Reduction Mechanisms of Ethylene Carbonate on Si Anodes of Lithium-Ion Batteries: Effects of Degree of Lithiation and Nature of Exposed Surface

Hoz, Julibeth M. Martínez de la; Leung, Kevin; Balbuena, Perla B.

doi:10.1021/am404365r

Cited by 75 publications

(124 citation statements)

References 44 publications

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“…In the case of Li 13 Si 4 , such a species receives two extra electrons from the anode surface producing an adsorbed CO 2− anion and a radical anion -OC 2 H 2 O 2− . 64 The EC and VC reduction can also be changed by the nearby salt and a new CO 2 formation pathway for VC was reported. 56 FEC, on the other hand, shows less dependence on the lithium content in Si.…”

Section: In Vivo Modification and Design Of The Seimentioning

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%

“…When Si becomes lithiated, its voltage drops, and therefore the lithium concentration in silicon greatly influences the electrolyte reduction reactions. 53,64,98,99 Martinez de la Hoz et al 64 found that EC can be reduced by two different twoelectron mechanisms (one simultaneous and one sequential) on intermediately lithiated silicon surfaces (LiSi). A later work done by Ma and Balbuena 98 provided a more detailed reduction mechanism of EC under the low lithiated state of silicon anode.…”

Section: Ec Solvent Decomposition Mechanismmentioning

confidence: 99%

“…Fluoroethylene carbonate (FEC) gained renewed interests, 56,64,98,120,121 as it shows promise as an electrolyte additive for improved SEI passivation on Si-and Sn-based anode. 122,123 It is insightful to compare how EC, VC, and FEC reduce differently on these electrode surfaces.…”

Section: In Vivo Modification and Design Of The Seimentioning

confidence: 99%

“…The lithium concentration in Si is correlated to the anode potential, and AIMD simulations were used to investigate its effect on the reduction pathways for EC and VC. 56,64,98,121 For example, on less lithiated Si anodes (LiSi 2 and LiSi), VC may be reduced via a two-electron mechanism, yielding an opened VC 2− anion. In the case of Li 13 Si 4 , such a species receives two extra electrons from the anode surface producing an adsorbed CO 2− anion and a radical anion -OC 2 H 2 O 2− .…”

Section: In Vivo Modification and Design Of The Seimentioning

confidence: 99%

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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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Section: In Vivo Modification and Design Of The Seimentioning

confidence: 99%

Section: Ec Solvent Decomposition Mechanismmentioning

confidence: 99%

Section: Ec Solvent Decomposition Mechanismmentioning

confidence: 99%

Section: In Vivo Modification and Design Of The Seimentioning

confidence: 99%

Section: In Vivo Modification and Design Of The Seimentioning

confidence: 99%

See 3 more Smart Citations

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

et al. 2018

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Tuning the Solid Electrolyte Interphase for Selective Li‐ and Na‐Ion Storage in Hard Carbon

et al. 2017

Self Cite

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Solid-electrolyte interphase (SEI) films with controllable properties are highly desirable for improving battery performance. In this paper, a combined experimental and theoretical approach is used to study SEI films formed on hard carbon in Li- and Na-ion batteries. It is shown that a stable SEI layer can be designed by precycling an electrode in a desired Li- or Na-based electrolyte, and that ionic transport can be kinetically controlled. Selective Li- and Na-based SEI membranes are produced using Li- or Na-based electrolytes, respectively. The Na-based SEI allows easy transport of Li ions, while the Li-based SEI shuts off Na-ion transport. Na-ion storage can be manipulated by tuning the SEI layer with film-forming electrolyte additives, or by preforming an SEI layer on the electrode surface. The Na specific capacity can be controlled to < 25 mAh g ; ≈ 1/10 of the normal capacity (250 mAh g ). Unusual selective/preferential transport of Li ions is demonstrated by preforming an SEI layer on the electrode surface and corroborated with a mixed electrolyte. This work may provide new guidance for preparing good ion-selective conductors using electrochemical approaches.

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Modeling the Solid Electrolyte Interphase: Machine Learning as a Game Changer?

Diddens

Appiah

Mabrouk

et al. 2022

Adv Materials Inter

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The solid electrolyte interphase (SEI) is a complex passivation layer that forms in situ on many battery electrodes such as lithium‐intercalated graphite or lithium metal anodes. Its essential function is to prevent the electrolyte from continuous electrochemical degradation, while simultaneously allowing ions to pass through, thus constituting an electronically insulating, but ionically conducting material. Its properties crucially affect the overall performance and aging of a battery cell. Despite decades of intense research, understanding the SEI's precise formation mechanism, structure, composition, and evolution remains a conundrum. State‐of‐the‐art computational modeling techniques are powerful tools to gain additional insights, although confronted with a trade‐off between accuracy and accessible time‐ and length scales. In this review, it is discussed how recent advances in data‐driven models, especially the development of fast and accurate surrogate simulators and deep generative models, can work with physics‐based and physics‐informed approaches to enable the next generation of breakthroughs in this field. Machine learning‐enhanced multiscale models can provide new pathways to inverse the design of interphases with desired properties.

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Reduction Mechanisms of Ethylene Carbonate on Si Anodes of Lithium-Ion Batteries: Effects of Degree of Lithiation and Nature of Exposed Surface

Cited by 75 publications

References 44 publications

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

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

Tuning the Solid Electrolyte Interphase for Selective Li‐ and Na‐Ion Storage in Hard Carbon

Modeling the Solid Electrolyte Interphase: Machine Learning as a Game Changer?

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