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Interconnected hollow carbon nanospheres for stable lithium metal anodes

Abstract

For future applications in portable electronics, electric vehicles and grid storage, batteries with higher energy storage density than existing lithium ion batteries need to be developed. Recent efforts in this direction have focused on high-capacity electrode materials such as lithium metal, silicon and tin as anodes, and sulphur and oxygen as cathodes. Lithium metal would be the optimal choice as an anode material, because it has the highest specific capacity (3,860 mAh g–1) and the lowest anode potential of all. However, the lithium anode forms dendritic and mossy metal deposits, leading to serious safety concerns and low Coulombic efficiency during charge/discharge cycles. Although advanced characterization techniques have helped shed light on the lithium growth process, effective strategies to improve lithium metal anode cycling remain elusive. Here, we show that coating the lithium metal anode with a monolayer of interconnected amorphous hollow carbon nanospheres helps isolate the lithium metal depositions and facilitates the formation of a stable solid electrolyte interphase. We show that lithium dendrites do not form up to a practical current density of 1 mA cm–2. The Coulombic efficiency improves to 99% for more than 150 cycles. This is significantly better than the bare unmodified samples, which usually show rapid Coulombic efficiency decay in fewer than 100 cycles. Our results indicate that nanoscale interfacial engineering could be a promising strategy to tackle the intrinsic problems of lithium metal anodes.

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Figure 1: Schematic diagrams of the different Li anode structures.
Figure 2: Fabrication of hollow carbon nanosphere-coated electrode.
Figure 3: Li deposition on a Cu substrate with and without carbon nanosphere modification.
Figure 4: Electrochemical characterization of the electrodes for Li deposition/dissolution.

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Acknowledgements

G.Z. acknowledges financial support from Agency for Science, Technology and Research (A*STAR), Singapore. The authors thank A. Jaffe for help with the Fourier transform infrared measurement and H. Yuan for help with the conductivity measurements. H.L. was supported by the Basic Science Research Program through the National Research Foundation of Korea (contract no. NRF-2012R1A6A3A03038593).

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G.Z and Y.C. conceived and designed the experiments. G.Z performed the experiments. S.W.L. performed the numerical simulation and provided data analysis. H.W.L. conducted in situ TEM characterization. G.Z. 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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Zheng, G., Lee, S., Liang, Z. et al. Interconnected hollow carbon nanospheres for stable lithium metal anodes. Nature Nanotech 9, 618–623 (2014). https://doi.org/10.1038/nnano.2014.152

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