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Issue 40, 2018
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Mechanistic insight into dendrite–SEI interactions for lithium metal electrodes

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Abstract

The stability and homogeneity of the solid electrolyte interphase (SEI) layer are critical toward understanding the root causes behind performance decay and safety concerns with lithium metal electrodes for energy storage. This study focuses on deducing mechanistic insights into the complexations between the Li metal electrode and SEI during electrodeposition. It is found that the formation of Li dendrite can be initiated by two distinct mechanisms: (i) aggressive Li-ion depletion near the anode–SEI interface at high reaction rates or low temperature attributed to transport limitations, and (ii) spatially varying reaction kinetics at the SEI–electrode interface due to SEI inhomogeneity even at low currents. Subsequent mechanical stability analyses reveal that significantly high stress is generated due to nonuniform Li electrodeposition which could lead to crack formation in the existing SEI layer, and consequently exposure of fresh lithium to the electrolyte resulting in enhanced capacity fading. Furthermore, a non-dimensional analysis relating the interfacial stress induced failure propensity to electrochemical Biot number and SEI heterogeneity factor is proposed, which delineates stable lithium deposition regimes.

Graphical abstract: Mechanistic insight into dendrite–SEI interactions for lithium metal electrodes

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Publication details

The article was received on 17 Aug 2018, accepted on 25 Sep 2018 and first published on 25 Sep 2018


Article type: Paper
DOI: 10.1039/C8TA07997H
Citation: J. Mater. Chem. A, 2018,6, 19664-19671

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    Mechanistic insight into dendrite–SEI interactions for lithium metal electrodes

    F. Hao, A. Verma and P. P. Mukherjee, J. Mater. Chem. A, 2018, 6, 19664
    DOI: 10.1039/C8TA07997H

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