Aqueous proton transfer across single-layer graphene

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, Sheng Dai, Adri C. T. van Duin, Matthew Neurock and Franz M. Geiger ()
Additional contact information
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
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
Franz M. Geiger: Northwestern University

Nature Communications, 2015, vol. 6, issue 1, 1-7

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms7539

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