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Ampere-hour-scale zinc–air pouch cells

Abstract

All-solid-state zinc–air pouch cells promise high energy-to-cost ratios with inherent safety; however, finding earth-abundant high power/energy cathodes and super-ionic electrolytes remains a fundamental challenge. Here we present realistic zinc–air pouch cells designed by the (101)-facet copper phosphosulfide [CPS(101)] as a cathode as well as anti-freezing chitosan-biocellulosics as super-ionic conductor electrolytes. The proposed CPS(101) exhibits trifunctional activity and stability (>30,000 cycles) towards reversible oxygen reactions and hydrogen evolution reactions, outperforming commercial Pt/C and RuO2. Furthermore, hydroxide super-ion conductors utilizing polymerized chitosan-biocellulosics reveal exceptional conductivity (86.7 mS cm−1 at 25 °C) with high mechanical/chemical robustness. High cell-level energy densities of 460 Wh kgcell–1/1,389 Wh l−1 are normally measured in pouch cells (1 Ah) with a cycle lifespan of 6,000/1,100 cycles at 25 mA cm−2 for 20/70% depths of discharge, and the highest densities we could achieve were 523 Wh kgcell–1/1,609 Wh l−1. Flexible pouch cells operate well at rates of 5–200 mA cm−2 over a broad temperature range of −20 to 80 °C.

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Fig. 1: Design strategy for high-energy ZPCs and a comparison with commercial energy storage cells.
Fig. 2: Bifunctional electrochemical (ORR and OER) performances and the kinetics for copper-based cathodes.
Fig. 3: Theoretical calculations of electrocatalytic CPS activities.
Fig. 4: Charge compensation mechanism of CPS(101) cathode.
Fig. 5: Synthesis and characterization of super-ionic CBC conductors.
Fig. 6: Electrochemical performances of flexible ZPCs under commercially available conditions.
Fig. 7: Electrochemical performance of CPS(101)||CBCs||patterned zinc||CBCs||CPS(101) pouch cells under harsh conditions.

Data availability

The data supporting the findings of this study are available within the article and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work was supported by the Creative Materials Discovery Program (grant no. 2018M3D1A1057844) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT. S.U.L. thanks the Basic Science Research Program through the NRF funded by the Ministry of Science, ICT and Future Planning (grant no. 2018R1A2B6006320).

Author information

Affiliations

Authors

Contributions

S.S.S. and J.-H.L. conceived of and designed the research projects. S.S.S., J.Y.J., and N.K.W. fabricated the materials, designed the pouch cells, and performed electrochemical measurements. C.-H.L. and S.U.L. performed the computational calculations. D.-H.K. and S.-H.K. characterized the materials. S.S.S. and J.-H.L. analysed the data and wrote the manuscript. All authors contributed to the interpretation of the results. J.-H.L. directed the research.

Corresponding authors

Correspondence to Sang Uck Lee or Jung-Ho Lee.

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Competing interests

The Republic of Korea patents related to this work have been filed (KR10-2020-0021252, KR 10-2020-0021253, KR 10-2020-0021894, KR 10-2020-0164652, KR 10-2020-0164653, KR 10-2020-0164654, KR 10-2020-0164655, KR 10-2020-0164656, KR 10-2020-0164657, KR 10-2021-0008626, KR 10-2021-0008627, KR 10-2021-0023680, KR 10-2021-0023682). The PCT patents to the work have also been filed (PCT/KR2021/002214, PCT/KR2021/002215, PCT/KR2021/002216, PCT/KR2021/002217, PCT/KR2021/002218).

Additional information

Peer review information Nature Energy thanks Yuan Chen and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–87, Notes 1–7, Tables 1–14 and Supplementary Methods.

Supplementary Video 1

Smartphone charging.

Supplementary Video 2

LED illumination.

Supplementary Video 3

Smartphone charging under flexible conditions.

Supplementary Video 4

LED illumination under flexible conditions.

Supplementary Video 5

LED illumination at 0 °C temperature.

Supplementary Data

OER CV stability and battery cycling after mechanical tests.

Source data

Source Data Fig. 1

Energy performance, pie chart distribution, and specific energy and power density values comparison.

Source Data Fig. 2

ORR CV cycles.

Source Data Fig. 6

Battery cycling for long-term stability.

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Shinde, S.S., Jung, J.Y., Wagh, N.K. et al. Ampere-hour-scale zinc–air pouch cells. Nat Energy (2021). https://doi.org/10.1038/s41560-021-00807-8

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