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Reductive decomposition reactions of ethylene carbonate by explicit electron transfer from lithium: an eReaxFF molecular dynamics study

Alternate online-layout PDF export for the Islam and van Duin J. Phys. Chem. C article on eReaxFF simulations of ethylene carbonate reduction by electron transfer from lithium; same DOI as 2016islam-venue-jp6b08688.

Summary

Same J. Phys. Chem. C article as 2016islam-venue-jp6b08688 (DOI 10.1021/acs.jpcc.6b08688). eReaxFF molecular dynamics follows ethylene carbonate reduction initiated by electron transfer from lithium—ring opening toward EC⁻/Li⁺-type radicals and subsequent radical termination—without a predefined reaction list, in the SEI-formation context summarized in the abstract. This slug registers an alternate PDF export (papers/Islam_eReaxFF_LiEC_JPC_2016_online.pdf); use 2016islam-venue-jp6b08688 for stable figure and page locators when the files differ cosmetically.

Methods

Protocol matches 2016islam-venue-jp6b08688 (Section 2 energy expression: ReaxFF bonded framework plus explicit Gaussian electrons, electron–nuclear coupling, and extended nonbonded tapers). The condensed cell contains 60 EC and 40 Li atoms with three-dimensional periodic boundaries. After structural relaxation at 1 K, production trajectories are reported at 300 K and 600 K (the latter reached by gradual heating), using NVT integration, a Berendsen thermostat with 100 fs damping, velocity Verlet with Δt = 0.1 fs, and Newtonian nuclei; each explicit electron carrier uses a 1 amu fictitious mass as stated in Section 3.2 of the article. Section 3 and figure captions discuss multi‑ps segments (e.g. ~120 ps tracking of o‑EC⁻/Li⁺ radical formation, 25 ps snapshots, and 600 ps validation boxes for termination products). The manuscript text indexed for this corpus entry does not name a commercial MD package. NPT barostats, static external electric fields, and umbrella or replica enhanced sampling are not part of the primary 60 EC / 40 Li workflow. This communication applies the published eReaxFF parametrization and benchmarks against literature quantum chemistry rather than reporting a new force-field fit or a standalone DFT production study.

Findings

Trajectories show electron transfer from lithium into EC, ring opening toward EC⁻/Li⁺-type radicals, and radical termination channels consistent with SEI precursor chemistry, without encoding reactions in advance. The authors report that eReaxFF reaction energetics for EC reduction align better with cited quantum-chemistry references than prior ReaxFF treatments that misestimated the EC electron affinity and gave overly fast dissociation kinetics. Side-by-side 300 K and 600 K runs illustrate how temperature changes which termination channels appear within the simulated time windows. The introduction stresses that salt, cosolvent, and additive chemistry at real electrode–electrolyte interfaces remains only partially explored and that ab initio MD remains too costly for large interfacial cells—motivating reactive force-field approaches with explicit electrons.

Corpus note. Duplicate PDF bytes relative to other registered paths for this DOI; cite 2016islam-venue-jp6b08688 for figure and page locators.

Limitations

The simplified EC plus Li model omits full salt and solvent mixtures and realistic electrode surface complexity. Pseudoclassical electrons are approximate. Reconcile pagination with Islam_eReaxFF_LiEC_JPC_C_2016.pdf versus other exports.

Relevance to group

Bibliography disambiguation entry for multiple PDF bytes of one van Duin-group eReaxFF SEI paper.

Citations and evidence anchors

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