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Defect-driven nanostructuring of low-nuclearity Pt-Mo ensembles for continuous gas-phase formic acid dehydrogenation

Author

Listed:
  • Luyao Guo

    (Zhejiang Normal University
    Chinese Academy of Sciences
    Dalian University of Technology)

  • Kaixuan Zhuge

    (Zhejiang University of Technology)

  • Siyang Yan

    (Dalian University of Technology)

  • Shiyi Wang

    (Zhejiang Normal University)

  • Jia Zhao

    (Zhejiang University of Technology)

  • Saisai Wang

    (Zhejiang University of Technology)

  • Panzhe Qiao

    (Chinese Academy of Sciences)

  • Jiaxu Liu

    (Dalian University of Technology)

  • Xiaoling Mou

    (Zhejiang Normal University
    Zhejiang Normal University)

  • Hejun Zhu

    (Chinese Academy of Sciences)

  • Ziang Zhao

    (Chinese Academy of Sciences)

  • Li Yan

    (Chinese Academy of Sciences)

  • Ronghe Lin

    (Zhejiang Normal University
    Zhejiang Normal University)

  • Yunjie Ding

    (Zhejiang Normal University
    Chinese Academy of Sciences
    Chinese Academy of Sciences)

Abstract

Supported metal clusters comprising of well-tailored low-nuclearity heteroatoms have great potentials in catalysis owing to the maximized exposure of active sites and metal synergy. However, atomically precise design of these architectures is still challenging for the lack of practical approaches. Here, we report a defect-driven nanostructuring strategy through combining defect engineering of nitrogen-doped carbons and sequential metal depositions to prepare a series of Pt and Mo ensembles ranging from single atoms to sub-nanoclusters. When applied in continuous gas-phase decomposition of formic acid, the low-nuclearity ensembles with unique Pt3Mo1N3 configuration deliver high-purity hydrogen at full conversion with unexpected high activity of 0.62 molHCOOH molPt−1 s−1 and remarkable stability, significantly outperforming the previously reported catalysts. The remarkable performance is rationalized by a joint operando dual-beam Fourier transformed infrared spectroscopy and density functional theory modeling study, pointing to the Pt-Mo synergy in creating a new reaction path for consecutive HCOOH dissociations.

Suggested Citation

  • Luyao Guo & Kaixuan Zhuge & Siyang Yan & Shiyi Wang & Jia Zhao & Saisai Wang & Panzhe Qiao & Jiaxu Liu & Xiaoling Mou & Hejun Zhu & Ziang Zhao & Li Yan & Ronghe Lin & Yunjie Ding, 2023. "Defect-driven nanostructuring of low-nuclearity Pt-Mo ensembles for continuous gas-phase formic acid dehydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42759-5
    DOI: 10.1038/s41467-023-42759-5
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    References listed on IDEAS

    as
    1. Dmitri A. Bulushev, 2021. "Progress in Catalytic Hydrogen Production from Formic Acid over Supported Metal Complexes," Energies, MDPI, vol. 14(5), pages 1-14, March.
    2. Davide Albani & Masoud Shahrokhi & Zupeng Chen & Sharon Mitchell & Roland Hauert & Núria López & Javier Pérez-Ramírez, 2018. "Selective ensembles in supported palladium sulfide nanoparticles for alkyne semi-hydrogenation," Nature Communications, Nature, vol. 9(1), pages 1-11, December.
    3. Tingting Hou & Qiquan Luo & Qi Li & Hualu Zu & Peixin Cui & Siwei Chen & Yue Lin & Jiajia Chen & Xusheng Zheng & Wenkun Zhu & Shuquan Liang & Jinlong Yang & Liangbing Wang, 2020. "Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
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