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Stabilizing Tin Anodes in Sodium-Ion Batteries by Alloying with Silicon
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-09-23 , DOI: 10.1021/acsaem.0c01641 Sayed Youssef Sayed 1 , W. Peter Kalisvaart 1 , Erik J. Luber 1 , Brian C. Olsen 1 , Jillian M. Buriak 1
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-09-23 , DOI: 10.1021/acsaem.0c01641 Sayed Youssef Sayed 1 , W. Peter Kalisvaart 1 , Erik J. Luber 1 , Brian C. Olsen 1 , Jillian M. Buriak 1
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Group IV of the periodic table is a promising column with respect to high capacity anode materials for sodium-ion batteries (SIBs). Unlike carbon which relies on interlayer defects, pores, and intercalation to store sodium, its heavier cousins—silicon, germanium, and tin—form binary alloys with sodium. Alloying does lead to the formation of high-capacity compounds, but they are, however, susceptible to large volumetric changes upon expansion that results in pulverization of the electrodes and poor cycling stability. Silicon and tin are particularly intriguing due to their high theoretical reversible capacities of 954 mAh/g (NaSi) and 847 mAh/g (Na15Sn4), respectively, but suffer from poor practical capacity and very short lifetimes, respectively. To buffer the detrimental effects of volume expansion and contraction, nanoscale multilayer anodes comprising silicon and tin films were prepared and compared with uniform films composed of atomically mixed silicon and tin as well as elemental silicon and tin films. The results reveal that the high capacity fade for elemental Sn is associated with detrimental anodic (desodiation) reactions at a high cutoff voltage with a threshold defined as ∼0.8 VNa. Binary mixtures of Si and Sn were tested in a number of different architectures, including multilayer films and cosputtered films with varying volume ratios of both elements. All mixed films showed improved capacity retention compared to the performance of anodes comprising only elemental Sn. A multilayer structure composed of 3 nm thick silicon and tin layers showed the highest Coulombic efficiency and retained 97% of its initial capacity after 100 cycles, which is vastly improved compared to 7% retention observed for the elemental Sn film. The alloying element, Si, plays two roles: it stabilizes grain growth/pulverization and also alters the surface chemistry of the anodes, thus affecting the formation of solid electrolyte interphase.
中文翻译：
通过与硅合金化来稳定钠离子电池中的锡阳极
关于钠离子电池（SIB）的高容量负极材料，元素周期表的第IV组是很有希望的一栏。与碳依赖于层间缺陷，孔隙和插层来存储钠的碳不同，碳的较重表亲（硅，锗和锡）与钠形成二元合金。合金化的确导致了高容量化合物的形成，但是，它们在膨胀时容易受到大体积变化的影响，这会导致电极粉化和较差的循环稳定性。硅和锡特别引人入胜，因为它们具有954 mAh / g（NaSi）和847 mAh / g（Na 15 Sn 4），但是它们分别具有较差的实用能力和非常短的使用寿命。为了缓冲体积膨胀和收缩的不利影响，制备了包含硅和锡膜的纳米级多层阳极，并将其与由原子混合的硅和锡以及元素硅和锡膜组成的均匀膜进行比较。结果表明，元素Sn的高容量衰减与在高截止电压（阈值定义为〜0.8 V Na）下的有害阳极（脱氧）反应有关。。Si和Sn的二元混合物已在多种不同的体系结构中进行了测试，包括多层膜和两种元素的体积比均不同的共溅射膜。与仅包含元素锡的阳极性能相比，所有混合膜均显示出改进的容量保持率。由3 nm厚的硅和锡层组成的多层结构显示出最高的库仑效率，并在100次循环后保留了其初始容量的97％，相比于元素Sn膜的7％保留率，它得到了极大的改善。Si合金元素起两个作用：稳定晶粒生长/粉碎，还改变阳极的表面化学性质，从而影响固体电解质中间相的形成。
更新日期：2020-10-26
中文翻译：
通过与硅合金化来稳定钠离子电池中的锡阳极
关于钠离子电池（SIB）的高容量负极材料，元素周期表的第IV组是很有希望的一栏。与碳依赖于层间缺陷，孔隙和插层来存储钠的碳不同，碳的较重表亲（硅，锗和锡）与钠形成二元合金。合金化的确导致了高容量化合物的形成，但是，它们在膨胀时容易受到大体积变化的影响，这会导致电极粉化和较差的循环稳定性。硅和锡特别引人入胜，因为它们具有954 mAh / g（NaSi）和847 mAh / g（Na 15 Sn 4），但是它们分别具有较差的实用能力和非常短的使用寿命。为了缓冲体积膨胀和收缩的不利影响，制备了包含硅和锡膜的纳米级多层阳极，并将其与由原子混合的硅和锡以及元素硅和锡膜组成的均匀膜进行比较。结果表明，元素Sn的高容量衰减与在高截止电压（阈值定义为〜0.8 V Na）下的有害阳极（脱氧）反应有关。。Si和Sn的二元混合物已在多种不同的体系结构中进行了测试，包括多层膜和两种元素的体积比均不同的共溅射膜。与仅包含元素锡的阳极性能相比，所有混合膜均显示出改进的容量保持率。由3 nm厚的硅和锡层组成的多层结构显示出最高的库仑效率，并在100次循环后保留了其初始容量的97％，相比于元素Sn膜的7％保留率，它得到了极大的改善。Si合金元素起两个作用：稳定晶粒生长/粉碎，还改变阳极的表面化学性质，从而影响固体电解质中间相的形成。
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