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.
The authors declare no competing interests
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Supplementary Figures 1–40, Supplementary Tables 1–3, Supplementary Notes 1–2, Supplementary References
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
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
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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Li, G., Liu, Z., Huang, Q. et al. Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects. Nat Energy 3, 1076–1083 (2018). https://doi.org/10.1038/s41560-018-0276-z
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