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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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.
The authors declare no competing interests.
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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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