Effect of Anode Composition on Solid Electrolyte Interphase Formation

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

“…The one-electron reduction is favored at a high EC concentration, while the two-electron reduction is favorable at a high Li-ion concentration. Recently, an AIMD work showed that both the salt-LiPF 6 and solvent-EC participate in SEI formation on Si anode, 103 consistent with the reduction voltage calculated by Delp et al 17 Additionally, the EC decomposition on un-lithiated, Licovered, and fully lithiated Sn surfaces, as well as on a pure Li surface, was studied by Moradabadi et al 99 They showed that the decomposition is preferred on Li/β-Sn (100) and Li 17 Sn 4 (001) surfaces rather than on Li (100) in spite of its lower potential, suggesting that decomposition of EC molecules not only depends on the surface potential but also akin to the surface chemical compositions and kinetics.…”

“…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.…”

Boosting Rechargeable Batteries R&D by Multiscale Modeling: Myth or Reality?

“…Another electrode surface was studied by Moradabadi et al, comparing the reduction of EC on different Sn- and Li-based electrodes: unlithiated Sn, Li-covered Sn, lithiated Sn (Li 17 Sn 4 ), and Li metal . Decomposition of EC was found for all surfaces except for the unlithiated Sn.…”

“…Another electrode surface was studied by Moradabadi et al, comparing the reduction of EC on different Sn- and Li-based electrodes: unlithiated Sn, Li-covered Sn, lithiated Sn (Li 17 Sn 4 ), and Li metal. 310 Decomposition of EC was found for all surfaces except for the unlithiated Sn. Additionally, a lower degree of electron transfer was required to reduce EC via a two-electron mechanism toward CO 3 2– on the Li-covered and lithiated Sn electrodes (−1.90 e and −1.84 e, respectively), as compared to the Li metal electrode (−2.4 e).…”

“…20 ps. As for the scientific field at large, most studies have focused on the decomposition of the organic carbonate electrolyte solvents at different common negative electrode surfaces: graphite, , lithium metal, − silicon, and tin . Starting with graphite and the processes that occur during (over)­charging and the risk of lithium plating and/or electrolyte degradation was modeled using fully lithiated LiC 6 layers in contact with the electrolyte in order to specifically study the effect of surface functionalization of different graphite edges. , Thereby, no lithiation process of the electrode can be simulated but rather the relevant electrolyte decomposition mechanisms.…”