IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v12y2021i1d10.1038_s41467-021-25640-1.html
   My bibliography  Save this article

Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion

Author

Listed:
  • Tianyu Zhang

    (University of Cincinnati)

  • Weitao Li

    (Shanghai University)

  • Kai Huang

    (East China University of Science and Technology)

  • Huazhang Guo

    (Shanghai University)

  • Zhengyuan Li

    (University of Cincinnati)

  • Yanbo Fang

    (University of Cincinnati)

  • Ram Manohar Yadav

    (Rice University)

  • Vesselin Shanov

    (University of Cincinnati
    University of Cincinnati)

  • Pulickel M. Ajayan

    (Rice University)

  • Liang Wang

    (Shanghai University)

  • Cheng Lian

    (East China University of Science and Technology)

  • Jingjie Wu

    (University of Cincinnati)

Abstract

A catalyst system with dedicated selectivity toward a single hydrocarbon or oxygenate product is essential to enable the industrial application of electrochemical conversion of CO2 to high-value chemicals. Cu is the only known metal catalyst that can convert CO2 to high-order hydrocarbons and oxygenates. However, the Cu-based catalysts suffer from diverse selectivity. Here, we report that the functionalized graphene quantum dots can direct CO2 to CH4 conversion with simultaneous high selectivity and production rate. The electron-donating groups facilitate the yield of CH4 from CO2 electro-reduction while electron-withdrawing groups suppress CO2 electro-reduction. The yield of CH4 on electron-donating group functionalized graphene quantum dots is positively correlated to the electron-donating ability and content of electron-donating group. The graphene quantum dots functionalized by either –OH or –NH2 functional group could achieve Faradaic efficiency of 70.0% for CH4 at −200 mA cm−2 partial current density of CH4. The superior yield of CH4 on electron-donating group- over the electron-withdrawing group-functionalized graphene quantum dots possibly originates from the maintenance of higher charge density of potential active sites (neighboring C or N) and the interaction between the electron-donating group and key intermediates. This work provides insight into the design of active carbon catalysts at the molecular scale for the CO2 electro-reduction.

Suggested Citation

  • Tianyu Zhang & Weitao Li & Kai Huang & Huazhang Guo & Zhengyuan Li & Yanbo Fang & Ram Manohar Yadav & Vesselin Shanov & Pulickel M. Ajayan & Liang Wang & Cheng Lian & Jingjie Wu, 2021. "Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25640-1
    DOI: 10.1038/s41467-021-25640-1
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-021-25640-1
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-021-25640-1?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. Jongyoun Kim & Taemin Lee & Hyun Dong Jung & Minkyoung Kim & Jungsu Eo & Byeongjae Kang & Hyeonwoo Jung & Jaehyoung Park & Daewon Bae & Yujin Lee & Sojung Park & Wooyul Kim & Seoin Back & Youngu Lee &, 2024. "Vitamin C-induced CO2 capture enables high-rate ethylene production in CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Yu Yang & Cheng Zhang & Chengyi Zhang & Yaohui Shi & Jun Li & Bernt Johannessen & Yongxiang Liang & Shuzhen Zhang & Qiang Song & Haowei Zhang & Jialei Huang & Jingwen Ke & Lei Zhang & Qingqing Song & , 2024. "Ligand-tuning copper in coordination polymers for efficient electrochemical C–C coupling," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Shengdong Xiao & Caroline Akinyi & Jimmy Longun & Jude O. Iroh, 2022. "Polyimide Copolymers and Nanocomposites: A Review of the Synergistic Effects of the Constituents on the Fire-Retardancy Behavior," Energies, MDPI, vol. 15(11), pages 1-29, May.
    4. Huazhang Guo & Yuhao Lu & Zhendong Lei & Hong Bao & Mingwan Zhang & Zeming Wang & Cuntai Guan & Bijun Tang & Zheng Liu & Liang Wang, 2024. "Machine learning-guided realization of full-color high-quantum-yield carbon quantum dots," Nature Communications, Nature, vol. 15(1), pages 1-10, 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_s41467-021-25640-1. 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.