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A high-rate and long-life organic–oxygen battery

Abstract

Alkali metal–oxygen batteries promise high gravimetric energy densities but suffer from low rate capability, poor cycle life and safety hazards associated with metal anodes. Here we describe a safe, high-rate and long-life oxygen battery that exploits a potassium biphenyl complex anode and a dimethylsulfoxide-mediated potassium superoxide cathode. The proposed potassium biphenyl complex–oxygen battery exhibits an unprecedented cycle life (3,000 cycles) with a superior average coulombic efficiency of more than 99.84% at a high current density of 4.0 mA cm−2. We further reduce the redox potential of biphenyl by adding the electron-donating methyl group to the benzene ring, which successfully achieved a redox potential of 0.14 V versus K/K+. This demonstrates the direction and opportunities to further improve the cell voltage and energy density of the alkali-metal organic–oxygen batteries.

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Fig. 1: Electrochemical characterization of the representative aromatic hydrocarbons and schematics of the organic–oxygen battery.
Fig. 2: Performance comparison between the K metal anode and the BpK anode in both O2 full-cell and symmetric-cell configurations.
Fig. 3: Rate capability and cycle life of the BpK–O2 cell.
Fig. 4: Analysis of the CE evolution of the BpK–O2 cell at early cycling stage.
Fig. 5: Characterization of discharge product.
Fig. 6: Effect of methylation on the redox potentials of the Bp molecule.

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Data supporting the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

The work described in this paper was supported by the Research Grant Council of the Hong Kong Administrative Region, China, under the Theme-based Research Scheme through Project T23-60I/17-R and General Research Fund CUHK 14207517. The authors are grateful to Y. Wang for assisting with the OEMS measurements.

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Authors

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G.C. and Y.-C.L. conceived the project, analysed the data and wrote the manuscript. G.C. performed the density functional theory calculation and conducted the experiments with contributions from W.W. (cell and electrolyte design), N.-C.L. (BpK titration and SEM/EDX measurements) and Z.L. (OEMS and Fenton’s reagent tests).

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Correspondence to Yi-Chun Lu.

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Supplementary Information

Supplementary Figures 1–20, Supplementary Tables 1–2, Supplementary Notes 1–4, Supplementary Video Captions 1–2, Supplementary References 1–25

Supplementary Video 1

Reaction of K metal and BpK with bulk water.

Supplementary Video 2

Reaction of K metal and BpK with bulk DMSO.

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Cong, G., Wang, W., Lai, NC. et al. A high-rate and long-life organic–oxygen battery. Nat. Mater. 18, 390–396 (2019). https://doi.org/10.1038/s41563-019-0286-7

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