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    Home > Chemicals Industry > Chemical Technology > Research on the construction of sub-nanoscale Pd and Pt metal clusters to achieve efficient dehydrogenation of organic hydrogen molecules

    Research on the construction of sub-nanoscale Pd and Pt metal clusters to achieve efficient dehydrogenation of organic hydrogen molecules

    • Last Update: 2022-05-20
    • Source: Internet
    • Author: User
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    Recently, the team of Liu Hongyang, a researcher at the Shenyang National Research Center for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, together with Professor Martin of Peking University, Professor Li Jun of Tsinghua University, Professor Wang Yanggang of Southern University of Science and Technology, Professor Zhou Wu of University of Chinese Academy of Sciences, and Professor Wang Ning of Hong Kong University of Science and Technology, etc.
    Collaboration to achieve efficient hydrogen production from organically supported hydrogen molecules by precisely constructing sub-nanoscale atomically dispersed Pd and Pt metal cluster catalytic materials, Journal of the American Chemical Society and Nature-Catalysis (Nature Catalysis) published the research results separately

    .

    Hydrogen has the advantages of high energy density, economical and environmental protection, but the storage and transportation of hydrogen is the bottleneck hindering the large-scale application of hydrogen energy
    .
    Using liquid organic hydrogen storage media (LOHC), such as cyclohexane, dodecahydrocarbazole and other dehydrogenation reactions, can produce hydrogen, and combined with its reverse hydrogenation reaction, the reversible storage, release and efficient transportation of hydrogen can be realized

    .
    Since the active catalytic components of the LOHC dehydrogenation process are mainly noble metal catalytic materials, it is of great scientific significance and industrial application value to enhance its catalytic performance by maximizing the utilization of noble metals

    .

    The research team precisely constructed isolated atomically dispersed platinum single atoms (Pt1), fully exposed platinum clusters (Ptn) of different sizes, and traditional platinum on the surface of defect-rich graphene-coated nano-diamond supports (ND@G) support.
    Nanoparticles (Ptp)

    .
    In the cyclohexane dehydrogenation reaction, although Pt1 has the highest metal atom utilization efficiency, it is still inactive even at 553

    K.
    In contrast, both sub-nanoscale fully exposed Ptn clusters and Ptp nanoparticle catalytic materials can catalyze this dehydrogenation reaction, but larger Pt nanoparticles are less active, while subnanoscale fully exposed Ptn clusters can catalyze this dehydrogenation reaction.
    The catalytic materials (with an average Pt–Pt coordination number around 2–3) showed the best catalytic dehydrogenation performance

    .
    Combining the experimental results with theoretical calculations, it is found that the activity difference of Pt catalytic materials mainly comes from the limited but continuous multi-site group effect during the activation of the CH bond (Fig.
    1)

    .

    Based on the above research work, the research team found that the sub-nanoscale fully exposed Pdn cluster catalytic material also showed excellent dehydrogenation and hydrogen production performance in the dodecahydrocarbazole dehydrogenation reaction
    .
    In addition, based on the differences in CO adsorption modes of different Pd species, the study quantitatively described the dispersion state of Pd on the surface of different catalysts by infrared spectroscopy, estimated the proportion of Pd species with different structures in the catalyst, and combined with X-ray absorption spectroscopy analysis As a result, the structure-activity relationship between the average coordination number of Pd species at different scales and the intrinsically active TOF was established, and the results showed that the highly active sub-nanoscale Pdn metal clusters have metal group sites that are favorable for activating reactant molecules as well as inhibiting products.
    Characterized by strong adsorption behavior (Fig.
    2)

    .
    The above findings provide a scientific basis and theoretical guidance for the design of a new generation of sub-nanoscale high-efficiency metal catalytic materials for hydrogen production

    .

    Liu Hongyang's research team used the design theory of sub-nanoscale metal catalytic materials to guide the production of practical industrial catalysts, and developed a low-content palladium-based catalyst for the hydrogenation of dinitrotoluene.
    The industrial application of hydrogen technology (Figure 3) will help companies reduce production costs and reduce carbon emissions

    .

    The research work has been supported by the key research and development plan of the Ministry of Science and Technology, the major research plan of the National Natural Science Foundation of China, the key project of the joint enterprise fund, the China-Hong Kong joint fund for international cooperation, the Liaoning Province Xingliao Talent Plan, the Chinese Academy of Sciences Institutional Research Project, the Chinese Postdoctoral Fund, etc.
    support

    .


    Figure 1.
    Sub-nanoscale fully exposed Ptn metal cluster catalytic material for efficient dehydrogenation of cyclohexane to hydrogen production (J.
    Am.
    Chem.
    Soc.
    2022, 144, 8, 3535–3542, cover)

    Figure 2.
    Sub-nanoscale fully exposed Pdn metal cluster catalytic material with high metal utilization and appropriate metallicity exhibits excellent activity for dehydrocarbazole dehydrogenation to hydrogen production

    .
    (Nat.
    Catal.
    doi: 10.
    1038/s41929-022-00769-4)

    Figure 3.
    Industrial application of sub-nanoscale palladium-based metal catalysts in a 120,000-ton catalytic hydrogenation process

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