Cobalt in Nitrogen-Doped Graphene as Single-Atom Catalyst for High-Sulfur Content Lithium–Sulfur Batteries
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- 14 February 2019
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 141 (9), 3977-3985
- https://doi.org/10.1021/jacs.8b12973
Abstract
Due to their high theoretical energy density and low cost, lithium-sulphur (Li–S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li-S batteries largely depends on the efficient reversible conversion of Li polysulphides to Li2S in discharge, and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co-N/G) can trigger the surface-mediated reaction of Li polysulphides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co-N-C coordination centre serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li2S in discharge and charge processes, respectively. The S@Co-N/G composite, with a high S mass ratio of 90 wt.%, can deliver a gravimetric capacity of 1210 mAh g-1, and exhibits an areal capacity of 5.1 mAh cm-2 with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm-2 on the electrode disk.Keywords
Funding Information
- National Natural Science Foundation of China (21503064, 51761145046)
- Chinese Academy of Sciences (100 Talents Program, XDB01020300)
- Ministry of Science and Technology of the People's Republic of China (2016YFA0200602, 2018YFA0208603)
- Ministry of Education of the People's Republic of China (WK3430000003)
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