Increased Stability Toward Oxygen Reduction Products for Lithium-Air Batteries with Oligoether-Functionalized Silane Electrolytes

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• 作者：Zhengcheng Zhang ; Jun Lu ; Rajeev S. Assary ; Peng Du ; Hsien-Hau Wang ; Yang-Kook Sun ; Yan Qin ; Kah Chun Lau ; Jeffrey Greeley ; Paul C. Redfern ; Hakim Iddir ; Larry A. Curtiss ; Khalil Amine
• 刊名：Journal of Physical Chemistry C
• 出版年：2011
• 出版时间：December 29, 2011
• 年：2011
• 卷：115
• 期：51
• 页码：25535-25542
• 全文大小：915K
• 年卷期：v.115,no.51(December 29, 2011)
• ISSN：1932-7455

文摘

The successful development of Li-air batteries would significantly increase the possibility of extending the range of electric vehicles. There is much evidence that typical organic carbonate based electrolytes used in lithium ion batteries form lithium carbonates from reaction with oxygen reduction products during discharge in lithium-air cells so more stable electrolytes need to be found. This combined experimental and computational study of an electrolyte based on a tri(ethylene glycol)-substituted trimethylsilane (1NM3) provides evidence that the ethers are more stable toward oxygen reduction discharge species. X-ray photoelectron spectroscopy (XPS) and FTIR experiments show that only lithium oxides and no carbonates are formed when 1NM3 electrolyte is used. In contrast XPS shows that propylene carbonate (PC) in the same cell configuration decomposes to form lithium carbonates during discharge. Density functional calculations of probable decomposition reaction pathways involving solvated oxygen reduction species confirm that oligoether substituted silanes, as well as other ethers, are more stable to the oxygen reduction products than propylene carbonate. These results indicate that the choice of electrolyte plays a key role in the performance of Li-air batteries.