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Harnessing strong metal–support interactions via a reverse route

Author

Listed:
  • Peiwen Wu

    (Oak Ridge National Laboratory
    Jiangsu University)

  • Shuai Tan

    (Oak Ridge National Laboratory)

  • Jisue Moon

    (Oak Ridge National Laboratory)

  • Zihao Yan

    (Virginia Polytechnic Institute and State University)

  • Victor Fung

    (University of California)

  • Na Li

    (Brookhaven National Laboratory
    Xi’an Jiaotong University)

  • Shi-Ze Yang

    (Oak Ridge National Laboratory)

  • Yongqiang Cheng

    (Oak Ridge National Laboratory)

  • Carter W. Abney

    (Oak Ridge National Laboratory)

  • Zili Wu

    (Oak Ridge National Laboratory)

  • Aditya Savara

    (Oak Ridge National Laboratory)

  • Ayyoub M. Momen

    (Oak Ridge National Laboratory)

  • De-en Jiang

    (University of California)

  • Dong Su

    (Brookhaven National Laboratory)

  • Huaming Li

    (Jiangsu University)

  • Wenshuai Zhu

    (Jiangsu University)

  • Sheng Dai

    (Oak Ridge National Laboratory
    University of Tennessee)

  • Huiyuan Zhu

    (Oak Ridge National Laboratory
    Virginia Polytechnic Institute and State University)

Abstract

Engineering strong metal–support interactions (SMSI) is an effective strategy for tuning structures and performances of supported metal catalysts but induces poor exposure of active sites. Here, we demonstrate a strong metal–support interaction via a reverse route (SMSIR) by starting from the final morphology of SMSI (fully-encapsulated core–shell structure) to obtain the intermediate state with desirable exposure of metal sites. Using core–shell nanoparticles (NPs) as a building block, the Pd–FeOx NPs are transformed into a porous yolk–shell structure along with the formation of SMSIR upon treatment under a reductive atmosphere. The final structure, denoted as Pd–Fe3O4–H, exhibits excellent catalytic performance in semi-hydrogenation of acetylene with 100% conversion and 85.1% selectivity to ethylene at 80 °C. Detailed electron microscopic and spectroscopic experiments coupled with computational modeling demonstrate that the compelling performance stems from the SMSIR, favoring the formation of surface hydrogen on Pd instead of hydride.

Suggested Citation

  • Peiwen Wu & Shuai Tan & Jisue Moon & Zihao Yan & Victor Fung & Na Li & Shi-Ze Yang & Yongqiang Cheng & Carter W. Abney & Zili Wu & Aditya Savara & Ayyoub M. Momen & De-en Jiang & Dong Su & Huaming Li , 2020. "Harnessing strong metal–support interactions via a reverse route," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-16674-y
    DOI: 10.1038/s41467-020-16674-y
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    Cited by:

    1. Jia Zhao & Ricardo Urrego-Ortiz & Nan Liao & Federico Calle-Vallejo & Jingshan Luo, 2024. "Rationally designed Ru catalysts supported on TiN for highly efficient and stable hydrogen evolution in alkaline conditions," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    2. Lei Zhang & Zhe Chen & Zhenpeng Liu & Jun Bu & Wenxiu Ma & Chen Yan & Rui Bai & Jin Lin & Qiuyu Zhang & Junzhi Liu & Tao Wang & Jian Zhang, 2021. "Efficient electrocatalytic acetylene semihydrogenation by electron–rich metal sites in N–heterocyclic carbene metal complexes," Nature Communications, Nature, vol. 12(1), pages 1-9, December.

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