Compared with lithium, magnesium shows a low propensity toward dendritic deposition due to its low surface self-diffusion barriers. However, due to the intrinsic surface roughness of the metal and the nonuniformity of the formed solid−electrolyte interphase, uneven deposition of Mg still happens, which brings about high local current density and continuous proliferation of the interphase, greatly exacerbating the passivation. Unfortunately, little attention has been paid to the deposition uniformity and the interfacial stability of Mg metal anodes, which result in a potential penalty. Herein, we modify the electrolyte with cathodically stable cations to guide smooth deposition via an electrostatic shielding strategy. The cations adsorbed on the initial protuberances effectively homogenize the charge flux by repulsing the incoming Mg 2+ away from the tips. Importantly, we prove the lateral growth can benefit the interphase stability and electrochemical reversibility.
Magnesium
ion batteries are a promising alternative of the lithium
counterpart; however, the poorly ion-conductive passivation layer
on Mg metal makes plating/stripping difficult. In addition to the
generally recognized chemical passivation, the interphase is dynamically
degraded by electrochemical side reactions. Especially under high
current densities, the interphase thickens, exacerbating the electrode
degradation. Herein, we adopt 3D Mg3Bi2 scaffolds
for Mg metal, of which the high surface area reduces the effective
current density to avoid continuous electrolyte decomposition and
the good Mg affinity homogenizes nucleation. The greatly alleviated
passivation layer could serve as a stable solid/electrolyte interface
instead. The symmetric cell delivers a low overpotential of 0.21 and
0.50 V at a current density of 0.1 and 4 mA cm–2, respectively, and a superior cycling performance over 300 cycles
at 0.5 mA cm–2 in a noncorrosive conventional electrolyte.
This work proves that the control of dynamic passivation can enable
high-power density Mg metal anodes.
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