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Nanomaterials 2021, 11, 810 17 of 29 alloys was very high, approximatively 99% after 30 cycles, because of the highly reversible behaviour of the two phases of bismuth and tin (Figure 11C). Table 5. Performances of Mg cells assembled with NP-Bi6Sn4 anode, with a focus on the contribution of each metal at different stages of the charge/discharge experiments. Contribution of Bi to Initial Specific Capacity 248 mAh g−1 Contribution of Bi to Specific Capacity at the 200th Cycle 154 mAh g−1 Percentage of Capacity Fading of Bi 37.9% Contribution of Sn to Initial Specific Capacity 164 mAh g−1 Contribution of Sn to Specific Capacity at the 200th Cycle 126 mAh g−1 Percentage of Capacity Fading of Sn 22.7% The chemical processes occurring within the electrode during charge and discharge are sketched in Figure 11E, and can be summarized as follows. During discharge (alloying), at first magnesium ions reacted with bismuth to form Mg3Bi2, while the unreacted tin behaved as a buffer matrix mitigating volume expansion. Then, magnesium ions reacted with tin and the previously formed Mg3Bi2 played the role of preventing further volume expansion. The dual phase unlocked the potential properties of tin, that otherwise would be characterized by poor kinetics and low electrochemical reactivity. Meanwhile, Mg3Bi2 acted as a superionic conductor [160], accelerating the magnesium ions transport and explaining the better rate performances of NP-Bi6Sn4, in which the bismuth phase was dominant. During the first charge (dealloying) process, magnesium ions were extracted from the electrode, bringing to formation of smaller-sized bismuth and tin nanocrystals. While the process occurred, Mg3Bi2 and tin served as a buffer matrix to prevent large volume shrinkage. Formation of the buffer matrix during charge and discharge, the unlocked potential of tin and the behaviour of Mg3Bi2 as a superionic conductor, combined with the effects of the porous structure and the increased density of grain/phase boundaries, explained all the good properties provided by the dual-phase bismuth–tin alloys [170]. 4.4. Titanium-Based Anodes Titanium-based anodic materials have been extensively studied for lithium- and sodium-based batteries [171–175], together with a broad examination of nanostructures and morphologies able to guarantee mechanical stability, high performance, ease of preparation on metal supports and efficient charge transport in one-dimensional materials. However, studies on titanium-based anodes in the field of MIBs are still few and the scientific community started publishing the first results in 2020. Luo et al. proposed layered sodium trititanate (Na2Ti3O7) and sodium hexatitanate (Na2Ti6O13) nanowires (NWs) as anodes for MIBs [176]; they were prepared by heat treat- ment of the titanate precursor under different washing conditions. The investigation highlighted that passing from the layered Na2Ti3O7 morphology to a more condensate three-dimensional microporous structure in Na2Ti6O13 boosted the magnesium ions stor- age performance. The two electrodes exhibited a NWs-based morphology (Figure 12A,B); transmission electron microscopy (TEM) images showed that Na2Ti3O7 displayed a large interlayer spacing of 0.84 nm, while for Na2Ti6O13 was equal to 0.75 nm. Overall, the interlayer distance was rather large, enough to guarantee an efficient magnesium ions storage and diffusion. Na2Ti6O13-based cells achieved initial discharge and charge capac- ity of 165.8 and 147.7 mAh g−1, respectively, at 10 mA g−1, with an outstanding initial coulombic efficiency of 89.1% (Figure 12C). The electrochemical reaction mechanism was investigated through different techniques, from which it emerged that the inserted magne- sium ions replaced the sites of sodium ions to form Mg–Ti–O. In this system, sodium ions could not reinsert into the structure because of the formation of insoluble NaCl particles. Such an irreversible structure change and NaCl salt formation led to a rapid worsening of Na2Ti3O7-based cells specific capacity values. On the other hand, Na2Ti6O13, with its regular three dimensional and microporous structure based on TiO6 octahedra, guaranteed better structural stability during the magnesium ions insertion and extraction processes.PDF Image | Overview on Anodes for Magnesium Batteries
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