Carbon-Nanotube-Encapsulated-Sulfur Cathodes for Lithium-Sulfur Batteries: Integrated Computational Design and Experimental Validation

Yuxiao Lin; Jeremy Ticey; Vladimir Oleshko; Yujie Zhu; Xinsheng Zhao; Chunsheng Wang; John Cumings; Yue Qi

doi:10.1021/acs.nanolett.1c04247

Carbon-Nanotube-Encapsulated-Sulfur Cathodes for Lithium-Sulfur Batteries: Integrated Computational Design and Experimental Validation

Nano Lett. 2022 Jan 12;22(1):441-447. doi: 10.1021/acs.nanolett.1c04247. Epub 2021 Dec 29.

Authors

Yuxiao Lin^{1

2}, Jeremy Ticey³, Vladimir Oleshko^{3

4}, Yujie Zhu⁵, Xinsheng Zhao¹, Chunsheng Wang⁶, John Cumings³, Yue Qi^{2

7}

Affiliations

¹ School of Physics and Electronic Engineering, Jiangsu Normal University, Xuzhou, Jiangsu Province, China, 221116.
² Department of Chemical Engineering and Materials Science, Michigan State University, East Lansing, Michigan 48824, United States.
³ Department of Materials Science and Engineering, University of Maryland, College Park, Maryland 20742, United States.
⁴ Material Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, United States.
⁵ School of Chemistry, Beihang University, Beijing, China 100191.
⁶ Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland 20742, United States.
⁷ School of Engineering, Brown University, Providence, Rhode Island 02912, United States.

PMID: 34965149
DOI: 10.1021/acs.nanolett.1c04247

Abstract

To mitigate lithium-polysulfides (Li-PSs) shuttle in lithium-sulfur batteries (LiSBs), a unique carbon-nanotube-encapsulated-sulfur (S@CNT) cathode material with optimum open-ring sizes (ORSs) on the CNT walls were designed using an integrated computational approach followed by experimental validation. By calculating the transport barrier of Li⁺ ion through ORSs on the CNT walls and comparing the molecular size of solvents and Li-PSs with ORSs, optimum open-rings with 16-30 surrounding carbon atoms were predicted to selectively allow transportation of Li⁺ ion and evaporated sulfur while blocking both Li-PS and solvent molecules. A CNT oxidation process was proposed and simulated to generate these ORSs, and the results indicated that the optimum ORSs can be achieved by narrowly controlling the oxidation parameters. Subsequently, S@CNT cathodes were experimentally synthesized, confirming that optimum ORSs were generated in CNT oxidized at 475 K and exhibited more stable cycling behavior.

Keywords: carbon-nanotube-encapsulated-sulfur cathodes; integrated computational design; lithium polysulfides shuttle; optimum open-ring size; theoretical criteria for the synthesis.