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Dithiine-linked metalphthalocyanine framework with undulated layers for highly efficient and stable H2O2 electroproduction

Author

Listed:
  • Qianjun Zhi

    (University of Science and Technology Beijing)

  • Rong Jiang

    (University of Science and Technology Beijing)

  • Xiya Yang

    (University of Science and Technology Beijing)

  • Yucheng Jin

    (University of Science and Technology Beijing)

  • Dongdong Qi

    (University of Science and Technology Beijing)

  • Kang Wang

    (University of Science and Technology Beijing)

  • Yunpeng Liu

    (Chinese Academy of Science)

  • Jianzhuang Jiang

    (University of Science and Technology Beijing)

Abstract

Realization of stable and industrial-level H2O2 electroproduction still faces great challenge due large partly to the easy decomposition of H2O2. Herein, a two-dimensional dithiine-linked phthalocyaninato cobalt (CoPc)-based covalent organic framework (COF), CoPc-S-COF, was afforded from the reaction of hexadecafluorophthalocyaninato cobalt (II) with 1,2,4,5-benzenetetrathiol. Introduction of the sulfur atoms with large atomic radius and two lone-pairs of electrons in the C-S-C linking unit leads to an undulated layered structure and an increased electron density of the Co center for CoPc-S-COF according to a series of experiments in combination with theoretical calculations. The former structural effect allows the exposition of more Co sites to enhance the COF catalytic performance, while the latter electronic effect activates the 2e− oxygen reduction reaction (2e− ORR) but deactivates the H2O2 decomposition capability of the same Co center, as a total result enabling CoPc-S-COF to display good electrocatalytic H2O2 production performance with a remarkable H2O2 selectivity of >95% and a stable H2O2 production with a concentration of 0.48 wt% under a high current density of 125 mA cm−2 at an applied potential of ca. 0.67 V versus RHE for 20 h in a flow cell, representing the thus far reported best H2O2 synthesis COFs electrocatalysts.

Suggested Citation

  • Qianjun Zhi & Rong Jiang & Xiya Yang & Yucheng Jin & Dongdong Qi & Kang Wang & Yunpeng Liu & Jianzhuang Jiang, 2024. "Dithiine-linked metalphthalocyanine framework with undulated layers for highly efficient and stable H2O2 electroproduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-44899-8
    DOI: 10.1038/s41467-024-44899-8
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    References listed on IDEAS

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    1. Huilong Fei & Juncai Dong & M. Josefina Arellano-Jiménez & Gonglan Ye & Nam Dong Kim & Errol L.G. Samuel & Zhiwei Peng & Zhuan Zhu & Fan Qin & Jiming Bao & Miguel Jose Yacaman & Pulickel M. Ajayan & D, 2015. "Atomic cobalt on nitrogen-doped graphene for hydrogen generation," Nature Communications, Nature, vol. 6(1), pages 1-8, December.
    2. Jinxing Chen & Qian Ma & Xiliang Zheng & Youxing Fang & Jin Wang & Shaojun Dong, 2022. "Kinetically restrained oxygen reduction to hydrogen peroxide with nearly 100% selectivity," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Peike Cao & Xie Quan & Xiaowa Nie & Kun Zhao & Yanming Liu & Shuo Chen & Hongtao Yu & Jingguang G. Chen, 2023. "Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. 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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