Oxygen-Plasma-Treated Fe-N-C Catalysts with Dual Binding Sites for Enhanced Electrocatalytic Polysulfide Conversion in Lithium-Sulfur Batteries

Euiyeon Jung, Seong Jun Kim, Jiheon Kim, Sojung Koo, Jaewoo Lee, Shin Yeong Kim, Vinod K. Paidi, Wonjae Ko, Junseok Moon, Kug Seung Lee, Sung Pyo Cho, Duho Kim, Seung Ho Yu, Yung Eun Sung, Taeghwan Hyeon

    Research output: Contribution to journalArticlepeer-review

    41 Citations (Scopus)

    Abstract

    Enhanced polysulfide conversion kinetics is essential for realizing lithium-sulfur batteries with high energy density and rate performance and promising cyclability. The modification of the local atomic structure of MNxactive sites in single-atom M-N-C catalysts was proposed to improve their electrocatalytic activity for demanding reactions by fine-tuning the interaction with reaction intermediates. Here, we demonstrate that engineering the binding geometry of lithium polysulfides (LiPSs) by introducing dual binding sites improves the LiPS conversion kinetics. We use mild oxygen plasma treatment to introduce oxygen species into the Fe-N-C catalyst. The plasma-treated Fe-N-C (pFeNG) catalyst with dual sulfiphilic (mononuclear iron) and lithiophilic (oxygen) binding sites has a lower polysulfide decomposition energy, especially for Li2S redox, which is known to be the most sluggish process. The pFeNG cathode shows significant improvement, especially at high C rates (916.3 mA h g-1at 5C), with promising cycling performance.

    Original languageEnglish
    Pages (from-to)2646-2653
    Number of pages8
    JournalACS Energy Letters
    Volume7
    Issue number8
    DOIs
    Publication statusPublished - 2022 Aug 12

    Bibliographical note

    Funding Information:
    T.H. and Y.-E.S. acknowledge the Institute for Basic Science (T.H.: IBS-R006-D1 and Y.-E.S.: IBS-R006-A2) for financial support. S.-H.Y. acknowledges support from the National Research Foundation of Korea (NRF) grant funded by the Korean Government (MSIT) (NRF-2020R1C1C1012308). D.K. acknowledges the Korea Government (MSIT) for support from the National Research Foundation of Korea (grant no. NRF-2022M3J7A1062940). XAS measurements at the 8C beamline of Pohang Accelerator Laboratory were supported by the National Research Foundation of Korea (grant no. NRF-2019M3D1A1079309). We thank the Korea Basic Science Institute at Busan center for the XPS measurements.

    Publisher Copyright:
    © 2022 American Chemical Society. All rights reserved.

    ASJC Scopus subject areas

    • Chemistry (miscellaneous)
    • Renewable Energy, Sustainability and the Environment
    • Fuel Technology
    • Energy Engineering and Power Technology
    • Materials Chemistry

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