Unraveling the Coupling Effect between Cathode and Anode toward Practical Lithium-Sulfur Batteries.

Gao, Runhua; Zhang, Mengtian; Han, Zhiyuan; Xiao, Xiao; Wu, Xinru; Piao, Zhihong; Lao, Zhoujie; Nie, Lu et al. · Adv Mater · 2024

basic_science · Level V

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Abstract

The localized reaction heterogeneity of the sulfur cathode and the uneven Li deposition on the Li anode are intractable issues for lithium-sulfur (Li-S) batteries under practical operation. Despite impressive progress in separately optimizing the sulfur cathode or Li anode, a comprehensive understanding of the highly coupled relationship between the cathode and anode is still lacking. In this work, inspired by the Butler-Volmer equation, a binary descriptor (I<sub>BD</sub> ) assisting the rational structural design of sulfur cathode by simultaneously considering the mass-transport index (I<sub>mass</sub> ) and the charge-transfer index (I<sub>charge</sub> ) is identified, and subsequently the relationship between I<sub>BD</sub> and the morphological evolution of Li anode is established. Guided by the I<sub>BD</sub> , a scalable electrode providing interpenetrated flow channels for efficient mass/charge transfer, full utilization of active sulfur, and mechanically elastic support for aggressive electrochemical reactions under practical conditions is reported. These characteristics induce a homogenous distribution of local current densities and reduced reaction heterogeneity on both sides of the cathode and anode. Impressive energy density of 318 Wh kg<sup>-1</sup> and 473 Wh L<sup>-1</sup> in an Ah-level pouch cell can be achieved by the design concept. This work offers a promising paradigm for unlocking the interaction between cathode and anode and designing high-energy practical Li-S batteries.