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Nitrogen-Doping Through Two-Step Pyrolysis of Polyacrylonitrile on Graphite Felts for Vanadium Redox Flow Batteries
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    Nitrogen-Doping Through Two-Step Pyrolysis of Polyacrylonitrile on Graphite Felts for Vanadium Redox Flow Batteries
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    • Sang Jun Yoon*
      Sang Jun Yoon
      Energy Materials Research Center, Korea Research Institute of Chemical Technology (KRICT), Daejeon 34114, South Korea
      Transfercentre Sustainable Electrochemistry, Saarland University, Saarbrücken 66123, Germany
      *Email: [email protected]
    • Sangwon Kim
      Sangwon Kim
      Bio Sensor Group, Korea Institute of Science and Technology Europe (KIST−EU), Saarbrücken 66123, Germany
      More by Sangwon Kim
    • Dong Kyu Kim
      Dong Kyu Kim
      School of Mechanical Engineering, Chung-Ang University, Seoul 06974, South Korea
      More by Dong Kyu Kim
    • Duk Man Yu
      Duk Man Yu
      Energy Materials Research Center, Korea Research Institute of Chemical Technology (KRICT), Daejeon 34114, South Korea
      More by Duk Man Yu
    • Rolf Hempelmann
      Rolf Hempelmann
      Transfercentre Sustainable Electrochemistry, Saarland University, Saarbrücken 66123, Germany
    • Young Taik Hong
      Young Taik Hong
      Energy Materials Research Center, Korea Research Institute of Chemical Technology (KRICT), Daejeon 34114, South Korea
    • Soonyong So*
      Soonyong So
      Energy Materials Research Center, Korea Research Institute of Chemical Technology (KRICT), Daejeon 34114, South Korea
      *Email: [email protected]
      More by Soonyong So
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    Energy & Fuels

    Cite this: Energy Fuels 2020, 34, 4, 5052–5059
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    https://doi.org/10.1021/acs.energyfuels.0c00689
    Published March 24, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    We report a facile method for the nitrogen-doping process using the same precursor material for graphite felt electrodes, polyacrylonitrile (PAN). To utilize the nitrogen content in PAN, two steps of thermal treatment of PAN-coated graphite felts are performed; a PAN solution is coated on a graphite felt, and the sample is oxidized at 280 °C under the ambient atmosphere and carbonized at 900 °C under N2, consecutively. Through the two-step pyrolysis, nitrogen is successfully doped on the graphite felts, and the concentration of PAN solution is controlled to enhance the performance of vanadium redox flow batteries (VRFBs). With 4 wt % of PAN coating solution, the electrode electrocatalytic activity is enhanced compared to that of a conventional electrode, and the voltage efficiency increases, resulting in higher energy efficiency under the various current densities. Especially at high current densities above 100 mA/cm2, the optimized nitrogen-doped electrode shows about 5% higher voltage and energy efficiencies and a higher long-term stability in terms of efficiencies and capacity retention. This nitrogen-doping process with the same precursor for the electrode offers potential for employing nitrogen-doping on the conventional electrode materials in an inexpensive way.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.energyfuels.0c00689.

    • Weight gain of electrodes depending on the PAN concentration; cyclic voltammograms of GF-ref, GF-P1, and GF-P4 at a scan rate of 2, 30, 50, and 120 mV/s; cycling performance of VRFBs employing GF-ref and O-GF-P0.5; cycling performance of VRFBs employing GF-ref, C-GF-P0.5, and C-GF-P1 at different current densities; and charge/discharge curves for VRFBs employing GF-ref and O-GF-P0.5 and employing GF-ref, C-GF-P0.5, and C-GF-P1 at the current density of 100 mA/cm2 (PDF)

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    This article is cited by 14 publications.

    1. Penghua Qian, Wanhai Zhou, Yuxia Zhang, Dongliang Chao, Ming Song. Review and Perspectives of Sulfonated Poly(ether ether ketone) Proton Exchange Membrane for Vanadium Flow Batteries. Energy & Fuels 2023, 37 (23) , 17681-17707. https://doi.org/10.1021/acs.energyfuels.3c02373
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    5. Huishan Chen, Sen Li, Yongxin Zhao, Xinyue Li, Hui Zhao, Longzhen Cheng, Renting Li, Pengcheng Dai. Carbon Felts Uniformly Modified with Bismuth Nanoparticles for Efficient Vanadium Redox Flow Batteries. Nanomaterials 2024, 14 (24) , 2055. https://doi.org/10.3390/nano14242055
    6. Sophie McArdle, Holger Fiedler, Jérôme Leveneur, John Kennedy, Aaron T. Marshall. Novel ion beam implantation of felt electrodes for the vanadium flow battery: Role of defects versus nitrogen groups for the VO2+/VO2+ redox reaction. Journal of Power Sources 2024, 608 , 234614. https://doi.org/10.1016/j.jpowsour.2024.234614
    7. Sophie McArdle, Felix Bauer, Simone Fiorini Granieri, Marius Ast, Fabio Di Fonzo, Aaron T. Marshall, Hannes Radinger. Defective Carbon for Next‐Generation Stationary Energy Storage Systems: Sodium‐Ion and Vanadium Flow Batteries. ChemElectroChem 2024, 11 (4) https://doi.org/10.1002/celc.202300512
    8. Shaotian Qi, Lei Dai, Wenjie Huo, Yingqiao Jiang, Sujuan Yuan, Yanna Xiao, Yongguang Liu, Ling Wang, Zhangxing He. Doping engineering strategies for electrodes and catalysts in vanadium redox flow battery. Composites Part B: Engineering 2023, 265 , 110947. https://doi.org/10.1016/j.compositesb.2023.110947
    9. Jianxiang Deng, Xinghua Cai, Chengde Huang. N, B codoped graphite felt for high‐performance 1,8‐dihydroxyanthraquinone redox flow battery. Energy Storage 2023, 5 (5) https://doi.org/10.1002/est2.435
    10. Cong Ding, Zhefei Shen, Ying Zhu, Yuanhui Cheng. Insights into the Modification of Carbonous Felt as an Electrode for Vanadium Redox Flow Batteries. Materials 2023, 16 (10) , 3811. https://doi.org/10.3390/ma16103811
    11. Sophie McArdle, Aaron T. Marshall. Why electrode orientation and carbon felt heterogeneity can influence the performance of flow batteries. Journal of Power Sources 2023, 562 , 232755. https://doi.org/10.1016/j.jpowsour.2023.232755
    12. Xuejiao Liu, Junping Hu, Jun Liu, Hongyi Liu, Sha Fu, Xiongwei Wu, Yuping Wu. Graphite Felt Electrode Modified by Quaternary Ammonium for Vanadium Redox Flow Battery with an Ultra-Long Cycle Life. Inorganics 2022, 10 (11) , 208. https://doi.org/10.3390/inorganics10110208
    13. Hoang X. Dang, Dominik P.J. Barz. Graphene electrode functionalization for high performance hybrid energy storage with vanadyl sulfate redox electrolytes. Journal of Power Sources 2022, 517 , 230712. https://doi.org/10.1016/j.jpowsour.2021.230712
    14. Tomofumi Kato, Yasuhiro Yamada, Yasushi Nishikawa, Toshiya Otomo, Hayato Sato, Satoshi Sato. Origins of peaks of graphitic and pyrrolic nitrogen in N1s X-ray photoelectron spectra of carbon materials: quaternary nitrogen, tertiary amine, or secondary amine?. Journal of Materials Science 2021, 56 (28) , 15798-15811. https://doi.org/10.1007/s10853-021-06283-5

    Energy & Fuels

    Cite this: Energy Fuels 2020, 34, 4, 5052–5059
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.energyfuels.0c00689
    Published March 24, 2020
    Copyright © 2020 American Chemical Society

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