Realizing four-electron conversion chemistry for all-solid-state Li||I2 batteries at room temperature

Zhu Cheng, Hang Liu, Menghang Zhang, Hui Pan, Chuanchao Sheng, Wei Li, Marnix Wagemaker, Ping He (pinghe@nju.edu.cn) and Haoshen Zhou (hszhou@nju.edu.cn)
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Zhu Cheng: Nanjing University
Hang Liu: Nanjing University
Menghang Zhang: Nanjing University
Hui Pan: Nanjing University
Chuanchao Sheng: Nanjing University
Wei Li: Nanjing University
Marnix Wagemaker: Delft University of Technology
Ping He: Nanjing University
Haoshen Zhou: Nanjing University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Rechargeable Li||I2 batteries based on liquid organic electrolytes suffer from pronounced polyiodides shuttling and safety concerns, which can be potentially tackled by the use of solid-state electrolytes. However, current all-solid-state Li||I2 batteries only demonstrate limited capacity based on a two-electron I−/I2 polyiodides chemistry at elevated temperatures, preventing them from rivaling state-of-the-art lithium-ion batteries. Herein, we report a fast, stable and high-capacity four-electron solid-conversion I−/I2/I+ chemistry in all-solid-state Li||I2 batteries at room temperature. Through the strategic use of a highly conductive, chlorine-rich solid electrolyte Li4.2InCl7.2 as the catholyte, we effectively activate the I2/I+ redox couple. This activation is achieved through a robust I-Cl interhalogen interaction between I2 and the catholyte, facilitated by an interface-mediated heterogeneous oxidation mechanism. Moreover, apart from serving as Li-ion conduction pathway, the Li4.2InCl7.2 catholyte is demonstrated to show a reversible redox behavior and contribute to the electrode capacity without compromising its conductivity. Based on the I−/I2/I+ four-electron chemistry, the as-designed all-solid-state Li||I2 batteries deliver a high specific capacity of 449 mAh g-1 at 44 mA g-1 based on I2 mass and an impressive cycling stability over 600 cycles with a capacity retention of 91% at 440 mA g-1 and at 25 °C.

Date: 2025
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DOI: 10.1038/s41467-025-56932-5

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