Journal
CHEMSUSCHEM
Volume 13, Issue 10, Pages 2761-2768Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202000289
Keywords
electrochemistry; electron transfer; lithium; nanotubes; sulfur
Funding
- Key Scientific Research Project of Education Department of Hunan [18A323]
- Supercomputing Center of Dalian University of Technology
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Here we propose an effective strategy to stabilize small sulfur species by using aminomethyl-functionalized carbon nanotubes (AM-CNT) without impairing the conductive channel of the carbon nanotube (CNT) cathode. The linear S-n clusters can be anchored strongly to the AM-CNT for the favorable size of n=5 and the maximum size of n=6 in the production of the cathode, which depresses the mass loss of active sulfur effectively and eliminates the formation of high-order polysulfides completely during the discharge process. The most stable 3 D cross-linked Inter-S-5-AM-CNT network shows a fast electron transfer redox reaction through the CNT skeleton that possesses a theoretical capacity of 1337 mA h g(-1) (based on sulfur) or 592 mA h g(-1) (based on the cathode). The discharge products of the linear S-5 cluster tend to form a hyperbranched tight structure through N...S...Li bridges that are fully impregnated in the AM-CNT bundles, and thus stabilize the entire system. Importantly, this study provides vital guidance into how to design cathodes based on small sulfur clusters for Li-S batteries to depress the shuttle effect intrinsically during charge-discharge cycles, which can be extended to the other small-sulfur-cluster-based batteries.
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