High-throughput quantum chemistry and virtual screening for lithium ion battery electrolyte additives

Halls, Mathew D.; Tasaki, Ken

doi:10.1016/j.jpowsour.2009.09.024

Cited by 95 publications

(101 citation statements)

References 24 publications

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“…In 2009, Han et al 145 calculated the ionization potential and oxidation potential for 108 organic molecules to search for electrolytes with high oxidation voltage. For the reduction reaction, 7381 EC-based structures have been screened by Halls and Tasaki 146 in 2010. Based on the comparison of the fundamental electrochemical properties of a reductive additive required for efficient SEI formation, many descriptors can be used, such as HOMO, LUMO, electron affinity (EA), relative dipole moment, and chemical hardness (η).…”

Section: In Vivo Modification and Design Of The Seimentioning

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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Section: In Vivo Modification and Design Of The Seimentioning

confidence: 99%

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

et al. 2018

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“…Later on an improved model resorted to the thermodynamics instead of kinetics to evaluate the additive candidates, arguing that the electrochemical potential at which the candidate decomposes is more decisive than kinetic rate. 38,39 Since the reduction/oxidation potentials of a given species are more easily accessible via computation than kinetic data, this latter model is now widely adopted by researchers to screen and evaluate potential SEI additives. Nevertheless, those two models share the common belief that a more reactive species might be a better candidate for interphase.…”

Section: Formation Mechanismmentioning

confidence: 99%

Interfacing electrolytes with electrodes in Li ion batteries

2011

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Aqui.Onde a terra termina e o mar j a não começa -A poetic definition of a binary liquid/solid interface by Lu ıs de Camões (1572). Since its birth in early 1990s, Li ion battery technology has been powering the rapid digitization of our daily life and finally made its debut in 2010 into the large format application for electrified vehicles such as the Nissan Leaf and GM Chevrolet Volt; however, much of the chemistry and processes underneath this amazing energy storage device still remain to be understood, among which is the interphase between electrolyte and electrodes. Interphases are formed in situ on electrode surfaces from sacrificial decomposition of electrolytes. Their ad hoc chemistry supports the reversible Li + -intercalation in both anode and cathode materials at extreme potentials, while preventing parasitic reductions/oxidations on the reactive surfaces of those electrodes; but their existence places restrictions on energy and power densities of the device by impeding Li + -transport and setting operating voltage limits, respectively. It has been the dream of battery engineers to maximize the former and minimize the latter. This review summarizes the most recent knowledge about the chemistry and formation mechanism of this elusive battery component on both anode and cathode surfaces. The attempts to tailor a desired interphasial chemistry via diversified means were also discussed.

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“…The first two describe the thermodynamic ability to accept a new electron and are used to assess the reduction potential, whereas η is a measure of reaction resistance and can serve as an indicator of the kinetics. Halls and Tasaki showed that a small η and low LUMO are favorable for SEI-forming additives [35]. Another couple of properties of importance were proposed by Park: the dipole moment ( μ ), and the binding energy with a lithium cation (BE).…”

Section: Introductionmentioning

confidence: 99%

SEI-forming electrolyte additives for lithium-ion batteries: development and benchmarking of computational approaches

2016

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SEI-forming additives play an important role in lithium-ion batteries, and the key to improving battery functionality is to determine if, how, and when these additives are reduced. Here, we tested a number of computational approaches and methods to determine the best way to predict and describe the properties of the additives. A wide selection of factors were evaluated, including the influences of the solvent and lithium cation as well as the DFT functional and basis set used. An optimized computational methodology was employed to assess the usefulness of different descriptors.Electronic supplementary materialThe online version of this article (doi:10.1007/s00894-016-3180-0) contains supplementary material, which is available to authorized users.

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High-throughput quantum chemistry and virtual screening for lithium ion battery electrolyte additives

Cited by 95 publications

References 24 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

Interfacing electrolytes with electrodes in Li ion batteries

SEI-forming electrolyte additives for lithium-ion batteries: development and benchmarking of computational approaches

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