IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v6y2015i1d10.1038_ncomms7539.html
   My bibliography  Save this article

Aqueous proton transfer across single-layer graphene

Author

Listed:
  • Jennifer L. Achtyl

    (Northwestern University)

  • Raymond R. Unocic

    (Center for Nanophase Materials Sciences, Oak Ridge National Laboratory)

  • Lijun Xu

    (University of Virginia)

  • Yu Cai

    (University of Virginia)

  • Muralikrishna Raju

    (Pennsylvania State University)

  • Weiwei Zhang

    (Pennsylvania State University)

  • Robert L. Sacci

    (Oak Ridge National Laboratory)

  • Ivan V. Vlassiouk

    (Oak Ridge National Laboratory)

  • Pasquale F. Fulvio

    (University of Puerto Rico, Río Piedras Campus
    Oak Ridge National Laboratory)

  • Panchapakesan Ganesh

    (Center for Nanophase Materials Sciences, Oak Ridge National Laboratory)

  • David J. Wesolowski

    (Oak Ridge National Laboratory)

  • Sheng Dai

    (Oak Ridge National Laboratory)

  • Adri C. T. van Duin

    (Pennsylvania State University)

  • Matthew Neurock

    (University of Virginia
    University of Minnesota)

  • Franz M. Geiger

    (Northwestern University)

Abstract

Proton transfer across single-layer graphene proceeds with large computed energy barriers and is therefore thought to be unfavourable at room temperature unless nanoscale holes or dopants are introduced, or a potential bias is applied. Here we subject single-layer graphene supported on fused silica to cycles of high and low pH, and show that protons transfer reversibly from the aqueous phase through the graphene to the other side where they undergo acid–base chemistry with the silica hydroxyl groups. After ruling out diffusion through macroscopic pinholes, the protons are found to transfer through rare, naturally occurring atomic defects. Computer simulations reveal low energy barriers of 0.61–0.75 eV for aqueous proton transfer across hydroxyl-terminated atomic defects that participate in a Grotthuss-type relay, while pyrylium-like ether terminations shut down proton exchange. Unfavourable energy barriers to helium and hydrogen transfer indicate the process is selective for aqueous protons.

Suggested Citation

  • Jennifer L. Achtyl & Raymond R. Unocic & Lijun Xu & Yu Cai & Muralikrishna Raju & Weiwei Zhang & Robert L. Sacci & Ivan V. Vlassiouk & Pasquale F. Fulvio & Panchapakesan Ganesh & David J. Wesolowski &, 2015. "Aqueous proton transfer across single-layer graphene," Nature Communications, Nature, vol. 6(1), pages 1-7, May.
  • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms7539
    DOI: 10.1038/ncomms7539
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/ncomms7539
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/ncomms7539?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. Llewellyn, Sue & Begkos, Christos & Ellwood, Sheila & Mellingwood, Chris, 2022. "Public value and pricing in English hospitals: Value creation or value extraction?," CRITICAL PERSPECTIVES ON ACCOUNTING, Elsevier, vol. 85(C).
    2. Z. F. Wu & P. Z. Sun & O. J. Wahab & Y. T. Tan & D. Barry & D. Periyanagounder & P. B. Pillai & Q. Dai & W. Q. Xiong & L. F. Vega & K. Lulla & S. J. Yuan & R. R. Nair & E. Daviddi & P. R. Unwin & A. K, 2023. "Proton and molecular permeation through the basal plane of monolayer graphene oxide," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    3. Marco Reidelbach & Marcus Weber & Petra Imhof, 2018. "Prediction of perturbed proton transfer networks," PLOS ONE, Public Library of Science, vol. 13(12), pages 1-23, 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:6:y:2015:i:1:d:10.1038_ncomms7539. 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.