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Selective Proton Transport for Hydrogen Production Using Graphene Oxide Membranes

Cite this: J. Phys. Chem. Lett. 2020, 11, 21, 9415–9420
Publication Date (Web):October 26, 2020
https://doi.org/10.1021/acs.jpclett.0c02481
Copyright © 2020 American Chemical Society
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Abstract

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Graphene oxide has shown exceptional properties in terms of water permeability and filtration characteristics. Here the suitability of graphene oxide membranes for the spatial separation of hydronium and hydroxide ions after photocatalytic water splitting is demonstrated. Instead of relying on classical size exclusion by adjusting the membrane laminates’ interlayer spacings, nonmodified graphene oxide is used to exploit the presence of its natural functional groups and surface charges for filtration. Despite a significantly larger interlayer spacing inside the membrane compared with the size of the hydrated radii of the ions, highly asymmetric transport behavior and a 6 times higher mobility for hydronium than for hydroxide are observed. DFT simulations reveal that hydroxide ions are more prone to interact and stick to the functional groups of graphene oxide, while diffusion of hydronium ions through the membrane is less impeded and aligns well with the concept of the Grotthuss mechanism.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.0c02481.

  • SEM images and XRD measurements showing thickness and interlayer spacing under measurement conditions of GO membrane; issue of water purity and its influence on the increase in current due to water splitting; reference measurements without the GO membrane as a separating agent; influences of CO2 adsorption, hydronium and hydroxide ion mobilities, cell dimensions, and ionic residues; Raman measurements investigating the chemical stability of TiO2 before and after water splitting experiments; experimental and computational methods (PDF)

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Cited By

This article is cited by 7 publications.

  1. Partha Bairi, Ayumi Furuse, Kazunori Fujisawa, Takuya Hayashi, Katsumi Kaneko. Effect of Pretreatment Conditions on the Precise Nanoporosity of Graphene Oxide. Langmuir 2022, 38 (50) , 15880-15886. https://doi.org/10.1021/acs.langmuir.2c02938
  2. Yu Jiang, Jiaojiao Ma, Chongyang Yang, Sheng Hu. One-Atom-Thick Crystals as Emerging Proton Sieves. The Journal of Physical Chemistry Letters 2021, 12 (51) , 12376-12383. https://doi.org/10.1021/acs.jpclett.1c03793
  3. Montree Hankoy, Chaiwat Phrompet, Chesta Ruttanapun, Prangtip Rittichote Kaewpengkrow, Supawan Vichaphund, Duangduen Atong, Mettaya Kitiwan, Phacharaphon Tunthawiroon. Enhancing the hydrogen permeation of alumina composite porous membranes via graphene oxide addition. International Journal of Hydrogen Energy 2023, 48 (4) , 1380-1390. https://doi.org/10.1016/j.ijhydene.2022.10.027
  4. Rui Liu, Yingxue Xu, Wanfen Pu, Peng Shi, Daijun Du, James J. Sheng, Huaisong Yong. Oligomeric ethylene-glycol brush functionalized graphene oxide with exceptional interfacial properties for versatile applications. Applied Surface Science 2022, 606 , 154856. https://doi.org/10.1016/j.apsusc.2022.154856
  5. Rolf David, Revati Kumar. Reactive events at the graphene oxide–water interface. Chemical Communications 2021, 57 (88) , 11697-11700. https://doi.org/10.1039/D1CC04589J
  6. Yu Gu, Jianfeng Zhao, Haifeng Zhou, Haiqing Jiang, Jingye Li, Bowu Zhang, Hongjuan Ma. Crosslinking imidazolium-intercalated GO membrane for acid recovery from low concentration solution. Carbon 2021, 183 , 830-839. https://doi.org/10.1016/j.carbon.2021.07.050
  7. Fangfang Dai, Feng Zhou, Junlang Chen, Shanshan Liang, Liang Chen, Haiping Fang. Ultrahigh water permeation with a high multivalent metal ion rejection rate through graphene oxide membranes. Journal of Materials Chemistry A 2021, 9 (17) , 10672-10677. https://doi.org/10.1039/D1TA00647A

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