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Reversible dehydrogenation and rehydrogenation of cyclohexane and methylcyclohexane by single-site platinum catalyst

Author

Listed:
  • Luning Chen

    (The Molecular Foundry, Lawrence Berkeley National Laboratory
    Xiamen University
    Chemical Sciences Division, Lawrence Berkeley National Laboratory)

  • Pragya Verma

    (The Molecular Foundry, Lawrence Berkeley National Laboratory)

  • Kaipeng Hou

    (University of California-Berkeley)

  • Zhiyuan Qi

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory)

  • Shuchen Zhang

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory)

  • Yi-Sheng Liu

    (Advanced Light Source, Lawrence Berkeley National Laboratory)

  • Jinghua Guo

    (Advanced Light Source, Lawrence Berkeley National Laboratory)

  • Vitalie Stavila

    (Sandia National Laboratories)

  • Mark D. Allendorf

    (Sandia National Laboratories)

  • Lansun Zheng

    (Xiamen University)

  • Miquel Salmeron

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory
    University of California-Berkeley)

  • David Prendergast

    (The Molecular Foundry, Lawrence Berkeley National Laboratory)

  • Gabor A. Somorjai

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory
    University of California-Berkeley)

  • Ji Su

    (The Molecular Foundry, Lawrence Berkeley National Laboratory
    Chemical Sciences Division, Lawrence Berkeley National Laboratory)

Abstract

Developing highly efficient and reversible hydrogenation-dehydrogenation catalysts shows great promise for hydrogen storage technologies with highly desirable economic and ecological benefits. Herein, we show that reaction sites consisting of single Pt atoms and neighboring oxygen vacancies (VO) can be prepared on CeO2 (Pt1/CeO2) with unique catalytic properties for the reversible dehydrogenation and rehydrogenation of large molecules such as cyclohexane and methylcyclohexane. Specifically, we find that the dehydrogenation rate of cyclohexane and methylcyclohexane on such sites can reach values above 32,000 molH2 molPt−1 h−1, which is 309 times higher than that of conventional supported Pt nanoparticles. Combining of DRIFTS, AP-XPS, EXAFS, and DFT calculations, we show that the Pt1/CeO2 catalyst exhibits a super-synergistic effect between the catalytic Pt atom and its support, involving redox coupling between Pt and Ce ions, enabling adsorption, activation and reaction of large molecules with sufficient versatility to drive abstraction/addition of hydrogen without requiring multiple reaction sites.

Suggested Citation

  • Luning Chen & Pragya Verma & Kaipeng Hou & Zhiyuan Qi & Shuchen Zhang & Yi-Sheng Liu & Jinghua Guo & Vitalie Stavila & Mark D. Allendorf & Lansun Zheng & Miquel Salmeron & David Prendergast & Gabor A., 2022. "Reversible dehydrogenation and rehydrogenation of cyclohexane and methylcyclohexane by single-site platinum catalyst," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28607-y
    DOI: 10.1038/s41467-022-28607-y
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    References listed on IDEAS

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    2. Martin Nielsen & Elisabetta Alberico & Wolfgang Baumann & Hans-Joachim Drexler & Henrik Junge & Serafino Gladiali & Matthias Beller, 2013. "Low-temperature aqueous-phase methanol dehydrogenation to hydrogen and carbon dioxide," Nature, Nature, vol. 495(7439), pages 85-89, March.
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    1. Zhaohua Wang & Chunyang Dong & Xuan Tang & Xuetao Qin & Xingwu Liu & Mi Peng & Yao Xu & Chuqiao Song & Jie Zhang & Xuan Liang & Sheng Dai & Ding Ma, 2022. "CO-tolerant RuNi/TiO2 catalyst for the storage and purification of crude hydrogen," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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