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      Compatible interface design of CoO-based Li-O 2 battery cathodes with long-cycling stability

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          Abstract

          Lithium-oxygen batteries with high theoretical energy densities have great potential. Recent studies have focused on different cathode architecture design to address poor cycling performance, while the impact of interface stability on cathode side has been barely reported. In this study, we introduce CoO mesoporous spheres into cathode, where the growth of crystalline discharge products (Li 2O 2) is directly observed on the CoO surface from aberration-corrected STEM. This CoO based cathode demonstrates more than 300 discharge/charge cycles with excessive lithium anode. Under deep discharge/charge, CoO cathode exhibited superior cycle performance than that of Co 3O 4 with similar nanostructure. This improved cycle performance can be ascribed to a more favorable adsorption configuration of Li 2O 2 intermediates (LiO 2) on CoO surface, which is demonstrated through DFT calculation. The favorable adsorption of LiO 2 plays an important role in the enhanced cycle performance, which reduced the contact of LiO 2 to carbon materials and further alleviated the side reactions during charge process. This compatible interface design may provide an effective approach in protecting carbon-based cathodes in metal-oxygen batteries.

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          Screening for superoxide reactivity in Li-O2 batteries: effect on Li2O2/LiOH crystallization.

          Robert Black, Si Oh, Jin-Hyon Lee … (2012)
          Unraveling the fundamentals of Li-O(2) battery chemistry is crucial to develop practical cells with energy densities that could approach their high theoretical values. We report here a straightforward chemical approach that probes the outcome of the superoxide O(2)(-), thought to initiate the electrochemical processes in the cell. We show that this serves as a good measure of electrolyte and binder stability. Superoxide readily dehydrofluorinates polyvinylidene to give byproducts that react with catalysts to produce LiOH. The Li(2)O(2) product morphology is a function of these factors and can affect Li-O(2) cell performance. This methodology is widely applicable as a probe of other potential cell components.
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            A stable cathode for the aprotic Li-O2 battery.

            Muhammed M. Ottakam Thotiyl, Stefan A. Freunberger, Zhangquan Peng … (2013)
            Rechargeable lithium-air (O2) batteries are receiving intense interest because their high theoretical specific energy exceeds that of lithium-ion batteries. If the Li-O2 battery is ever to succeed, highly reversible formation/decomposition of Li2O2 must take place at the cathode on cycling. However, carbon, used ubiquitously as the basis of the cathode, decomposes during Li2O2 oxidation on charge and actively promotes electrolyte decomposition on cycling. Replacing carbon with a nanoporous gold cathode, when in contact with a dimethyl sulphoxide-based electrolyte, does seem to demonstrate better stability. However, nanoporous gold is not a suitable cathode; its high mass destroys the key advantage of Li-O2 over Li ion (specific energy), it is too expensive and too difficult to fabricate. Identifying a suitable cathode material for the Li-O2 cell is one of the greatest challenges at present. Here we show that a TiC-based cathode reduces greatly side reactions (arising from the electrolyte and electrode degradation) compared with carbon and exhibits better reversible formation/decomposition of Li2O2 even than nanoporous gold (>98% capacity retention after 100 cycles, compared with 95% for nanoporous gold); it is also four times lighter, of lower cost and easier to fabricate. The stability may originate from the presence of TiO2 (along with some TiOC) on the surface of TiC. In contrast to carbon or nanoporous gold, TiC seems to represent a more viable, stable, cathode for aprotic Li-O2 cells.
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              A nanostructured cathode architecture for low charge overpotential in lithium-oxygen batteries.

              Jun Lu, D Abdel-Hady, H. Albishri … (2012)
              The lithium-oxygen battery, of much interest because of its very high-energy density, presents many challenges, one of which is a high-charge overpotential that results in large inefficiencies. Here we report a cathode architecture based on nanoscale components that results in a dramatic reduction in charge overpotential to ~0.2 V. The cathode utilizes atomic layer deposition of palladium nanoparticles on a carbon surface with an alumina coating for passivation of carbon defect sites. The low charge potential is enabled by the combination of palladium nanoparticles attached to the carbon cathode surface, a nanocrystalline form of lithium peroxide with grain boundaries, and the alumina coating preventing electrolyte decomposition on carbon. High-resolution transmission electron microscopy provides evidence for the nanocrystalline form of lithium peroxide. The new cathode material architecture provides the basis for future development of lithium-oxygen cathode materials that can be used to improve the efficiency and to extend cycle life.
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                Author and article information

                Journal
                Journal ID (nlm-ta): Sci Rep
                Journal ID (iso-abbrev): Sci Rep
                Title: Scientific Reports
                Publisher: Nature Publishing Group
                ISSN (Electronic): 2045-2322
                Publication date (Electronic): 27 February 2015
                Publication date Collection: 2015
                Volume: 5
                Electronic Location Identifier: 8335
                Affiliations
                [1 ]Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences , Qingdao 266101, P. R. China
                [2 ]University of Chinese Academy of Sciences , Beijing 100049, P. R. China
                [3 ]Institute of Physics, Chinese Academy of Sciences , Beijing 100080, P. R. China
                Author notes
                [*]

                These authors contributed equally to this work.

                Article
                Publisher Item ID: srep08335
                DOI: 10.1038/srep08335
                PMC ID: 4342555
                PubMed ID: 25720845
                SO-VID: 13944567-18df-4d79-99b0-579c9ad226b7
                Copyright © Copyright © 2015, Macmillan Publishers Limited. All rights reserved
                License:

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder in order to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                Date received : 23 October 2014
                Date accepted : 12 January 2015
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                Subject: Article

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