阐明复合阳极在预锂化和常规充电过程中从石墨到硅的 "转移锂化"。

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ChemSusChem Pub Date : 2024-11-19 DOI:10.1002/cssc.202401290
Lars Frankenstein, Pascal Jan Glomb, Marvin Mohrhardt, Steffen Böckmann, Leon Focks, Aurora Gomez-Martin, Tobias Placke, Michael Ryan Hansen, Martin Winter, Johannes Kasnatscheew
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引用次数: 0

摘要

硅基阳极可以提高锂离子电池的比能量和能量密度。然而,由于体积引起的材料应力和容量损失,复合阳极中只能部分利用硅,通常与最先进的石墨一起使用,即所谓的硅/铬复合材料。在这项工作中,我们研究了各种硅纳米线(SiNWs),它们是这些复合材料中一种很有前景的硅结构,并通过预石墨化对其进行了改性。虽然带电的预石墨化阳极在初始循环中对 Li|Li+ 的电位低于 0 V,但它们并没有显示出金属锂的迹象,这很可能暗示了在从石墨化的 Gr 到 Si 的持续 "转移石墨化 "过程中引发的表面锂耗竭,通过核磁共振 (NMR)、X 射线衍射 (XRD) 和存储后放电过程中各自电压平台的容量变化,可以看出 LiC6 信号减少,LixSiy 信号增加。在带电状态下储存期间,开路电压稳定,随后的放电容量也相似,这表明不太可能存在自放电。最后,通过固态 7Li NMR,对不同硅形态(即无定形和结晶)以及钝化锂金属粉末(PLMP)预锂化过程中的转移锂化过程进行了验证。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Elucidating 'Transfer-Lithiation' from Graphite to Si within Composite Anodes during Pre-Lithiation and Regular Charging.

Si-based anodes can increase specific energy and energy density of Li ion batteries. However, the volume-induced material stress and capacity loss necessitates only a partial Si utilization within composite anodes, typically with state-of-the-art graphite, so called Si/Gr composites. In this work, various Si nanowires (SiNWs), a promising Si architecture for these composites, are investigated and modified via pre-lithiation. Though, charged pre-lithiated anodes show potentials below 0 V vs. Li|Li+ in the initial cycles, they do not show indications for metallic Li, which is likely a hint for a triggered surface Li depletion in course of a continuous "transfer-lithiation" from lithiated Gr to Si, which is indicated by decreasing LiC6 and increasing LixSiy signals via nuclear magnetic resonance (NMR), X-ray diffraction (XRD) as well as shifts in capacities of respective voltage plateaus during discharge after storage. A relevant contribution of self-discharge is unlikely as shown by a stable open-circuit-voltage during storage in charged state and similar subsequent discharge capacities, being consequently a hint for an intra-electrode capacity shift. The process of transfer lithiation is finally validated via solid-state 7Li NMR for varied Si morphology, i. e., amorphous and crystalline, as well as during pre-lithiation with passivated lithium metal powder (PLMP).

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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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