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

doi:10.1021/acsenergylett.2c01132

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 journal › Article › peer-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 MN_xactive 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 language	English
Pages (from-to)	2646-2653
Number of pages	8
Journal	ACS Energy Letters
Volume	7
Issue number	8
DOIs	https://doi.org/10.1021/acsenergylett.2c01132
Publication status	Published - 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

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsenergylett.2c01132

Cite this

Jung, E., Kim, S. J., Kim, J., Koo, S., Lee, J., Kim, S. Y., Paidi, V. K., Ko, W., Moon, J., Lee, K. S., Cho, S. P., Kim, D., Yu, S. H., Sung, Y. E., & Hyeon, T. (2022). Oxygen-Plasma-Treated Fe-N-C Catalysts with Dual Binding Sites for Enhanced Electrocatalytic Polysulfide Conversion in Lithium-Sulfur Batteries. ACS Energy Letters, 7(8), 2646-2653. https://doi.org/10.1021/acsenergylett.2c01132

Jung, E, Kim, SJ, Kim, J, Koo, S, Lee, J, Kim, SY, Paidi, VK, Ko, W, Moon, J, Lee, KS, Cho, SP, Kim, D, Yu, SH, Sung, YE & Hyeon, T 2022, 'Oxygen-Plasma-Treated Fe-N-C Catalysts with Dual Binding Sites for Enhanced Electrocatalytic Polysulfide Conversion in Lithium-Sulfur Batteries', ACS Energy Letters, vol. 7, no. 8, pp. 2646-2653. https://doi.org/10.1021/acsenergylett.2c01132

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

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.",

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

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: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

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doi = "10.1021/acsenergylett.2c01132",

language = "English",

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AU - Jung, Euiyeon

AU - Kim, Seong Jun

AU - Kim, Jiheon

AU - Koo, Sojung

AU - Lee, Jaewoo

AU - Kim, Shin Yeong

AU - Paidi, Vinod K.

AU - Ko, Wonjae

AU - Moon, Junseok

AU - Lee, Kug Seung

AU - Cho, Sung Pyo

AU - Kim, Duho

AU - Yu, Seung Ho

AU - Sung, Yung Eun

AU - Hyeon, Taeghwan

N1 - 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.

PY - 2022/8/12

Y1 - 2022/8/12

N2 - 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.

AB - 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.

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

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

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