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Reversible multielectron transfer I−/IO3− cathode enabled by a hetero-halogen electrolyte for high-energy-density aqueous batteries

Nature Energy (2024)Cite this article

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Abstract

The ever-increasing need for energy-dense batteries with high safety is fuelling global research and innovations in new redox chemistry and device design. Here we show an aqueous battery employing highly concentrated hetero-halogen electrolytes that contain I− and Br-, resulting in a multielectron transfer process of I−/IO3−. The intermediate bromide species IBr and Br2, generated during the electrochemical process, enhances the reaction kinetics and alleviates the potential gap between oxidation and reduction. When using a 6 M I− electrolyte to achieve over 30 M electron transfers, the I−/IO3− cathode displayed a high specific capacity of over 840 Ah lcatholyte−1. A battery with Cd/Cd2+ as the anode demonstrated a high energy density of over 1,200 Wh lcatholyte−1. Even at an exceptionally high current density of 120 mA cm−2, an energy efficiency of 72% was obtained. Our work demonstrates that safe aqueous batteries with high energy density are possible, offering a development option for grid-scale energy storage and even electric vehicles.

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Fig. 1: The multielectron transfer process of I−/IO3− with or without the addition of Br−.
Fig. 2: Characterization of multielectron transfer of halogen electrolytes IBA.
Fig. 3: In situ observation of the charge‒discharge process of IBA under an optical microscope.
Fig. 4: Performance of a single flow aqueous battery using IBA as the catholyte and Cd/Cd2+, silicotungstic acid or V2+/V3+ as the anode.
Fig. 5: IBA-based batteries outperform current battery systems.

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Acknowledgements

We thank Y. Xi at Dalian Institute of Chemical Physics for his support in battery test. This work was financially supported by National Natural Science Foundation of China (grant number 21925804, received by X.L., 22209179, received by C.X.), International Partnership Program of the Chinese Academy of Sciences (number 121421KYSB20210028, received by X.L.).

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Author notes

  1. These authors contributed equally: Congxin Xie, Chao Wang.

Authors and Affiliations

  1. Division of Energy Storage, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China

    Congxin Xie, Yue Xu, Tianyu Li & Xianfeng Li

  2. State Key Laboratory of Catalysis, iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China

    Chao Wang & Qiang Fu

  3. University of Chinese Academy of Sciences, Beijing, China

    Chao Wang & Yue Xu

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Contributions

C.X. conceived the idea, performed the experiment and wrote the manuscript. Y.X. tested the performance of some batteries. In situ Raman test was performed by C.W. and Q.F. T.L. completed relevant theoretical calculations. X.L. supervised the work, discussed the results and revised the manuscript.

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Correspondence to Xianfeng Li.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–43, Discussion, Tables 1–4 and captions for Supplementary Videos 1 and 2.

Supplementary Video 1

During the charge–discharge process, the morphology change of the positive electrode surface of the battery assembled by IBA was detected by optical microscope. The components of each step are marked in the video.

Supplementary Video 1

Similar to Supplementary Video 1, Supplementary Video 2 is the morphology detection of IA assembled battery during charge–discharge process.

Source data

Source Data Fig. 1

Mechanism and electrochemical testing.

Source Data Fig. 2

Spectral characterization of electrochemical mechanisms.

Source Data Fig. 3

In situ optical microscope testing.

Source Data Fig. 4

Battery performance testing.

Source Data Fig. 5

Performance comparison of different electrode materials.

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Xie, C., Wang, C., Xu, Y. et al. Reversible multielectron transfer I−/IO3− cathode enabled by a hetero-halogen electrolyte for high-energy-density aqueous batteries. Nat Energy (2024). https://doi.org/10.1038/s41560-024-01515-9

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