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Nanomaterials 2021, 11, 810 12 of 29 Finally, tin offers better performances in terms of recycling than bismuth, as shown in Figure 4 (tin > 50%, bismuth < 1%). One of the first studies on this topic was that of Singh et al., based on tin powder films for insertion anodes [165]. By plotting galvanostatic charge–discharge curves for both tin- and bismuth-based anodes at a low current density of C/500 in an organo-haloaluminate electrolyte, the superior electrochemical performances of tin were put in light. The insertion potential into tin anode was found to be equal to 0.15 V vs. Mg2+/Mg, against 0.23 V vs. Mg2+/Mg for the bismuth anode, and a hysteresis between insertion and de-insertion of 50 mV was observed for tin, much lower than that of 90 mV for bismuth. The tin anode showed an initial impressive specific capacity of 903 mAh g−1, but, unfortunately, the discharge process revealed to be highly irreversible, with a sharp reduction in reversible capacity (Figure 8B). Rate capability measurements also showed that, at rates above C/500, the specific capacity of the tin anode rapidly decreased. This was possibly due to a poor insertion kinetics of the tin anode, even though the Coulombic efficiency seemed to increase with the charge–discharge rate. The sharp reduction of initial capacity was also observed in full cell setups, with Mg(TFSI)2 0.5 M in DME/organohaloaluminate electrolyte and Mo6S8 cathode. The resulting electrochemical performances were quite similar for both systems: 82 mAh g−1 at the first cycle, followed by a stable value of less than 50 mAh g−1 for the following ones [165]. Beyond pure tin, some tin-based compounds were also studied. Cheng et al., for example, focused on a tin–antimony alloy by means of a combined computational and experimental approach [166]. In their first study, they discovered that, during the first cycle, an irreversible process led to the formation of a porous structure composed of antimony- rich and pure tin sub-structures. After this initial phase (conditioning), they observed that the nanosized tin particles had a highly reversible behaviour, while the antimony- rich zones showed low Coulombic efficiency due to trapping. Thus, the antimony-rich zones lowered the specific capacity of the anode, but they seemed to be necessary to reach formation of stable tin nanoparticles [166]. Another study focused on the behaviour of the tin–antimony alloy after conditioning led to the conclusion that the alloy had superior properties than that of pure tin [167]. Overall, the advantages of the tin–antimony alloy can be summarized as follows: (1) improved kinetics for magnesiation/demagnesiation result in lower overpotentials (Figure 9A); (2) improved specific capacity at the same current density (420 mAh g−1 vs. less than 300 mAh g−1 for pure tin at a 50 mA g−1) (Figure 9B); (3) excellent rate capability with 70% capacity retention (300 mA g−1 at very high current densities of 1000 mA g−1 (Figure 9C); (4) good cyclability, with 270 mAh g−1 after 200 cycles at a current density of 500 mA g−1 (Figure 9D). Wang et al. used density functional theory (DFT) calculations to study magnesium cation diffusion properties in β- and α-Sn. They found a diffusion barrier for an isolated magnesium atom of 0.395 eV in the α-Sn and of 0.435 eV in the β-Sn. Moreover, a higher magnesium concentration decreased the diffusion barrier in the case of α-Sn, while an opposite behaviour was expected for β-Sn. Thus, the α form of tin seemed to represent a better alternative than the β phase as an anode material for MIBs [168].PDF Image | Overview on Anodes for Magnesium Batteries
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