Abstract
Zn/MnO2 batteries, driven by a dual deposition reaction, are a prominent avenue for achieving high energy density in aqueous systems. Introducing an initially dual-electrode-free (anode/cathode) configuration can further boost energy density to over 200 Wh kg−1, but with limited cycle life due to the poor reversibility of Zn/MnO2 deposition and stripping. Drawing inspiration from soft templating strategies in material synthesis, here we apply this approach to electrodeposition and stripping by designing an in situ formed liquid crystal interphase. This concept is achieved by incorporating just 0.1 mM of surfactant molecules into the electrolyte, which induces favourable c-axis orientations in depositing both hexagonal Zn and MnO2. This enhancement subsequently increases the deposition/stripping reversibility and promotes the cycle life of the dual-electrode-free battery, achieving 80% capacity retention after ~950 cycles. This liquid crystal interphase chemistry also holds great promise for regulating deposition in other crystal systems, opening an exciting research direction for next-generation high-energy-density and long-duration energy storage based on aqueous chemistries.
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Acknowledgements
This work is supported by the Aqueous Battery Consortium, an energy innovation hub under the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering. We also acknowledge the use and support of the Stanford Nano Shared Facilities and the Stanford Nanofabrication Facility and the use of the computer time allocation m2997 at the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under contract number DE-AC02-05CH11231. Y.C. acknowledges cryo-EM support from the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering under contract DE-AC02-76SF00515. M.B. acknowledges support by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, Catalysis Science Program, to the SUNCAT Center for Interface Science and Catalysis.
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Y.L. and Y.C. (corresponding author) conceived the project and designed the experiments. Y.L. performed electrochemical measurements and soft matter characterizations. Y.L. and X.X. performed SEM and XRD experiments. E.Z.C. and M.B. carried out DFT calculations. W.L. carried out two-dimensional computation. Y.C. carried out cryo-(S)TEM experiments. Y.Y. performed XPS experiments. All authors discussed the results and commented on the manuscript.
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Li, Y., Zheng, X., Carlson, E.Z. et al. In situ formation of liquid crystal interphase in electrolytes with soft templating effects for aqueous dual-electrode-free batteries. Nat Energy 9, 1350–1359 (2024). https://doi.org/10.1038/s41560-024-01638-z
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DOI: https://doi.org/10.1038/s41560-024-01638-z
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