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Surpassing the single-atom catalytic activity limit through paired Pt-O-Pt ensemble built from isolated Pt1 atoms

Author

Listed:
  • Hui Wang

    (Tianjin University)

  • Jin-Xun Liu

    (University of Michigan
    University of Michigan)

  • Lawrence F. Allard

    (Oak Ridge National Laboratory)

  • Sungsik Lee

    (X-ray Science Division)

  • Jilei Liu

    (Tufts University)

  • Hang Li

    (Tianjin University)

  • Jianqiang Wang

    (Tianjin University)

  • Jun Wang

    (Tianjin University)

  • Se H. Oh

    (General Motors Global Research and Development)

  • Wei Li

    (General Motors Global Research and Development)

  • Maria Flytzani-Stephanopoulos

    (Tufts University)

  • Meiqing Shen

    (Tianjin University
    Tianjin University
    Collaborative Innovation Center of Chemical Science and Engineering)

  • Bryan R. Goldsmith

    (University of Michigan
    University of Michigan)

  • Ming Yang

    (General Motors Global Research and Development)

Abstract

Despite the maximized metal dispersion offered by single-atom catalysts, further improvement of intrinsic activity can be hindered by the lack of neighboring metal atoms in these systems. Here we report the use of isolated Pt1 atoms on ceria as “seeds” to develop a Pt-O-Pt ensemble, which is well-represented by a Pt8O14 model cluster that retains 100% metal dispersion. The Pt atom in the ensemble is 100–1000 times more active than their single-atom Pt1/CeO2 parent in catalyzing the low-temperature CO oxidation under oxygen-rich conditions. Rather than the Pt-O-Ce interfacial catalysis, the stable catalytic unit is the Pt-O-Pt site itself without participation of oxygen from the 10–30 nm-size ceria support. Similar Pt-O-Pt sites can be built on various ceria and even alumina, distinguishable by facile activation of oxygen through the paired Pt-O-Pt atoms. Extending this design to other reaction systems is a likely outcome of the findings reported here.

Suggested Citation

  • Hui Wang & Jin-Xun Liu & Lawrence F. Allard & Sungsik Lee & Jilei Liu & Hang Li & Jianqiang Wang & Jun Wang & Se H. Oh & Wei Li & Maria Flytzani-Stephanopoulos & Meiqing Shen & Bryan R. Goldsmith & Mi, 2019. "Surpassing the single-atom catalytic activity limit through paired Pt-O-Pt ensemble built from isolated Pt1 atoms," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11856-9
    DOI: 10.1038/s41467-019-11856-9
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    Cited by:

    1. Zihao Zhang & Jinshu Tian & Yubing Lu & Shize Yang & Dong Jiang & Weixin Huang & Yixiao Li & Jiyun Hong & Adam S. Hoffman & Simon R. Bare & Mark H. Engelhard & Abhaya K. Datye & Yong Wang, 2023. "Memory-dictated dynamics of single-atom Pt on CeO2 for CO oxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Tengfei Zhang & Peng Zheng & Jiajian Gao & Xiaolong Liu & Yongjun Ji & Junbo Tian & Yang Zou & Zhiyi Sun & Qiao Hu & Guokang Chen & Wenxing Chen & Xi Liu & Ziyi Zhong & Guangwen Xu & Tingyu Zhu & Fabi, 2024. "Simultaneously activating molecular oxygen and surface lattice oxygen on Pt/TiO2 for low-temperature CO oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. 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.
    4. Khandelwal, Akshat & Maarisetty, Dileep & Baral, Saroj Sundar, 2022. "Fundamentals and application of single-atom photocatalyst in sustainable energy and environmental applications," Renewable and Sustainable Energy Reviews, Elsevier, vol. 167(C).
    5. Yufei Zhao & Priyank V. Kumar & Xin Tan & Xinxin Lu & Xiaofeng Zhu & Junjie Jiang & Jian Pan & Shibo Xi & Hui Ying Yang & Zhipeng Ma & Tao Wan & Dewei Chu & Wenjie Jiang & Sean C. Smith & Rose Amal & , 2022. "Modulating Pt-O-Pt atomic clusters with isolated cobalt atoms for enhanced hydrogen evolution catalysis," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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