Title: Mechanism of Li nucleation at graphite anodes and mitigation strategies
Authors: Peng, Chao
Bhandari, Arihant
Dziedzic, Jacek
Owen, John R.
Skylaris, Chris-Kriton
Kramer, Denis 
Language: en
Subject (DDC): DDC::500 Naturwissenschaften und Mathematik::540 Chemie::541 Physikalische Chemie
Issue Date: 20-Jul-2021
Publisher: Royal Society of Chemistry
Document Type: Article
Journal / Series / Working Paper (HSU): Journal of materials chemistry A 
Volume: 9
Issue: 31
Page Start: 16798
Page End: 16804
Publisher Place: London [u.a.]
Lithium metal plating is a critical safety issue in Li-ion cells with graphite anodes, and contributes significantly to ageing, drastically limiting the lifetime and inducing capacity loss. Nonetheless, the nucleation mechanism of metallic Li on graphite anodes is still poorly understood. But in-depth understanding is needed to rationally design mitigation measures. In this work, we conducted First-Principles studies to elucidate the Li nucleation mechanism on graphite surfaces. These large-scale density-functional-theory (DFT) calculations indicate that nano-particulate Li forms much more readily than classical nucleation theory predicts. Further, our calculations indicate a crucial role of topological surface states near the zigzag edge, lowering the nucleation barrier by a further 1.32 eV relative to nucleation on the basal plane. Li nucleation, therefore, is likely to initiate at or near the zigzag edges of graphitic particles. Finally, we suggest that chemical doping with a view to reducing the effect of the topological surface states might be a potential mitigation strategy to increase nucleation barriers and reduce the propensity to plate Li near the zigzag edge.
Organization Units (connected with the publication): Computational Material Design 
ISSN: 2050-7488
DOI: 10.1039/D1TA03447B
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