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Monosymmetric Fe-N4 sites enabling durable proton exchange membrane fuel cell cathode by chemical vapor modification

Author

Listed:
  • Jingsen Bai

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Tuo Zhao

    (FAW Jiefang Automotive CO.LTD.)

  • Mingjun Xu

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Bingbao Mei

    (Chinese Academy of Sciences)

  • Liting Yang

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Zhaoping Shi

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Siyuan Zhu

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Ying Wang

    (Chinese Academy of Sciences)

  • Zheng Jiang

    (University of Science and Technology of China)

  • Jin Zhao

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Junjie Ge

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Meiling Xiao

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Changpeng Liu

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Wei Xing

    (Chinese Academy of Sciences
    University of Science and Technology of China)

Abstract

The limited durability of metal-nitrogen-carbon electrocatalysts severely restricts their applicability for the oxygen reduction reaction in proton exchange membrane fuel cells. In this study, we employ the chemical vapor modification method to alter the configuration of active sites from FeN4 to the stable monosymmetric FeN2+N’2, along with enhancing the degree of graphitization in the carbon substrate. This improvement effectively addresses the challenges associated with Fe active center leaching caused by N-group protonation and free radicals attack due to the 2-electron oxygen reduction reaction. The electrocatalyst with neoteric active site exhibited excellent durability. During accelerated aging test, the electrocatalyst exhibited negligible decline in its half-wave potential even after undergoing 200,000 potential cycles. Furthermore, when subjected to operational conditions representative of fuel cell systems, the electrocatalyst displayed remarkable durability, sustaining stable performance for a duration exceeding 248 h. The significant improvement in durability provides highly valuable insights for the practical application of metal-nitrogen-carbon electrocatalysts.

Suggested Citation

  • Jingsen Bai & Tuo Zhao & Mingjun Xu & Bingbao Mei & Liting Yang & Zhaoping Shi & Siyuan Zhu & Ying Wang & Zheng Jiang & Jin Zhao & Junjie Ge & Meiling Xiao & Changpeng Liu & Wei Xing, 2024. "Monosymmetric Fe-N4 sites enabling durable proton exchange membrane fuel cell cathode by chemical vapor modification," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47817-0
    DOI: 10.1038/s41467-024-47817-0
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    References listed on IDEAS

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    1. Gege Yang & Jiawei Zhu & Pengfei Yuan & Yongfeng Hu & Gan Qu & Bang-An Lu & Xiaoyi Xue & Hengbo Yin & Wenzheng Cheng & Junqi Cheng & Wenjing Xu & Jin Li & Jinsong Hu & Shichun Mu & Jia-Nan Zhang, 2021. "Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    2. Hua Xie & Xiaohong Xie & Guoxiang Hu & Venkateshkumar Prabhakaran & Sulay Saha & Lorelis Gonzalez-Lopez & Abhijit H. Phakatkar & Min Hong & Meiling Wu & Reza Shahbazian-Yassar & Vijay Ramani & Mohamad, 2022. "Ta–TiOx nanoparticles as radical scavengers to improve the durability of Fe–N–C oxygen reduction catalysts," Nature Energy, Nature, vol. 7(3), pages 281-289, March.
    3. Shengwen Liu & Chenzhao Li & Michael J. Zachman & Yachao Zeng & Haoran Yu & Boyang Li & Maoyu Wang & Jonathan Braaten & Jiawei Liu & Harry M. Meyer & Marcos Lucero & A. Jeremy Kropf & E. Ercan Alp & Q, 2022. "Atomically dispersed iron sites with a nitrogen–carbon coating as highly active and durable oxygen reduction catalysts for fuel cells," Nature Energy, Nature, vol. 7(7), pages 652-663, July.
    4. Long Jiao & Rui Zhang & Gang Wan & Weijie Yang & Xin Wan & Hua Zhou & Jianglan Shui & Shu-Hong Yu & Hai-Long Jiang, 2020. "Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    5. Huishan Shang & Xiangyi Zhou & Juncai Dong & Ang Li & Xu Zhao & Qinghua Liu & Yue Lin & Jiajing Pei & Zhi Li & Zhuoli Jiang & Danni Zhou & Lirong Zheng & Yu Wang & Jing Zhou & Zhengkun Yang & Rui Cao , 2020. "Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    6. Yang Xia & Xunhua Zhao & Chuan Xia & Zhen-Yu Wu & Peng Zhu & Jung Yoon (Timothy) Kim & Xiaowan Bai & Guanhui Gao & Yongfeng Hu & Jun Zhong & Yuanyue Liu & Haotian Wang, 2021. "Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production rates," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
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