A high-energy-density and long-life lithium-ion battery via reversible oxide–peroxide conversion

Abstract

Li–O2 batteries have received considerable attention owing to their high theoretical gravimetric energy densities. However, the sluggish kinetic barrier between gaseous O2 and solid products leads to severe polarized overpotenial. Besides, the gas-open cell architecture and cumbrous O2 storage accessories bring additional burdens on practical application. Here, by pre-embedding Li2O nanoparticles into an iridium–graphene catalytic host, we confine the O2-free reversible Li2O/Li2O2 interconversion within a sealed cell environment. After rationally controlling the depth of charge, the O2/superoxo-free charge capacity can be extended to 400 mAh g–1 (based on the entire cathodic loading mass), with only 0.12 V round-trip overpotential. Ultrastable rechargeability can be achieved for over 2,000 cycles with 99.5% coulombic efficiency. Moreover, matched with a silicon anode, the full-cell output gravimetric energy density can reach nearly 600 Wh kg–1 (based on the loading mass of both electrodes). This work shows that reversible oxide–peroxide conversion can be utilized for the development of high-energy-density sealed battery technologies.

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Fig. 1: Schematic representations of oxygen-based beyond-intercalation Li battery systems.
Fig. 2: Characteristics of nano-Li2O embedded Iridium–rGO matrix.
Fig. 3: Characterization of the Li2O–Ir–rGO electrode during electrochemical transformation.
Fig. 4: Proposed reaction mechanism of Li2O oxidation.
Fig. 5: Rational charge/discharge depth for reversible Li2O/Li2O2 conversion on Li2O–Ir–rGO cathode.
Fig. 6: Cycling performance of half-cell (Li metal anode) and full-cell (Si anode) systems assembled with the Li2O–Ir–rGO cathode.

Data availability

All data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was partially supported by the National Basic Research Programme of China (grant no. 2016YFB0100203) and NSF of China (grant no. 21633003, U1801251). Financial support from the Advanced Low Carbon Technology Research and Development Programme, specially promoting research for innovative next-generation batteries (SPRING), from the Japan Science and Technology Agency is acknowledged. H.D. acknowledges scholarships from the China Scholarship Council. We thank Y. Sun (NIMS, Japan), Z. Chang (AIST, Japan) and X. Mu (Nanjing University, China) for their help in DEMS characterization, schematic cartoon production and general discussion.

Author information

Y.Q. and H.Z. contributed to the design of the research and performed the experimental data analysis. Y.Q. conducted the electrochemical and spectroscopic characterizations. K.J. performed the synthesis and assessment of the Ir–rGO cathodic substrate. H.D. performed the fabrication of both the Li2O-based cathode plate and related full-cell systems. All authors co-wrote the manuscript. H.Z. supervised the work. All authors discussed the results and commented on the manuscript.

Correspondence to Haoshen Zhou.

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Supplementary Information

Supplementary Discussion, Supplementary Figs. 1–25, Supplementary Tables 1–3 and Supplementary References.

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Qiao, Y., Jiang, K., Deng, H. et al. A high-energy-density and long-life lithium-ion battery via reversible oxide–peroxide conversion. Nat Catal 2, 1035–1044 (2019) doi:10.1038/s41929-019-0362-z

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