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Durable Carbon-Coated Li2S Core–Shell Spheres for High Performance Lithium/Sulfur Cells

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    Durable Carbon-Coated Li2S Core–Shell Spheres for High Performance Lithium/Sulfur Cells
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    † Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720, United States
    ‡ Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    § Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China
    ∥ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    ⊥ The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    [email protected]
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    Cite this: J. Am. Chem. Soc. 2014, 136, 12, 4659–4663
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    https://doi.org/10.1021/ja412943h
    Published February 28, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    Lithium sulfide (Li2S) is an attractive cathode material with a high theoretical specific capacity (1166 mAh g–1). However, the poor cycle life and rate capability have remained significant challenges, preventing its practical application. Here, Li2S spheres with size control have been synthesized for the first time, and a CVD method for converting them into stable carbon-coated Li2S core–shell (Li2S@C) particles has been successfully employed. These Li2S@C particles with protective and conductive carbon shells show promising specific capacities and cycling performance with a high initial discharge capacity of 972 mAh g–1 Li2S (1394 mAh g–1 S) at the 0.2C rate. Even with no added carbon, a very high Li2S content (88 wt % Li2S) electrode composed of 98 wt % 1 μm Li2S@C spheres and 2 wt % binder shows rather stable cycling performance, and little morphology change after 400 cycles at the 0.5C rate.

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    Supporting Information

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    Experimental details for the preparation of Li2S and Li2S@C spheres with three different sizes; electrochemical and materials characterization; XRD pattern of Li2S@C at 700 °C; cycle performance of Li2S@C with 5 wt % C; SEM images of products with different synthesis conditions; SEM images of particles obtained with different amounts of toluene at different times; morphology of the Li2S@C materials after polysulfide dissolution tests; TEM analysis of Li2S@C spheres before and after dissolving Li2S; cycling performance of uncoated Li2S spheres, commercial Li2S, and carbon-coated milled-commercial Li2S; rate performances of all three sizes of Li2S@C particles; SEM image of commercial Li2S; CVs of commercial Li2S before and after milling; SEM images of carbon fiber paper before and after drop casting. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: J. Am. Chem. Soc. 2014, 136, 12, 4659–4663
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