Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 9, Pages 3977-3985Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b12973
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Funding
- National Natural Science Foundation of China [21503064, 51761145046]
- MOST [2016YFA0200602, 2018YFA0208603]
- Strategic Priority Research Program of CAS [XDB01020300]
- 100 Talents Program of the Chinese Academy of Sciences
- Fundamental Research Funds for the Central Universities [WK3430000003]
- National Program for Support of Topnotch Young Professional
- iChEM
- USTCSCC Supercomputer Center
- SCCAS Supercomputer Center
- Tianjin Supercomputer Center
- Shanghai Supercomputer Center
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Because of their high theoretical energy density and low cost, lithium-sulfur (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 polysulfides 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 surfacemediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co-N-C coordination center 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 it 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.
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