A Highly Conductive COF@CNT Electrocatalyst Boosting Polysulfide Conversion for Li-S Chemistry

Jie Xu, Weiqiang Tang, Chao Yang, Ingo Manke, Nan Chen, Feili Lai, Ting Xu, Shuhao An*, Honglai Liu, Zhiliang Zhang, Yongjie Cao, Nan Wang, Shuangliang Zhao, Dongfang Niu*, Renjie Chen*

*Corresponding author for this work

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Abstract

The catalysis of covalent organic frameworks (COFs) in Li-S chemistry is largely blocked by a weak chemical interaction and low conductivity. Herein, a new kind of diketopyrrolopyrrole (DPP)-based COF is in situ fabricated onto the carbon nanotube (CNT) surface (denoted as COF@CNT) to uncover the electrocatalysis behavior by its strong chemical interaction and highly conductive property. We declare that the electrocatalytic activity of DPP-COF can be maximized by introducing an appropriate content of CNT (66 wt %); the analyses including density functional theory calculations, X-ray photoelectron spectroscopy, Fourier transform infrared, and Raman show that the DPP moiety can mediate the conversion of polysulfides contributed by a CO/C-O bonding conversion. Hence, the modified battery shows a 0.042% decay rate over 1000 cycles and achieves a desirable capacity of 8.7 mAh cm-2 with 10 mg cm-2 sulfur loading and lean electrolyte (E/S = 5). This work will inspire the rational design of COF@support hybrids for various electrocatalysis applications.

Original languageEnglish
Pages (from-to)3053-3062
Number of pages10
JournalACS Energy Letters
Volume6
Issue number9
DOIs
Publication statusPublished - 10 Sept 2021

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Xu, J., Tang, W., Yang, C., Manke, I., Chen, N., Lai, F., Xu, T., An, S., Liu, H., Zhang, Z., Cao, Y., Wang, N., Zhao, S., Niu, D., & Chen, R. (2021). A Highly Conductive COF@CNT Electrocatalyst Boosting Polysulfide Conversion for Li-S Chemistry. ACS Energy Letters, 6(9), 3053-3062. https://doi.org/10.1021/acsenergylett.1c00943