Towards high throughput screening of electrochemical stability of battery electrolytes

Borodin, Oleg; Olguin, Marco; Spear, Carrie; Leiter, Kenneth W.; Knap, Jaroslaw

doi:10.1088/0957-4484/26/35/354003

Cited by 182 publications

(273 citation statements)

References 116 publications

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“…6,8 Furthermore, EC has a higher reduction potential. 9 Li 2 CO 3 is not present or only found in small quantities in recent studies. 6,7,10 Its presence in several older studies is believed to correlate to water and CO 2 contamination.…”

mentioning

confidence: 76%

Revealing SEI Morphology: In-Depth Analysis of a Modeling Approach

Single

Horstmann

Latz

2017

J. Electrochem. Soc.

109

134

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In this article, we present a novel theory for the long term evolution of the solid electrolyte interphase (SEI) in lithium-ion batteries and propose novel validation measurements. Both SEI thickness and morphology are predicted by our model as we take into account two transport mechanisms, i.e., solvent diffusion in the SEI pores and charge transport in the solid SEI phase. We show that a porous SEI is created due to the interplay of these transport mechanisms. Different dual layer SEIs emerge from different electrolyte decomposition reactions. We reveal the behavior of such dual layer structures and discuss its dependence on system parameters. Model analysis enables us to interpret SEI thickness fluctuations and link them to the rate-limiting transport mechanism. Our results are general and independent of specific modeling choices, e.g., for charge transport and reduction reactions. In the near future, automotive and mobile applications demand power storage with large energy and power density. Currently, lithiumion batteries (LIBs) are the technology of choice for devices with these demands. They operate at high cell potentials and offer high specific capacities while providing long lifetimes. The latter is a consequence of the stable chemistry of modern LIB systems. A significant part of this stability can be attributed to the passivation ability of the solid electrolyte interphase (SEI). This thin layer forms between the negative electrode and the electrolyte. Hence contact between these phases is prevented and the continuous reduction of electrolyte molecules is suppressed. These reduction processes occur because the operating potential of the negative electrode lies well below the stability window of the electrolyte.1 They are suppressed because reduction products quickly form the SEI during the first charge of a pristine electrode. The self passivating ability is one of the most important distinctions between a well and a badly performing lithium-ion battery chemistry. It is of such importance because the reduction reactions consume lithium-ions, directly reducing battery capacity. However, a real SEI is not perfectly passivating and electrolyte reduction is never completely suppressed. Consequently, the lifetime of a battery is directly related to the long-term passivating ability of the SEI.Numerous studies on SEI have been conducted since Peled reported on this correlation in 1979.2 Most of these studies are experimental, investigating cycling stability as well as SEI impedance and composition. Theoretical studies are scarce in comparison, despite established methods such as DFT and DFT/MD derivatives. This can be partially explained with the chemical diversity of SEI, which has been investigated by Aurbach et al. for decades. Results are summarized in Refs. 3, 4 and include the study of SEI formation on graphite electrodes in organic solvent mixtures. The most significant finding of this time is that ethylene carbonate (EC) forms a stable SEI on graphite as opposed to propylene carbonate (PC). Another...

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mentioning

confidence: 76%

Revealing SEI Morphology: In-Depth Analysis of a Modeling Approach

Single

Horstmann

Latz

2017

J. Electrochem. Soc.

109

134

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“…5 for the subset of the previously screened data. 84,85 The oxidation and reduction stability for the representative model systems was estimated from the absolute oxidation and reduction potentials of a complexes relative to an electron at rest in vacuum with a subsequent subtraction of 1.4 V to convert them to the commonly used Li/Li + potential scale and compared with experimental data. 86 Note that the oxidation stability of the isolated DME and EC molecules in implicit solvent was predicted to be 5.8 and 6.9 V versus Li/Li + , 86 which is clearly much higher than the experimentally observed stability of DME and EC-based electrolytes.…”

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confidence: 99%

In situ surface protection for enhancing stability and performance of conversion-type cathodes

Borodin

Yushin

2017

MRS Energy & Sustainability

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Lithium and lithium-ion batteries (LBs and LIBs) are the most popular battery systems for electrochemical energy storage technologies. Commercial LIBs utilize intercalation-type cathode materials, mostly nickel (Ni)-based and cobalt (Co)-based cathodes, showing specific capacities of up to ∼200 mA h/g (theoretical capacity below 300 mA h/g), which limit the specific energy of batteries, and are additionally expensive and toxic. An EPA study showed that the Ni-and Co-containing batteries that use solvent-based electrode processing have the highest potential for negative environmental impacts. 1 These impacts include resource depletion, global warming, ecological toxicity, and human health impacts with the largest contributing processes include those associated with the production, processing, and use of cobalt and nickel metal compounds, which may cause adverse respiratory, pulmonary, and neurological effects in those exposed. 1 The study suggested cathode material substitution and solvent-less electrode processing to reduce these impacts. 1 The uneven distribution of Co in the earth crust 2 and the insufficient use of suitable personal protection equipment in many Co mining developing countries 3,4 created a major concern. For example, Amnesty International findings of major exploitations of children in Co mines and the related child sickness and deaths 3,4 demonstrate some of the most horrific examples of child labor, which international community should not tolerate and certainly should not encourage through growing market demands for Co. The growing Co contained-electronic waste ABSTRACTThe use of in situ formed protective layer on conversion cathodes was introduced as a cheap and simple strategy to shield these materials from undesirable interactions with liquid electrolytes.Conversion-type cathodes have been viewed as promising candidates to replace Ni-and Co-based intercalation-type cathodes for next-generation lithium (Li) and Li-ion batteries with higher specific energy, lower cost, and potentially longer cycle life. Typically, in conversion reactions two or three Li ions may be stored per just one atom of chalcogen (e.g., S or Se) or transition metal (e.g., Fe or Cu used in halides). Unfortunately, in conversion chemistries the active materials or intermediate charge/discharge products suffer from various unfavorable interactions and dissolution in organic electrolytes. In this mini-review article, we discuss the current interfacial challenges and focus on the protective layers in situ formed on the cathode surface to effectively shield conversion materials from undesirable interactions with liquid electrolytes. We further explore the mechanisms and current progress of forming such protective layers by using various salts, solvents, and additives together with the insight from molecular modeling. Finally, we discuss future opportunities and perspectives of in situ surface protection.Keywords: Li; S; F; coating; energy storage Review DiSCUSSiON POiNTS• Conversion-type cathodes have been viewed as promi...

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“…[31][32][33] The inclusion of these interactions into screening analyses will lead to more accurate predictions of the stability window of candidate electrolytes. 34 Towards this goal, the present study aims to quantify the renormalization of HOMO/LUMO levels of several common electrolyte solvents that arise from interactions with prototypical Mg battery electrodes. As illustrated in Figure 1, electrode interactions are critical for electrolyte stability as oxidation and/or reduction of the electrolyte occurs through electron transfer at interfaces with solid electrodes.…”

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confidence: 99%

Interface-Induced Renormalization of Electrolyte Energy Levels in Magnesium Batteries

Kumar¹,

Siegel

2016

J. Phys. Chem. Lett.

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A promising strategy for increasing the energy density of Li-ion batteries is to substitute a multivalent (MV) metal for the commonly used lithiated carbon anode. Magnesium is a prime candidate for such a MV battery due to its high volumetric capacity, abundance, and limited tendency to form dendrites. One challenge that is slowing the implementation of Mg-based batteries, however, is the development of efficient and stable electrolytes. Computational screening for molecular species having sufficiently wide electrochemical windows is a starting point for the identification of optimal electrolytes. Nevertheless, this window can be altered via interfacial interactions with electrodes. These interactions are typically omitted in screening studies, yet they have the potential to generate large shifts to the HOMO and LUMO of the electrolyte components. The present study quantifies the stability of several common electrolyte solvents on model electrodes of relevance for Mg batteries. Many-body perturbation theory calculations based on the G 0 W 0 method were used to predict shifts in a solvent's electronic levels arising from interfacial interactions. In molecules exhibiting large dipole moments, our calculations indicate that these interactions reduce the HOMO− LUMO gap by ∼25% (compared to isolated molecules). We conclude that electrode interactions can narrow an electrolyte's electrochemical window significantly, thereby accelerating redox decomposition reactions. Accounting for these interactions in screening studies presents an opportunity to refine predictions of electrolyte stability.

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Towards high throughput screening of electrochemical stability of battery electrolytes

Cited by 182 publications

References 116 publications

Revealing SEI Morphology: In-Depth Analysis of a Modeling Approach

Revealing SEI Morphology: In-Depth Analysis of a Modeling Approach

In situ surface protection for enhancing stability and performance of conversion-type cathodes

Interface-Induced Renormalization of Electrolyte Energy Levels in Magnesium Batteries

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