Component-/structure-dependent elasticity of solid electrolyte interphase layer in Li-ion batteries: Experimental and computational studies

Shin, Hosop; Park, Jong‐Hyun; Han, Sangwoo; Sastry, Ann Marie; Lu, Wei

doi:10.1016/j.jpowsour.2014.11.120

Cited by 145 publications

(152 citation statements)

References 73 publications

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“…Shang et al 187 computed the elastic properties of Li 2 CO 3 with DFT. With the integration of experimental and computational studies, Shin et al 188 gave the stiffness of dominant constituents in SEI in the order of LiF > Li 2 CO 3 > Li 2 EDC > LiMC > PEO. The stiffness decreases roughly from the inorganic components to the organic and then to the polymeric parts.…”

Section: Correlation Of Sei Properties With Battery Performance Starmentioning

confidence: 99%

“…The stiffness decreases roughly from the inorganic components to the organic and then to the polymeric parts. 188 According to the recent simulations with the APPLE&P force field, Li 2 BDC is less stiff than Li 2 EDC. 177 In addition to the bulk modulus, the work of adhesion is equally important for the SEI.…”

Section: Correlation Of Sei Properties With Battery Performance Starmentioning

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: Correlation Of Sei Properties With Battery Performance Starmentioning

confidence: 99%

Section: Correlation Of Sei Properties With Battery Performance Starmentioning

confidence: 99%

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

et al. 2018

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“…Among the factors affecting the SEI layer's evolution, a strong dependence on temperature and state of charge has been proved to exist for its morphology, composition and Lithium ionic conductivity [7,37]. Continuum theory for the growth of an SEI layer have been recently proposed by many authors [128,180,181,182,183,184,77,185,186,187,188,189,190,191].…”

Section: Microscopic Phenomena and Their Modelingmentioning

confidence: 99%

Computational modeling of Li-ion batteries

2016

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This review focuses on energy storage materials modeling, with particular emphasis on Li-ion batteries. Theoretical and computational analyses not only provide a better understanding of the intimate behavior of actual batteries under operational and extreme conditions, but they may tailor new materials and shape new architectures in a complementary way to experimental approaches. Modeling can therefore play a very valuable role in the design and lifetime prediction of energy storage materials and devices. Batteries are inherently multi-scale, in space and time. The macro-structural characteristic lengths (the thickness of a single cell, for instance) are order of magnitudes larger than the particles that form the microstructure of the porous electrodes, which in turn are scale-separated from interface layers at which atomistic intercalations occur. Multi-physics modeling concepts, methodologies, and simulations at different scales, as well as scale transition strategies proposed in the recent literature are here revised. Finally, computational challenges toward the next generation of Li-ion batteries are discussed.

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“…This high degree of cross linking, in turn, implies that this polymeric matrix can have elastomeric properties. We remind that in a polymer, elasticity and high failure strain always requires a high degree of cross-linking.Estimates for bulk and shear moduli for different components of SEI obtained using atomic force spectroscopy and molecular dynamics calculations suggest that the polymeric matrix has the lowest elastic modulus of 1-2 GPa (compared to 10-20 GPa for lithium organocarbonates);55 . This can be compared with 40-70 GPa for the inner mineral layer of SEI on lithiated silicon 56.…”

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confidence: 99%

What Makes Fluoroethylene Carbonate Different?

2015

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Rechargeable lithium-ion batteries containing silicon-based negative electrodes have the potential to revolutionize electrical energy storage, but the cyclic and acyclic organic carbonate solvents (such as ethylene and propylene carbonates) that are commonly used in graphite Li-ion batteries, yield unsatisfactory performance when used with such Li alloying electrodes. It has been found by trial-and-error that additions of the closely related carbonate additive, fluoroethylene carbonate (FEC) to conventional electrolytes, yields a robust solid electrolyte interphase (SEI) on the Li x Si y alloy surface.Several mechanisms for this protective action have been considered in the literature and modeled theoretically; however, at present these mechanisms remain hypothetical. In this study, we use radiolysis, laser photoionization, electron paramagnetic resonance, and transient absorption spectroscopy to establish the redox chemistry of FEC. While the oxidation chemistry is similar to that of other organic carbonates, the reduction chemistry of the fluorinated molecule is strikingly different. Specifically, one-electron reduction of bulk FEC causes the fission of two (instead of one) C-O bonds, resulting in concerted defluorination and decarboxylation; in contrast, the reduction of the ethylene and propylene carbonate results in ring-opening and the formation of a radical anion. For FEC, the reduction yields the vinoxyl radical that can abstract an H atom from another FEC molecule, initiating both the chain reaction causing FEC decomposition and radical polymerization involving the reaction products. The resulting polymer can further defluorinate yielding the interior radicals that migrate and recombine to produce a highly cross-linked network. This feature implies that the outer SEI resulting from FEC reduction may exhibit elastomeric properties, which would account for its cohesion during expansion and contraction of silicon particles in the course of Li alloying/dealloying cycling.

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Component-/structure-dependent elasticity of solid electrolyte interphase layer in Li-ion batteries: Experimental and computational studies

Cited by 145 publications

References 73 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

Computational modeling of Li-ion batteries

What Makes Fluoroethylene Carbonate Different?

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