IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-47817-0.html
   My bibliography  Save this article

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
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-47817-0
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-47817-0?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    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.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Xiao Zhou & Yuan Min & Changming Zhao & Cai Chen & Ming-Kun Ke & Shi-Lin Xu & Jie-Jie Chen & Yuen Wu & Han-Qing Yu, 2024. "Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Xin Zhao & Ruiqi Fang & Fengliang Wang & Xiangpeng Kong & Yingwei Li, 2022. "Atomic design of dual-metal hetero-single-atoms for high-efficiency synthesis of natural flavones," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Hongqiang Jin & Peipei Li & Peixin Cui & Jinan Shi & Wu Zhou & Xiaohu Yu & Weiguo Song & Changyan Cao, 2022. "Unprecedentedly high activity and selectivity for hydrogenation of nitroarenes with single atomic Co1-N3P1 sites," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Wei Peng & Jiaxin Liu & Xiaoqing Liu & Liqun Wang & Lichang Yin & Haotian Tan & Feng Hou & Ji Liang, 2023. "Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Zhimeng Tang & Lei Xu & Cheng Xie & Lirong Guo & Libo Zhang & Shenghui Guo & Jinhui Peng, 2023. "Synthesis of CuCo2S4@Expanded Graphite with crystal/amorphous heterointerface and defects for electromagnetic wave absorption," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    6. Yao-Jie Lei & Xinxin Lu & Hirofumi Yoshikawa & Daiju Matsumura & Yameng Fan & Lingfei Zhao & Jiayang Li & Shijian Wang & Qinfen Gu & Hua-Kun Liu & Shi-Xue Dou & Shanmukaraj Devaraj & Teofilo Rojo & We, 2024. "Understanding the charge transfer effects of single atoms for boosting the performance of Na-S batteries," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    7. Meihuan Liu & Jing Zhang & Hui Su & Yaling Jiang & Wanlin Zhou & Chenyu Yang & Shuowen Bo & Jun Pan & Qinghua Liu, 2024. "In situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    8. Siran Xu & Sihua Feng & Yue Yu & Dongping Xue & Mengli Liu & Chao Wang & Kaiyue Zhao & Bingjun Xu & Jia-Nan Zhang, 2024. "Dual-site segmentally synergistic catalysis mechanism: boosting CoFeSx nanocluster for sustainable water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    9. Jun Qi & Yadong Du & Qi Yang & Na Jiang & Jiachun Li & Yi Ma & Yangjun Ma & Xin Zhao & Jieshan Qiu, 2023. "Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    10. Deyou Yu & Licong Xu & Kaixing Fu & Xia Liu & Shanli Wang & Minghua Wu & Wangyang Lu & Chunyu Lv & Jinming Luo, 2024. "Electronic structure modulation of iron sites with fluorine coordination enables ultra-effective H2O2 activation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    11. Kejun Bu & Qingyang Hu & Xiaohuan Qi & Dong Wang & Songhao Guo & Hui Luo & Tianquan Lin & Xiaofeng Guo & Qiaoshi Zeng & Yang Ding & Fuqiang Huang & Wenge Yang & Ho-Kwang Mao & Xujie Lü, 2022. "Nested order-disorder framework containing a crystalline matrix with self-filled amorphous-like innards," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    12. Juncai Dong & Yangyang Liu & Jiajing Pei & Haijing Li & Shufang Ji & Lei Shi & Yaning Zhang & Can Li & Cheng Tang & Jiangwen Liao & Shiqing Xu & Huabin Zhang & Qi Li & Shenlong Zhao, 2023. "Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    13. Liangbo Xie & Pengfei Wang & Yi Li & Dongpeng Zhang & Denghui Shang & Wenwen Zheng & Yuguo Xia & Sihui Zhan & Wenping Hu, 2022. "Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N–CuO for organic pollutants degradation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    14. Lin, P.Z. & Sun, J. & He, C.X. & Wu, M.C. & Zhao, T.S., 2024. "Modeling proton exchange membrane fuel cells with platinum-group-metal-free catalysts," Applied Energy, Elsevier, vol. 360(C).
    15. Arthur G. Fink & Roxanna S. Delima & Alexandra R. Rousseau & Camden Hunt & Natalie E. LeSage & Aoxue Huang & Monika Stolar & Curtis P. Berlinguette, 2024. "Indirect H2O2 synthesis without H2," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    16. Guo, Bingran & Guo, Jianing & Yang, Wenlu & Tian, Xiyao & Wang, Xi & Xiang, Zhonghua & Wu, Mingxing, 2022. "Highly dispersed iron/nickel dual-sites in hierarchical porous carbon materials as high-performance bifunctional oxygen electrocatalysts for Zn-air batteries," Renewable Energy, Elsevier, vol. 201(P2), pages 117-124.
    17. Xingkun Wang & Liangliang Xu & Cheng Li & Canhui Zhang & Hanxu Yao & Ren Xu & Peixin Cui & Xusheng Zheng & Meng Gu & Jinwoo Lee & Heqing Jiang & Minghua Huang, 2023. "Developing a class of dual atom materials for multifunctional catalytic reactions," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    18. Cong Fang & Jian Zhou & Lili Zhang & Wenchao Wan & Yuxiao Ding & Xiaoyan Sun, 2023. "Synergy of dual-atom catalysts deviated from the scaling relationship for oxygen evolution reaction," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    19. Jinfa Chang & Guanzhi Wang & Xiaoxia Chang & Zhenzhong Yang & Han Wang & Boyang Li & Wei Zhang & Libor Kovarik & Yingge Du & Nina Orlovskaya & Bingjun Xu & Guofeng Wang & Yang Yang, 2023. "Interface synergism and engineering of Pd/Co@N-C for direct ethanol fuel cells," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    20. Yangyang Liu & Can Li & Chunhui Tan & Zengxia Pei & Tao Yang & Shuzhen Zhang & Qianwei Huang & Yihan Wang & Zheng Zhou & Xiaozhou Liao & Juncai Dong & Hao Tan & Wensheng Yan & Huajie Yin & Zhao-Qing L, 2023. "Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47817-0. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.