Layered reduced graphene oxide with nanoscale interlayer gaps as a stable host for lithium metal anodes

Abstract

Metallic lithium is a promising anode candidate for future high-energy-density lithium batteries. It is a light-weight material, and has the highest theoretical capacity (3,860 mAh g–1) and the lowest electrochemical potential of all candidates. There are, however, at least three major hurdles before lithium metal anodes can become a viable technology: uneven and dendritic lithium deposition, unstable solid electrolyte interphase and almost infinite relative dimension change during cycling. Previous research has tackled the first two issues, but the last is still mostly unsolved. Here we report a composite lithium metal anode that exhibits low dimension variation (20%) during cycling and good mechanical flexibility. The anode is composed of 7 wt% ‘lithiophilic’ layered reduced graphene oxide with nanoscale gaps that can host metallic lithium. The anode retains up to 3,390 mAh g–1 of capacity, exhibits low overpotential (80 mV at 3 mA cm–2) and a flat voltage profile in a carbonate electrolyte. A full-cell battery with a LiCoO2 cathode shows good rate capability and flat voltage profiles.

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Figure 1: Fabrication of a layered Li–rGO composite film.
Figure 2: Characterization of the materials.
Figure 3: Li deposition behaviour and in situ characterization.
Figure 4: Electrochemical characterization of the Li–rGO electrodes.
Figure 5: Electrochemical performance of the LCO/Li–rGO cells.

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Acknowledgements

Y.C. acknowledges the support from the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy under the Battery Materials Research (BMR) program.

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D.L., Y.L. and Y.C. conceived the idea and experiments. D.L. and Y.L. carried out the synthesis and performed the materials characterizations and electrochemical measurements. Z.L. assisted the electrochemical measurements. H.W.L. conducted in situ TEM characterization. J.S. performed the first-principles calculations. H.W. and K.Y. assisted in the Raman and XPS measurement. J.X. assisted the XPS analysis. D.L., Y.L. and Y.C. co-wrote the paper. All authors discussed the results and commented on the manuscript.

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Correspondence to Yi Cui.

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The authors declare no competing financial interests.

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Lin, D., Liu, Y., Liang, Z. et al. Layered reduced graphene oxide with nanoscale interlayer gaps as a stable host for lithium metal anodes. Nature Nanotech 11, 626–632 (2016). https://doi.org/10.1038/nnano.2016.32

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