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Nanomaterials 2021, 11, 810 9 of 29 4.1. Bismuth-Based Anodes Bismuth-based anodes are among the most studied alternative anodes, due to the rhombohedral crystalline structure of bismuth that allows formation of alloys with high volumetric capacity [158]. The gravimetric capacity theoretically achievable is also high, about 385 mAh g−1, hypothesizing the transfer of six electrons and the formation of the alloy according to the following reaction [159]: 2Bi+3Mg2+ +6e− →Mg3Bi2 (1) An interesting superionic conductivity of magnesium ions in β-Mg3Bi2 has been shown [160]. The electrochemical behaviour of this alloy and some of its derivatives was studied by Matsui et al. [158], by adopting bismuth, antimony and Bi1−xSbX alloys at different stoichiometries as anode materials for MIBs. Antimony showed very poor cycling performances, but bismuth and Bi0.88Sb0.12 alloy exhibited impressive results at a current density corresponding to 1C (see Table 3). The capacity fading detected by the authors was probably due to losses of electrical contact caused by periodic volume change of the anode during cycling. Table 3. Performances of Mg cells assembled with Bi and Bi0.88Sb0.12 anodes. Maximum Specific Capacity (mAh g−1) Bi 257 Bi0.88 Sb0.12 298 Specific Capacity at the 100th Cycle (mAh g−1) 222 215 Shao et al. studied the electrochemical characteristics of bismuth nanotubes (NTs), synthesized by hydrothermal reaction [161]. The purpose was to reduce the diffusion length of magnesium ions in order to mitigate the kinetic hurdles that exist in alternative anode materials. The experiments were conducted for both bismuth NTs and microparticles, in Mg(BH4)2 + LiBH4 diglyme electrolytes. Figure 7 displays the cyclic voltammograms (CV), the discharge/charge profile and the rate/cycling performances of the cells assembled by Shao et al. The results clearly showed superior performances in the case of a bismuth nanostructured anode, especially at high C rates (Figure 7c). At 5C, the specific capacity was 216 mAh g−1 for bismuth NTs vs. 51 mAh g−1 for bismuth microparticles. The former also showed narrower peaks and lower overpotential (Figure 7A), together with a faster response. At low C rates, i.e., between C/20 and C/2, the performances of the two structures were almost comparable. Furthermore, bismuth NTs were studied in a full cell setup, by choosing Mo6Se8 as cathode and an electrolyte consisting of Mg(TFSI)2 0.4 M in diglyme. A mid-point discharge voltage of about 0.75 V and a specific capacity of 90 mAh g−1 were observed. The full cell also exhibited a 92.3% capacity retention after 200 cycles (Figure 7D). X-ray diffraction (XRD) analysis confirmed the high reversibility of magnesium ions insertion. A weakness, though, was the large voltage hysteresis between magnesium alloying and dealloying, which resulted in energy losses. Other drawbacks were the exotic nature of the anodic material and its manufacturing costs, which made it difficult to be used in large scale commercial systems [110].PDF Image | Overview on Anodes for Magnesium Batteries
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