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Synthesis of a metallic mesoporous pyrochlore as a catalyst for lithium–O2 batteries

Nature Chemistry volume 4, pages 1004–1010 (2012)Cite this article

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Abstract

The lithium–O2 ‘semi-fuel’ cell based on the reversible reaction of Li and O2 to form Li2O2 can theoretically provide energy densities that exceed those of Li-ion cells by up to a factor of five. A key limitation that differentiates it from other lithium batteries is that it requires effective catalysts (or ‘promoters’) to enable oxygen reduction and evolution. Here, we report the synthesis of a novel metallic mesoporous oxide using surfactant templating that shows promising catalytic activity and results in a cathode with a high reversible capacity of 10,000 mAh g−1 (∼1,000 mAh g−1 with respect to the total electrode weight including the peroxide product). This oxide also has a lower charge potential for oxygen evolution from Li2O2 than pure carbon. The properties are explained by the high fraction of surface defect active sites in the metallic oxide, and its unique morphology and variable oxygen stoichiometry. This strategy for creating porous metallic oxides may pave the way to new cathode architectures for the Li–O2 cell.

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Figure 1: Synthesis and structure of MP lead ruthenium pyrochlore.
Figure 2: Electrochemical characteristics and XRD patterns of the electrochemical discharge products from the Li–O2 battery.
Figure 3: Schematic of the proposed MP pyrochlore catalyst mechanism in the Li–air cell.
Figure 4: Electrocatalytic oxidation of Li2O2 and corresponding XRD pattern of the charged electrode.

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Acknowledgements

The authors acknowledge the Natural Sciences and Engineering Council of Canada for support through its Strategic, Discovery, and Canada Research Chair programmes.

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Authors and Affiliations

  1. Department of Chemistry, University of Waterloo, Waterloo, N2L 3G1, Ontario, Canada

    Si Hyoung Oh, Robert Black, Ekaterina Pomerantseva, Jin-Hyon Lee & Linda F. Nazar

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  1. Si Hyoung Oh
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Contributions

S.H.O. and L.F.N. developed the concept and designed the experiments. S.H.O. carried out the experimental work. R.B. and E.P. helped with the design and experiments, as well as the SEM imaging. J.H.L. contributed to some experiments involving characterization and electrochemistry.

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Correspondence to Linda F. Nazar.

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Oh, S., Black, R., Pomerantseva, E. et al. Synthesis of a metallic mesoporous pyrochlore as a catalyst for lithium–O2 batteries. Nature Chem 4, 1004–1010 (2012). https://doi.org/10.1038/nchem.1499

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