IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v7y2016i1d10.1038_ncomms12165.html
   My bibliography  Save this article

Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites

Author

Listed:
  • Vincent Wing-hei Lau

    (Max Planck Institute for Solid State Research
    University of Munich)

  • Igor Moudrakovski

    (Max Planck Institute for Solid State Research)

  • Tiago Botari

    (Duke University)

  • Simon Weinberger

    (Max Planck Institute for Solid State Research
    University of Munich)

  • Maria B. Mesch

    (Inorganic Chemistry III, University of Bayreuth)

  • Viola Duppel

    (Max Planck Institute for Solid State Research)

  • Jürgen Senker

    (Inorganic Chemistry III, University of Bayreuth)

  • Volker Blum

    (Duke University)

  • Bettina V. Lotsch

    (Max Planck Institute for Solid State Research
    University of Munich
    Nanosystems Initiative and Center for Nanoscience (CeNS))

Abstract

The heptazine-based polymer melon (also known as graphitic carbon nitride, g-C3N4) is a promising photocatalyst for hydrogen evolution. Nonetheless, attempts to improve its inherently low activity are rarely based on rational approaches because of a lack of fundamental understanding of its mechanistic operation. Here we employ molecular heptazine-based model catalysts to identify the cyanamide moiety as a photocatalytically relevant ‘defect’. We exploit this knowledge for the rational design of a carbon nitride polymer populated with cyanamide groups, yielding a material with 12 and 16 times the hydrogen evolution rate and apparent quantum efficiency (400 nm), respectively, compared with the unmodified melon. Computational modelling and material characterization suggest that this moiety improves coordination (and, in turn, charge transfer kinetics) to the platinum co-catalyst and enhances the separation of the photogenerated charge carriers. The demonstrated knowledge transfer for rational catalyst design presented here provides the conceptual framework for engineering high-performance heptazine-based photocatalysts.

Suggested Citation

  • Vincent Wing-hei Lau & Igor Moudrakovski & Tiago Botari & Simon Weinberger & Maria B. Mesch & Viola Duppel & Jürgen Senker & Volker Blum & Bettina V. Lotsch, 2016. "Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites," Nature Communications, Nature, vol. 7(1), pages 1-10, November.
  • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms12165
    DOI: 10.1038/ncomms12165
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/ncomms12165
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/ncomms12165?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
    ---><---

    Citations

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


    Cited by:

    1. Qiyou Wang & Kang Liu & Kangman Hu & Chao Cai & Huangjingwei Li & Hongmei Li & Matias Herran & Ying-Rui Lu & Ting-Shan Chan & Chao Ma & Junwei Fu & Shiguo Zhang & Ying Liang & Emiliano Cortés & Min Li, 2022. "Attenuating metal-substrate conjugation in atomically dispersed nickel catalysts for electroreduction of CO2 to CO," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Liu, Enli & Lin, Xue & Hong, Yuanzhi & Yang, Lan & Luo, Bifu & Shi, Weilong & Shi, Junyou, 2021. "Rational copolymerization strategy engineered C self-doped g-C3N4 for efficient and robust solar photocatalytic H2 evolution," Renewable Energy, Elsevier, vol. 178(C), pages 757-765.
    3. Aiwen Wang & Meng Du & Jiaxin Ni & Dongqing Liu & Yunhao Pan & Xiongying Liang & Dongmei Liu & Jun Ma & Jing Wang & Wei Wang, 2023. "Enhanced and synergistic catalytic activation by photoexcitation driven S−scheme heterojunction hydrogel interface electric field," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Chih-Li Chang & Wei-Cheng Lin & Li-Yu Ting & Chin-Hsuan Shih & Shih-Yuan Chen & Tse-Fu Huang & Hiroyuki Tateno & Jayachandran Jayakumar & Wen-Yang Jao & Chen-Wei Tai & Che-Yi Chu & Chin-Wen Chen & Chi, 2022. "Main-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, 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:7:y:2016:i:1:d:10.1038_ncomms12165. 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.

    We have no bibliographic references for this item. You can help adding them by using 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.