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Magnesium alloys are a promising anode material for high-energy density lithium metal batteries. Nevertheless, the cycling stability of such magnesium anodes in conjunction with Ni layered oxide cathodes is limited by the formation of Mg dendrites that can penetrate the separator and lead to internal short-circuits. Using molecular simulations, we have identified a magnesium concentration in an alloying range that effectively controls the plating and stripping of lithium atoms on the Mg anode surface and thus improves cycling performance.

Lithium is the most abundant alkali metal and is found in nature as lithium oxide (LiO), lithium carbonate (LiCl), and in several magnesium minerals including MgSO48H2O and Mg(NO3)2. The addition of lithium to the Mg lattice decreases the density of the alloys and results in a structural phase transition from close-packed hexagonal (hcp) to body-centered cubic (bcc) structure [1,2]. This change reduces the stress on the alloys during deformation and enhances their plasticity, and the bcc phase also increases their resistance to oxidation.

Another benefit of magnesium is its reactivity to the electrolyte, which enables Mg to exhibit a relatively low standard electrode potential of -3.040 V vs. SHE in cyclic voltammetry experiments. This is in contrast to pure Li, which has a significantly higher negative electrode potential and suffers from uncontrolled dendrite growth, leading to poor Coulombic efficiency.

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