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Enhanced Li–S Batteries Using Amine-Functionalized Carbon Nanotubes in the Cathode

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Department of Materials Science & Engineering and Department of Chemical and Biomolecular Engineering, Cornell University, Ithaca, New York 14853, United States
Cite this: ACS Nano 2016, 10, 1, 1050–1059
Publication Date (Web):December 4, 2015
https://doi.org/10.1021/acsnano.5b06373
Copyright © 2015 American Chemical Society

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    Abstract

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    The rechargeable lithium–sulfur (Li–S) battery is an attractive platform for high-energy, low-cost electrochemical energy storage. Practical Li–S cells are limited by several fundamental issues, including the low conductivity of sulfur and its reduction compounds with Li and the dissolution of long-chain lithium polysulfides (LiPS) into the electrolyte. We report on an approach that allows high-performance sulfur–carbon cathodes to be designed based on tethering polyethylenimine (PEI) polymers bearing large numbers of amine groups in every molecular unit to hydroxyl- and carboxyl-functionalized multiwall carbon nanotubes. Significantly, for the first time we show by means of direct dissolution kinetics measurements that the incorporation of CNT-PEI hybrids in a sulfur cathode stabilizes the cathode by both kinetic and thermodynamic processes. Composite sulfur cathodes based the CNT-PEI hybrids display high capacity at both low and high current rates, with capacity retention rates exceeding 90%. The attractive electrochemical performance of the materials is shown by means of DFT calculations and physical analysis to originate from three principal sources: (i) specific and strong interaction between sulfur species and amine groups in PEI; (ii) an interconnected conductive CNT substrate; and (iii) the combination of physical and thermal sequestration of LiPS provided by the CNT=PEI composite.

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