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The simplest construction of single-site catalysts by the synergism of micropore trapping and nitrogen anchoring

Author

Listed:
  • Zhiqi Zhang

    (Nanjing University)

  • Yugang Chen

    (Nanjing University)

  • Liqi Zhou

    (Nanjing University)

  • Chi Chen

    (Chinese Academy of Sciences)

  • Zhen Han

    (Nanjing University)

  • Bingsen Zhang

    (Institute of Metal Research, Chinese Academy of Sciences)

  • Qiang Wu

    (Nanjing University)

  • Lijun Yang

    (Nanjing University)

  • Lingyu Du

    (Nanjing University)

  • Yongfeng Bu

    (Nanjing University)

  • Peng Wang

    (Nanjing University
    Nanjing University)

  • Xizhang Wang

    (Nanjing University)

  • Hui Yang

    (Chinese Academy of Sciences)

  • Zheng Hu

    (Nanjing University)

Abstract

Single-site catalysts feature high catalytic activity but their facile construction and durable utilization are highly challenging. Herein, we report a simple impregnation-adsorption method to construct platinum single-site catalysts by synergic micropore trapping and nitrogen anchoring on hierarchical nitrogen-doped carbon nanocages. The optimal catalyst exhibits a record-high electrocatalytic hydrogen evolution performance with low overpotential, high mass activity and long stability, much superior to the platinum-based catalysts to date. Theoretical simulations and experiments reveal that the micropores with edge-nitrogen-dopants favor the formation of isolated platinum atoms by the micropore trapping and nitrogen anchoring of [PtCl6]2-, followed by the spontaneous dechlorination. The platinum-nitrogen bonds are more stable than the platinum-carbon ones in the presence of adsorbed hydrogen atoms, leading to the superior hydrogen evolution stability of platinum single-atoms on nitrogen-doped carbon. This method has been successfully applied to construct the single-site catalysts of other precious metals such as palladium, gold and iridium.

Suggested Citation

  • Zhiqi Zhang & Yugang Chen & Liqi Zhou & Chi Chen & Zhen Han & Bingsen Zhang & Qiang Wu & Lijun Yang & Lingyu Du & Yongfeng Bu & Peng Wang & Xizhang Wang & Hui Yang & Zheng Hu, 2019. "The simplest construction of single-site catalysts by the synergism of micropore trapping and nitrogen anchoring," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-09596-x
    DOI: 10.1038/s41467-019-09596-x
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    Cited by:

    1. Yang Si & Yueyue Jiao & Maolin Wang & Shengling Xiang & Jiangyong Diao & Xiaowen Chen & Jiawei Chen & Yue Wang & Dequan Xiao & Xiaodong Wen & Ning Wang & Ding Ma & Hongyang Liu, 2024. "Fully exposed Pt clusters for efficient catalysis of multi-step hydrogenation reactions," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Shengtai Hou & Xuefeng Ma & Yuan Shu & Jiafeng Bao & Qiuyue Zhang & Mingshu Chen & Pengfei Zhang & Sheng Dai, 2021. "Self-regeneration of supported transition metals by a high entropy-driven principle," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    3. Liang Shen & Minghui Zhu & Jing Xu, 2021. "Effect of micropores on the structure and CO2 methanation performance of supported Ni/SiO2 catalyst," Greenhouse Gases: Science and Technology, Blackwell Publishing, vol. 11(6), pages 1213-1221, December.

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