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Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects

Nature Energyvolume 3pages10761083 (2018) | Download Citation


The cycle life and energy density of rechargeable metal batteries are largely limited by the dendritic growth of their metal anodes (lithium, sodium or zinc). Here we develop a three-dimensional cross-linked polyethylenimine lithium-ion-affinity sponge as the lithium metal anode host to mitigate the problem. We show that electrokinetic surface conduction and electro-osmosis within the high-zeta-potential sponge change the concentration and current density profiles, which enables dendrite-free plating/stripping of lithium with a high Coulombic efficiency at high deposition capacities and current densities, even at low temperatures. The use of a lithium-hosting sponge leads to a significantly improved cycling stability of lithium metal batteries with a limited amount of lithium (for example, the areal lithium ratio of negative to positive electrodes is 0.6) at a commercial-level areal capacity. We also observed dendrite-free morphology in sodium and zinc anodes, which indicates a broader promise of this approach.

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The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

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This material is based on work supported by the Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technology Office, under Award no. DE-EE0007795 (experimental work) and DE-EE0007803 (modelling work). The authors appreciate T. Stecko at The Pennsylvania State University for the analysis of MCT data.

Author information


  1. Department of Mechanical and Nuclear Engineering, The Pennsylvania State University, University Park, PA, USA

    • Guoxing Li
    • , Daiwei Wang
    •  & Donghai Wang
  2. Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, USA

    • Zhe Liu
    • , Qingquan Huang
    •  & Long-Qing Chen
  3. Department of Chemistry, The Pennsylvania State University, University Park, PA, USA

    • Yue Gao
  4. Department of Chemical Engineering, The Pennsylvania State University, University Park, PA, USA

    • Michael Regula


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G.L. and Do.W. conceived and designed the experiments. G.L. performed the laboratory experiments, characterization of materials and analysis of the results. Z.L. performed the simulation. Z.L. and L.C. proposed the explanation for the simulation. Y.G. performed the XPS measurements. G.L. and Do.W. prepared the manuscript and all the authors discussed the results and commented on the manuscript.

Competing interests

The authors declare no competing interests

Corresponding author

Correspondence to Donghai Wang.

Supplementary information

  1. Supplementary Information

    Supplementary Figures 1–40, Supplementary Tables 1–3, Supplementary Notes 1–2, Supplementary References

  2. Supplementary Video 1

    The MCT data of 3D PPS shows that the pores in 3D PPS have a high interconnectivity. The interconnected pores account for 99.99% of the total pore volume. Red represents isolated pores and white represents sponge walls in the video. The free-standing and thick 3D PPS samples were prepared using the same experimental conditions with 3D PPS@Cu for the characterization

  3. Supplementary Video 2

    The electro-osmosis pumps the electrolyte to flow from negative to positive through the cross-linked branched PEI modified plastic microtube (inner diameter: 850 µm, length: 1.8 cm). The movie speed is quadrupled

  4. Supplementary Video 3

    The un-modified plastic microtube (inner diameter: 850 µm, length: 1.8 cm) cannot provide the electro-osmosis. The movie speed is quadrupled

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