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      • Magnetism in lithium-oxygen discharge product.

        Lu, Jun,Jung, Hun-Ji,Lau, Kah Chun,Zhang, Zhengcheng,Schlueter, John A,Du, Peng,Assary, Rajeev S,Greeley, Jeffrey,Ferguson, Glen A,Wang, Hsien-Hau,Hassoun, Jusef,Iddir, Hakim,Zhou, Jigang,Zuin, Lucia Wiley-VCH 2013 ChemSusChem Vol.6 No.7

        <P>Nonaqueous lithium-oxygen batteries have a much superior theoretical gravimetric energy density compared to conventional lithium-ion batteries, and thus could render long-range electric vehicles a reality. A molecular-level understanding of the reversible formation of lithium peroxide in these batteries, the properties of major/minor discharge products, and the stability of the nonaqueous electrolytes is required to achieve successful lithium-oxygen batteries. We demonstrate that the major discharge product formed in the lithium-oxygen cell, lithium peroxide, exhibits a magnetic moment. These results are based on dc-magnetization measurements and a lithium-oxygen cell containing an ether-based electrolyte. The results are unexpected because bulk lithium peroxide has a significant band gap. Density functional calculations predict that superoxide-type surface oxygen groups with unpaired electrons exist on stoichiometric lithium peroxide crystalline surfaces and on nanoparticle surfaces; these computational results are consistent with the magnetic measurement of the discharged lithium peroxide product as well as EPR measurements on commercial lithium peroxide. The presence of superoxide-type surface oxygen groups with spin can play a role in the reversible formation and decomposition of lithium peroxide as well as the reversible formation and decomposition of electrolyte molecules.</P>

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

        Zhang, Zhengcheng,Lu, Jun,Assary, Rajeev S.,Du, Peng,Wang, Hsien-Hau,Sun, Yang-Kook,Qin, Yan,Lau, Kah Chun,Greeley, Jeffrey,Redfern, Paul C.,Iddir, Hakim,Curtiss, Larry A.,Amine, Khalil American Chemical Society 2011 JOURNAL OF PHYSICAL CHEMISTRY C - Vol.115 No.51

        <P>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 (<ext-link xlink:type='simple'>1NM3</ext-link>) 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 <ext-link xlink:type='simple'>1NM3</ext-link> 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.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpccck/2011/jpccck.2011.115.issue-51/jp2087412/production/images/medium/jp-2011-087412_0009.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/jp2087412'>ACS Electronic Supporting Info</A></P>

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