Modeling solid-electrolyte interfacial phenomena in silicon anodes

Soto, FA; Hoz, JM Martinez de la; Seminario, JM; Pb, Balbuena

doi:10.1016/j.coche.2016.08.017

Cited by 34 publications

(33 citation statements)

References 51 publications

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“…SEI growth is faster forh igher currents because the SEI current increases with j int accordingt oE quations (25) and (27). The causef or the transition in time dependence is as hift from diffusion-limited to migration-limited growth.…”

Section: Ultra Long-termsei Growthmentioning

confidence: 99%

“…[23][24][25][26] On the microscale, atomistic simulations were used to analyze the chemical structure, composition, and reactionso ft he SEI. [7,[27][28][29] On the mesoscale, detailed continuum modelss hed light on the processes at the electrochemical interfaces. [30][31][32] In these mesoscale models, it is well-established that transport processes limit SEI growth during long-term battery storage.T ransport limitations lead to ac apacity fade proportionalt ot he square root of elapsed time, that is, p t. Different mechanismsw ere proposed to explain this behavior, [6,33] including solvent diffusion, [2,[30][31][32][34][35][36][37][38][39][40] electronc onduction, [4,30,32,37,[41][42][43][44] electron tunneling, [31,36,45] and the diffusion of neutral lithium atoms.…”

Section: Introductionmentioning

confidence: 99%

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Solid–Electrolyte Interphase During Battery Cycling: Theory of Growth Regimes

2020

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The capacity fade of modern lithium ion batteries is mainly caused by the formation and growth of the solid–electrolyte interphase (SEI). Numerous continuum models support its understanding and mitigation by studying SEI growth during battery storage. However, only a few electrochemical models discuss SEI growth during battery operation. In this article, a continuum model is developed that consistently captures the influence of open‐circuit potential, current direction, current magnitude, and cycle number on the growth of the SEI. The model is based on the formation and diffusion of neutral lithium atoms, which carry electrons through the SEI. Recent short‐ and long‐term experiments provide validation for our model. SEI growth is limited by either reaction, diffusion, or migration. For the first time, the transition between these mechanisms is modelled. Thereby, an explanation is provided for the fading of capacity with time t of the form t β with the scaling coefficent β , 0≤ β ≤1. Based on the model, critical operation conditions accelerating SEI growth are identified.

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Section: Ultra Long-termsei Growthmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Solid–Electrolyte Interphase During Battery Cycling: Theory of Growth Regimes

2020

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“…Nano-structured Si can avoid Si fracture, but because of the high surface area, it must be optimized along with a chemically and mechanically stable SEI in order to avoid SEI mechanical-electrochemical degradation and to achieve high Coulombic efficiency. 45 In terms of lithium metal anode, dendrites, which can lead to short circuits and electronically disconnected lithium, is still an unresolved issue. 37,[39][40][41] The origin of the issue is the extremely active Li metal surface, as SEI has to form on Li surfaces.…”

Section: Solid Electrolyte Interphase (Sei) In Li-ion Batteriesmentioning

confidence: 99%

“…Leung and Budzien compared EC decomposition on the basal plane of lithiated graphite (LiC 6 ), terminated with =O, -OH and -H and found that C = O edges provide a larger driving force for EC reduction 62 The observation that EC is more inclined to decompose in the presence of oxygen/ hydroxyl termination is consistent with other simulation results. 96 Besides graphite, EC decomposition was simulated on Li, 57,60,97 Si, 45,64,98 and Sn 99 electrodes as well. Due to the lower potential of Li metal than graphite, the decomposition of EC on Li metal is spontaneous and much faster than that on LiC 6 surfaces.…”

Section: Ec Solvent Decomposition Mechanismmentioning

confidence: 99%

Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries

et al. 2018

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A passivation layer called the solid electrolyte interphase (SEI) is formed on electrode surfaces from decomposition products of electrolytes. The SEI allows Li + transport and blocks electrons in order to prevent further electrolyte decomposition and ensure continued electrochemical reactions. The formation and growth mechanism of the nanometer thick SEI films are yet to be completely understood owing to their complex structure and lack of reliable in situ experimental techniques. Significant advances in computational methods have made it possible to predictively model the fundamentals of SEI. This review aims to give an overview of state-of-the-art modeling progress in the investigation of SEI films on the anodes, ranging from electronic structure calculations to mesoscale modeling, covering the thermodynamics and kinetics of electrolyte reduction reactions, SEI formation, modification through electrolyte design, correlation of SEI properties with battery performance, and the artificial SEI design. Multiscale simulations have been summarized and compared with each other as well as with experiments. Computational details of the fundamental properties of SEI, such as electron tunneling, Li-ion transport, chemical/mechanical stability of the bulk SEI and electrode/(SEI/) electrolyte interfaces have been discussed. This review shows the potential of computational approaches in the deconvolution of SEI properties and design of artificial SEI. We believe that computational modeling can be integrated with experiments to complement each other and lead to a better understanding of the complex SEI for the development of a highly efficient battery in the future.

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“…8,19,20 Lithium dendrite growth has been extensively investigated in the last decades, 21 but lithium dendrite growth is still almost inevitable during charge and discharge cycles of the battery. 22,23 Lithium dendrites growth has been detected at the solid-electrolyte interphase (SEI) cracks. 16,21 On the other hand, recently Zhang et al were able to produce dendrite free electrodes using FEC/LiNO 3 electrolyte, 24 and Mashayek et al 25 has reported Liion diffusion through the SEI of Li-metal batteries.…”

Section: Introductionmentioning

confidence: 99%