IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-42759-5.html
   My bibliography  Save this article

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
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-42759-5
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-023-42759-5?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. 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.
    2. 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.
    3. 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.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Dmitri A. Bulushev, 2021. "Advanced Catalysis in Hydrogen Production from Formic Acid and Methanol," Energies, MDPI, vol. 14(20), pages 1-5, October.
    2. Davide Clematis & Daria Bellotti & Massimo Rivarolo & Loredana Magistri & Antonio Barbucci, 2023. "Hydrogen Carriers: Scientific Limits and Challenges for the Supply Chain, and Key Factors for Techno-Economic Analysis," Energies, MDPI, vol. 16(16), pages 1-31, August.
    3. Haifeng Shen & Huanyu Jin & Haobo Li & Herui Wang & Jingjing Duan & Yan Jiao & Shi-Zhang Qiao, 2023. "Acidic CO2-to-HCOOH electrolysis with industrial-level current on phase engineered tin sulfide," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    4. Gromov, Nikolay V. & Medvedeva, Tatiana B. & Lukoyanov, Ivan A. & Ogorodnikova, Olga L. & Panchenko, Valentina N. & Parmon, Valentin N. & Timofeeva, Maria N., 2024. "Hydrolysis-oxidation of starch to formic acid in the presence of vanadium-containing molybdophosphoric heteropoly acid (H3+xPMo12-xVxO40): Effect of acidity and vanadium content on the yield of formic," Renewable Energy, Elsevier, vol. 220(C).
    5. Qiaoxi Liu & Wenjie Xu & Hao Huang & Hongwei Shou & Jingxiang Low & Yitao Dai & Wanbing Gong & Youyou Li & Delong Duan & Wenqing Zhang & Yawen Jiang & Guikai Zhang & Dengfeng Cao & Kecheng Wei & Ran L, 2024. "Spectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    6. Xinchun Yang & Dmitri A. Bulushev & Jun Yang & Quan Zhang, 2022. "New Liquid Chemical Hydrogen Storage Technology," Energies, MDPI, vol. 15(17), pages 1-18, August.
    7. Xiaoyang Pan & Xuhui Yang & Maoqing Yu & Xiaoxiao Lu & Hao Kang & Min-Quan Yang & Qingrong Qian & Xiaojing Zhao & Shijing Liang & Zhenfeng Bian, 2023. "2D MXenes polar catalysts for multi-renewable energy harvesting applications," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    8. Ekaterina Matus & Olga Sukhova & Ilyas Ismagilov & Mikhail Kerzhentsev & Olga Stonkus & Zinfer Ismagilov, 2021. "Hydrogen Production through Autothermal Reforming of Ethanol: Enhancement of Ni Catalyst Performance via Promotion," Energies, MDPI, vol. 14(16), pages 1-16, August.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42759-5. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.