chen‐Zi Zhao, Jun‐Wei Zhao, Zhiyuan Dong, Zhenwei Zhu, Wenjie Meng, Xue‐Fei Wen, Peng Wu, Jian Pei, Meng‐Yao Wang, Xue‐Kun Cao, Jiang‐Kui Hu, Xiang Chen, Jingyi Qiu, Hao Zhang, Jia‐Qi Huang, Qiang Zhang

ABSTRACT

The pursuit of high‐energy‐density lithium metal batteries requires simultaneous optimization of electrode architecture, electrolyte formulation, and interfacial stability. Here, we establish a fundamental parameter g(σ e , D e ) that quantifies the relationship between electrolyte dosage and capacity utilization in ultra‐thick electrodes (>100.0 µm), enabling precise determination of the minimal electrolyte requirement (1.1 g Ah −1 ). Through systematic investigation of electrolyte compatibility with high‐loading cathodes (> 10.0 mAh cm −2 ) at high voltages (4.8 V), we develop an optimized formulation that forms stable interfaces while suppressing parasitic reactions. By integrating these advances—including a lightweight lithium metal anode—we demonstrate a 54.2 Ah pouch cell achieving 769 Wh kg −1 , representing a 150% improvement over conventional lithium‐ion batteries. This work provides both theoretical and practical frameworks for engineering next‐generation batteries through electrolyte minimization and interface stabilization.

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