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NATURE COMMUNICATIONS | https://doi.org/10.1038/s41467-020-20334-6 ARTICLE and the reflected images of the electrode surface were obtained. The setup diagram is shown in Fig. 3a. The imaging area was 200–400 μm away from the top elec- trode’s projection. Different current densities (5–80 mA cm−2) were applied, and four electrolytes (Electrolyte 1: 2 M ZnSO4 in seawater; Electrolyte 2: 2 M ZnSO4 with 0.1 M MnSO4 in seawater; Electrolyte 3: 2 M ZnSO4 with 0.1 M MnSO4 in DI water; Electrolyte 4: 2 M ZnSO4 in DI water) were tested to investigate the Zn plating process. To compare with the 3D Zn-Mn alloy, a pristine Zn foil anode was also tested in Electrolyte 2. After the Zn plating, the current density of 80 mA cm−2 was used to analyze the stripping process of the 3D Zn-Mn anode. DFT calculations. Density functional theory (DFT) simulation was conducted to analyze the adsorption and kinetics of Zn ad-atoms on the experimentally con- firmed Zn3Mn (110) surface. For the simplicity and the efficiency of the calculation, the simulation was conducted on the cubic cell to extract the effect of Mn sub- stitution alone. The simulation model was constructed with 40 Zn and 16 Mn atoms in a unit cell of 1.08 × 0.76 × 2.08 nm. The x, y, and z directions of the cell correspond to [001], [1–10], and [110] crystal orientation, respectively. A vacuum layer of 1.2 nm was included in the z-direction to avoid the interaction from the neighboring cells in a periodic boundary condition. Vienna Ab-initio Simulation Package (VASP) was used in the calculation63,64, with projector augmented wave (PAW) pseudopotential65,66 and generalized gradient approximation by Perdew- Burke-Ernzerhof67. The plane wave energy cut off was 400 eV and 3 × 5 × 1 k-points were selected based on the Monkhorst-Pack method68. First, the conjugate gradient structure optimization was performed while fixing the atoms in the bottom two layers. Then, a Zn atom was placed on the surface at 10 × 10 grid points and structural optimization was performed. Here only the ad-atom was relaxed in z-direction while fixing the x and y coordinates. Also, a Zn ad-atom was placed on a surface lattice point and structure optimization was conducted to calculate the binding energy. The binding energy calculation was also performed on the Zn (110) surface for comparison. The binding energies were calculated by the (total energy of the system w/o Zn ad-atom) + (isolated Zn atom) – (total energy of the model w/ Zn ad-atom). Data availability The data that support the findings of this study are available from the corresponding author upon reasonable request. Received: 9 October 2020; Accepted: 26 November 2020; References 1. Armand, M. & Tarascon, J. M. Building better batteries. Nature 451, 652–657 (2008). 2. Pan, H. L. et al. Reversible aqueous zinc/manganese oxide energy storage from conversion reactions. Nat. Energy 1, 16039 (2016). 3. 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