Two-electron reduction of ethylene carbonate: A quantum chemistry re-examination of mechanisms
By K. Leung. 2013
137 citations recorded by the source corpus.
Abstract Passivating solid-electrolyte interphase (SEI) films arising from electrolyte decomposition on low-voltage lithium ion battery anode surfaces are critical for battery operations. We review the recent theoretical literature on electrolyte decomposition and emphasize the modeling work on two-electron reduction of ethylene carbonate (EC, a key battery organic solvent). One of the two-electron pathways, which releases CO gas, is re-examined using simple quantum chemistry calculations. Excess electrons are shown to preferentially attack EC in the order (broken EC−) > (intact EC−) > EC. This confirms the viability of two electron processes and emphasizes that they need to be considered when interpreting SEI experiments. A speculative estimate of the crossover between one- and two-electron regimes under a homogeneous reaction zone approximation is proposed.
Subfields: Electrical and Electronic Engineering, Process Chemistry and Technology, Renewable Energy, Sustainability and the Environment
View Paper: https://www.semanticscholar.org/paper/2b77c223f86ab0f033b97a287e094143a01c64e8
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In Electrical and Electronic Engineering
In Process Chemistry and Technology
In Renewable Energy, Sustainability and the Environment
Citations in the corpus
- Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries (2018, methodology): “The calculated reaction rate depends on computational methods, and as Perdew–Burke–Ernzerhof hybrid (PBE0) functional finds much slower ring-opening dynamics, while Perdew–Burke–Ernzerhof (PBE) functional is more suited to two-electron reactions.(60,65) Leung(65) computed the energy barriers, took t”
- The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling (2016, background): “Certain interfacial reduction and oxidation reactions have been described in the literature using AIMD.[182-188] APPLE&P (Atomistic Polarizable Potential for Liquids, Electrolytes, & Polymers) is another many-body polarizable force field for MD simulations that can capture electrostatic interactions”