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Directly Formed Alucone on Lithium Metal for High-Performance Li Batteries and Li–S Batteries with High Sulfur Mass Loading

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† ‡ Energy Systems Division and Joint Center for Energy Storage Research (JCESR), Argonne National Laboratory, Argonne, Illinois 60439, United States
§ Department of Mechanical and Industrial Engineering, University of Illinois at Chicago, Chicago, Illinois 60607, United States
Materials Science and Engineering, Sandia National Laboratories, Albuquerque, New Mexico 87185, United States
Cite this: ACS Appl. Mater. Interfaces 2018, 10, 8, 7043–7051
Publication Date (Web):January 30, 2018
Copyright © 2018 American Chemical Society

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    Lithium metal is considered the “holy grail” of next-generation battery anodes. However, severe parasitic reactions at the lithium–electrolyte interface deplete the liquid electrolyte and the uncontrolled formation of high surface area and dendritic lithium during cycling causes rapid capacity fading and battery failure. Engineering a dendrite-free lithium metal anode is therefore critical for the development of long-life batteries using lithium anodes. In this study, we deposit a conformal, organic/inorganic hybrid coating, for the first time, directly on lithium metal using molecular layer deposition (MLD) to alleviate these problems. This hybrid organic/inorganic film with high cross-linking structure can stabilize lithium against dendrite growth and minimize side reactions, as indicated by scanning electron microscopy. We discovered that the alucone coating yielded several times longer cycle life at high current rates compared to the uncoated lithium and achieved a steady Coulombic efficiency of 99.5%, demonstrating that the highly cross-linking structured material with great mechanical properties and good flexibility can effectively suppress dendrite formation. The protected Li was further evaluated in lithium–sulfur (Li–S) batteries with a high sulfur mass loading of ∼5 mg/cm2. After 140 cycles at a high current rate of ∼1 mA/cm2, alucone-coated Li–S batteries delivered a capacity of 657.7 mAh/g, 39.5% better than that of a bare lithium–sulfur battery. These findings suggest that flexible coating with high cross-linking structure by MLD is effective to enable lithium protection and offers a very promising avenue for improved performance in the real applications of Li–S batteries.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.7b15879.

    • Scanning line detection by ABF TEM, EDX imaging, symmetric cell testing, asymmetric cell testing, lithium–sulfur battery testing at different cycling rates (PDF)

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