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 Hu, Yongfeng Sun, Yang-Kook Scrosati, Bruno Curtiss, Larry A. Amine, Kahlil 2024-01-20T12:03:23Z 2024-01-20T12:03:23Z 2021-08-31 2013-07 1864-5631 https://pubs.kist.re.kr/handle/201004/127942 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. English WILEY-V C H VERLAG GMBH NONAQUEOUS LI-O-2 BATTERIES TOTAL-ENERGY CALCULATIONS ETHER-BASED ELECTROLYTES AUGMENTED-WAVE METHOD LI-AIR BATTERIES BASIS-SET LIMITATIONS PERSPECTIVE CHALLENGES STABILITY Magnetism in Lithium-Oxygen Discharge Product Article 10.1002/cssc.201300223 1 CHEMSUSCHEM, v.6, no.7, pp.1196 - 1202 CHEMSUSCHEM 6 7 1196 1202 scie scopus 000321309600017 Chemistry, Multidisciplinary Green & Sustainable Science & Technology Chemistry Science & Technology - Other Topics Article NONAQUEOUS LI-O-2 BATTERIES TOTAL-ENERGY CALCULATIONS ETHER-BASED ELECTROLYTES AUGMENTED-WAVE METHOD LI-AIR BATTERIES BASIS-SET LIMITATIONS PERSPECTIVE CHALLENGES STABILITY batteries density functional calculations lithium peroxide magnetic properties superoxide