IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v12y2021i1d10.1038_s41467-021-27238-z.html
   My bibliography  Save this article

Molecular-level insights into the electronic effects in platinum-catalyzed carbon monoxide oxidation

Author

Listed:
  • Wenyao Chen

    (East China University of Science and Technology)

  • Junbo Cao

    (East China University of Science and Technology)

  • Jia Yang

    (Norwegian University of Science and Technology)

  • Yueqiang Cao

    (East China University of Science and Technology)

  • Hao Zhang

    (Soochow University
    Chinese Academy of Sciences)

  • Zheng Jiang

    (Chinese Academy of Sciences
    Chinese Academy of Sciences)

  • Jing Zhang

    (East China University of Science and Technology)

  • Gang Qian

    (East China University of Science and Technology)

  • Xinggui Zhou

    (East China University of Science and Technology)

  • De Chen

    (Norwegian University of Science and Technology)

  • Weikang Yuan

    (East China University of Science and Technology)

  • Xuezhi Duan

    (East China University of Science and Technology)

Abstract

A molecular-level understanding of how the electronic structure of metal center tunes the catalytic behaviors remains a grand challenge in heterogeneous catalysis. Herein, we report an unconventional kinetics strategy for bridging the microscopic metal electronic structure and the macroscopic steady-state rate for CO oxidation over Pt catalysts. X-ray absorption and photoelectron spectroscopy as well as electron paramagnetic resonance investigations unambiguously reveal the tunable Pt electronic structures with well-designed carbon support surface chemistry. Diminishing the electron density of Pt consolidates the CO-assisted O2 dissociation pathway via the O*-O-C*-O intermediate directly observed by isotopic labeling studies and rationalized by density-functional theory calculations. A combined steady-state isotopic transient kinetic and in situ electronic analyses identifies Pt charge as the kinetics indicators by being closely related to the frequency factor, site coverage, and activation energy. Further incorporation of catalyst structural parameters yields a novel model for quantifying the electronic effects and predicting the catalytic performance. These could serve as a benchmark of catalyst design by a comprehensive kinetics study at the molecular level.

Suggested Citation

  • Wenyao Chen & Junbo Cao & Jia Yang & Yueqiang Cao & Hao Zhang & Zheng Jiang & Jing Zhang & Gang Qian & Xinggui Zhou & De Chen & Weikang Yuan & Xuezhi Duan, 2021. "Molecular-level insights into the electronic effects in platinum-catalyzed carbon monoxide oxidation," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27238-z
    DOI: 10.1038/s41467-021-27238-z
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-021-27238-z
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-021-27238-z?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. Wenshuai Zhu & Zili Wu & Guo Shiou Foo & Xiang Gao & Mingxia Zhou & Bin Liu & Gabriel M. Veith & Peiwen Wu & Katie L. Browning & Ho Nyung Lee & Huaming Li & Sheng Dai & Huiyuan Zhu, 2017. "Taming interfacial electronic properties of platinum nanoparticles on vacancy-abundant boron nitride nanosheets for enhanced catalysis," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
    2. Colleen Jackson & Graham T. Smith & David W. Inwood & Andrew S. Leach & Penny S. Whalley & Mauro Callisti & Tomas Polcar & Andrea E. Russell & Pieter Levecque & Denis Kramer, 2017. "Electronic metal-support interaction enhanced oxygen reduction activity and stability of boron carbide supported platinum," Nature Communications, Nature, vol. 8(1), pages 1-11, August.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Tengfei Zhang & Peng Zheng & Jiajian Gao & Xiaolong Liu & Yongjun Ji & Junbo Tian & Yang Zou & Zhiyi Sun & Qiao Hu & Guokang Chen & Wenxing Chen & Xi Liu & Ziyi Zhong & Guangwen Xu & Tingyu Zhu & Fabi, 2024. "Simultaneously activating molecular oxygen and surface lattice oxygen on Pt/TiO2 for low-temperature CO oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

    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. Wu, Zexing & Chen, Zhi & Xu, Kunhan & Li, Bin & Li, Zhenjiang & Xu, Guangrui & Xiao, Weiping & Ma, Tianyi & Fu, Yunlei & Wang, Lei, 2023. "Cationic defects coupled with trace Pt under the assistance of corrosive engineering for efficient hydrogen electrocatalysis with large current density," Renewable Energy, Elsevier, vol. 210(C), pages 196-202.
    2. Chenlu Wang & Liping Zhou & Chengzhe Liu & Jiaming Qiao & Xinrui Han & Luyang Wang & Yaxi Liu & Bi Xu & Qinfang Qiu & Zizhuo Zhang & Jiale Wang & Xiaoya Zhou & Mengqi Zeng & Lilei Yu & Lei Fu, 2024. "Pt nanoshells with a high NIR-II photothermal conversion efficiency mediates multimodal neuromodulation against ventricular arrhythmias," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    3. Jiayi Chen & Mohammed Aliasgar & Fernando Buendia Zamudio & Tianyu Zhang & Yilin Zhao & Xu Lian & Lan Wen & Haozhou Yang & Wenping Sun & Sergey M. Kozlov & Wei Chen & Lei Wang, 2023. "Diversity of platinum-sites at platinum/fullerene interface accelerates alkaline hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

    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:12:y:2021:i:1:d:10.1038_s41467-021-27238-z. 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.