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An active and durable molecular catalyst for aqueous polysulfide-based redox flow batteries

Nature Energy volume 8, pages 1355–1364 (2023)Cite this article

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Abstract

Aqueous redox flow battery (RFB) is one of the most promising technologies for grid-scale energy storage systems. Polysulfides are particularly attractive active materials owing to their low cost and high capacity, but the low energy efficiency and low operating current density limit their practical applications. Here we report an active and durable molecule catalyst, riboflavin sodium phosphate (FMN-Na), to transform sluggish polysulfide reduction reactions to fast redox reactions of FMN-Na via homogeneous catalysis. The FMN-Na catalyst substantially reduces the overpotential of a polysulfide–ferrocyanide RFB (S-Fe RFB) from more than 800 mV to 241 mV at 30 mA cm−2. A catalysed S-Fe flow cell was demonstrated for 2,000 cycles at 40 mA cm−2 with a low decay rate of 0.00004% per cycle (0.0017% per day). A catalysed polysulfide–iodide RFB operated for 1,300 cycles under 40 mA cm−2 without capacity decay. This work addresses the bottleneck of polysulfide-based RFBs for long-duration energy storage applications.

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Fig. 1: The design principle for molecular catalysts on polysulfide reduction.
Fig. 2: Electrochemical performance and cycling stability of S-Fe and S-I flow cells.
Fig. 3: Operando UV-vis study on the FMN3−/FMN5− concentration evolution.
Fig. 4: Extended cycling stability of catalysed S-Fe flow cells.
Fig. 5: Extended cycling stability of catalysed S-I flow cells.
Fig. 6: Theoretical calculation on the reaction mechanism of FMN-Na and K2S4.

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The datasets analysed and generated during the current study are included in the paper and its Supplementary Information.

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Acknowledgements

The work described in this paper was supported by Research Grants Council of the Hong Kong Special Administrative Region under grant nos. N_CUHK435/18 (received by Y.-C.L.), RFS2223-4S03 (received by Y.-C.L.) and C1002-21GF (received by Y.-C.L. and J.F.). Y.-C.L. acknowledges the support from Xplorer Prize by New Cornerstone Science Foundation.

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Authors and Affiliations

  1. Electrochemical Energy and Interfaces Laboratory, Department of Mechanical and Automation Engineering, The Chinese University of Hong Kong, Hong Kong SAR, China

    Jiafeng Lei, Yanxin Yao, Yang Shi, Ka Lok Leung & Yi-Chun Lu

  2. Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, China

    Yaqin Zhang & Jun Fan

  3. Luquos Energy Limited, Hong Kong SAR, China

    Yanxin Yao & Ka Lok Leung

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  1. Jiafeng Lei
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Contributions

J.L. and Y.-C.L. conceived the projects, analysed the data and wrote the manuscript. J.L. conducted the electrochemical measurements and material characterizations. Y.Y., Y.S. and K.L.L. assisted with the electrochemical measurements. Y.Z. and J.F. conducted the theoretical calculation.

Corresponding author

Correspondence to Yi-Chun Lu.

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Competing interests

J.L. and Y.-C.L. are inventors of a patent application (US Patent application number 17/705,171) on the molecular catalysts described herein. The other authors declare no competing interests.

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Nature Energy thanks Xiaodong Lei and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–38, Notes 1 and 2, Table 1 and references.

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Lei, J., Zhang, Y., Yao, Y. et al. An active and durable molecular catalyst for aqueous polysulfide-based redox flow batteries. Nat Energy 8, 1355–1364 (2023). https://doi.org/10.1038/s41560-023-01370-0

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