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Although lithium–oxygen batteries have attracted attention due to their extremely high energy densities, rational design, and critical evaluation of high-energy-density cathode for practical Li–O2 batteries is still urgently needed. Herein, the multiscale, angstrom-to-millimeter, precisely controllable synthesis of binder-free cathodes with minimally stacked graphene free from edge sites is demonstrated. The proposed Li–O2 battery, based on a hierarchically porous cathode with a practical mass loading of >4.0 mg cm−2, simultaneously exhibits an unprecedented specific areal (>30.0 mAh cm−2), mass (>6300 mAh g−1), and volumetric (>480 mAh cm−3) capacities. The battery displays the optimal energy density of 793 Wh kg−1 critically normalized to the total mass of all active materials including electrolytes and even discharge products Li2O2. Comprehensive in situ characterizations demonstrate a unique discharge mechanism in hierarchical pores which contributes to competitive battery performance. Superior rate performance in a current density range of 0.1 to 0.8 mA cm−2 and long-cycle stability (>260 cycles) at a current density of 0.4 mA cm−2, outperforming state-of-the-art carbon cathodes. This study yields insight into next-generation carbon cathodes, not only for use in practical Li–O2 batteries, but also in other metal–gas batteries with high energy densities.

Rights:

• Creative Commons BY-NC-ND Attribution-NonCommercial-NoDerivs 4.0 International
  

Keyword: lithium oxygen battery

Date published: 2023-11-10

Publisher: Wiley

Journal:

• Advanced Energy Materials (ISSN: 16146832) vol. 14 issue. 2 2303055

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Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1002/aenm.202303055

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Updated at: 2024-06-20 08:30:29 +0900

Published on MDR: 2024-06-20 08:30:29 +0900