First-Principles Modeling of the Initial Stages of Organic Solvent Decomposition on LixMn2O4(100) Surfaces

被引：118

作者：

Leung, Kevin ^{[1
]}

机构：

[1] Sandia Natl Labs, Albuquerque, NM 87185 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2012年 / 116卷 / 18期

关键词：

LITHIUM-ION BATTERIES; OXIDATIVE DECOMPOSITION; PROPYLENE CARBONATE; REDOX POTENTIALS; LAYER FORMATION; ELECTROCHEMICAL OXIDATION; REDUCTION-MECHANISMS; LIMN2O4; ELECTRODES; MOLECULAR-DYNAMICS; ETHYLENE CARBONATE;

D O I：

10.1021/jp212415x

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Density functional theory and ab initio molecular dynamics simulations are applied to investigate the initial steps of ethylene carbonate (EC) decomposition on spinel Li0.6Mn2O4(100) surfaces. EC is a key component of the electrolyte used in lithium ion batteries. We predict a slightly exothermic EC bond-breaking event on this oxide facet, which facilitates subsequent EC oxidation and proton transfer to the oxide surface. Both the proton and the partially decomposed EC fragment weaken the Mn-O ionic bonding network. Implications for an interfacial film made of decomposed electrolyte on cathode surfaces, and LixMn2O4 dissolution during power cycling, are discussed.

引用

收藏

页码：9852 / 9861

页数：10

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