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Unraveling the coordination structure-performance relationship in Pt1/Fe2O3 single-atom catalyst

Author

Listed:
  • Yujing Ren

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Yan Tang

    (Tsinghua University)

  • Leilei Zhang

    (Chinese Academy of Sciences)

  • Xiaoyan Liu

    (Chinese Academy of Sciences)

  • Lin Li

    (Chinese Academy of Sciences)

  • Shu Miao

    (Chinese Academy of Sciences)

  • Dang Sheng Su

    (Chinese Academy of Sciences)

  • Aiqin Wang

    (Chinese Academy of Sciences)

  • Jun Li

    (Tsinghua University
    Southern University of Science and Technology)

  • Tao Zhang

    (Chinese Academy of Sciences)

Abstract

Heterogeneous single-atom catalyst (SAC) opens a unique entry to establishing structure–performance relationship at the molecular level similar to that in homogeneous catalysis. The challenge lies in manipulating the coordination chemistry of single atoms without changing single-atom dispersion. Here, we develop an efficient synthetic method for SACs by using ethanediamine to chelate Pt cations and then removing the ethanediamine by a rapid thermal treatment (RTT) in inert atmosphere. The coordination chemistry of Pt single atoms on a Fe2O3 support is finely tuned by merely adjusting the RTT temperature. With the decrease in Pt-O coordination number, the oxidation state of Pt decreases, and consequently the hydrogenation activity increases to a record level without loss of chemoselectivity. The tunability of the local coordination chemistry, oxidation states of the metal, and the catalytic performance of single atoms reveals the unique role of SACs as a bridge between heterogeneous and homogeneous catalysis.

Suggested Citation

  • Yujing Ren & Yan Tang & Leilei Zhang & Xiaoyan Liu & Lin Li & Shu Miao & Dang Sheng Su & Aiqin Wang & Jun Li & Tao Zhang, 2019. "Unraveling the coordination structure-performance relationship in Pt1/Fe2O3 single-atom catalyst," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12459-0
    DOI: 10.1038/s41467-019-12459-0
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    Cited by:

    1. Jingyi Yang & Yike Huang & Haifeng Qi & Chaobin Zeng & Qike Jiang & Yitao Cui & Yang Su & Xiaorui Du & Xiaoli Pan & Xiaoyan Liu & Weizhen Li & Botao Qiao & Aiqin Wang & Tao Zhang, 2022. "Modulating the strong metal-support interaction of single-atom catalysts via vicinal structure decoration," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Jiajing Pei & Huishan Shang & Junjie Mao & Zhe Chen & Rui Sui & Xuejiang Zhang & Danni Zhou & Yu Wang & Fang Zhang & Wei Zhu & Tao Wang & Wenxing Chen & Zhongbin Zhuang, 2024. "A replacement strategy for regulating local environment of single-atom Co-SxN4−x catalysts to facilitate CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Ruiling Zhang & Yaozhou Li & Xuan Zhou & Ao Yu & Qi Huang & Tingting Xu & Longtao Zhu & Ping Peng & Shuyan Song & Luis Echegoyen & Fang-Fang Li, 2023. "Single-atomic platinum on fullerene C60 surfaces for accelerated alkaline hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Huaning Jiang & Weiwei Yang & Mingquan Xu & Erqing Wang & Yi Wei & Wei Liu & Xiaokang Gu & Lixuan Liu & Qian Chen & Pengbo Zhai & Xiaolong Zou & Pulickel M. Ajayan & Wu Zhou & Yongji Gong, 2022. "Single atom catalysts in Van der Waals gaps," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    5. Tianyu Zhang & Jing Jin & Junmei Chen & Yingyan Fang & Xu Han & Jiayi Chen & Yaping Li & Yu Wang & Junfeng Liu & Lei Wang, 2022. "Pinpointing the axial ligand effect on platinum single-atom-catalyst towards efficient alkaline hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    6. Wei Liu & Haisong Feng & Yusen Yang & Yiming Niu & Lei Wang & Pan Yin & Song Hong & Bingsen Zhang & Xin Zhang & Min Wei, 2022. "Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    7. 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.
    8. Dong Cao & Haoxiang Xu & Hongliang Li & Chen Feng & Jie Zeng & Daojian Cheng, 2022. "Volcano-type relationship between oxidation states and catalytic activity of single-atom catalysts towards hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    9. Yan Shen & Chunjin Ren & Lirong Zheng & Xiaoyong Xu & Ran Long & Wenqing Zhang & Yong Yang & Yongcai Zhang & Yingfang Yao & Haoqiang Chi & Jinlan Wang & Qing Shen & Yujie Xiong & Zhigang Zou & Yong Zh, 2023. "Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    10. Jie Wei & Hua Tang & Li Sheng & Ruyang Wang & Minghui Fan & Jiale Wan & Yuheng Wu & Zhirong Zhang & Shiming Zhou & Jie Zeng, 2024. "Site-specific metal-support interaction to switch the activity of Ir single atoms for oxygen evolution reaction," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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