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Photo-induced ultrafast active ion transport through graphene oxide membranes.

ABSTRACT: Layered graphene oxide membranes (GOM) with densely packed sub-nanometer-wide lamellar channels show exceptional ionic and molecular transport properties. Mass and charge transport in existing materials follows their concentration gradient, whereas attaining anti-gradient transport, also called active transport, remains a great challenge. Here, we demonstrate a coupled photon-electron-ion transport phenomenon through the GOM. Upon asymmetric light illumination, cations are able to move thermodynamically uphill over a broad range of concentrations, at rates much faster than that via simple diffusion. We propose, as a plausible mechanism, that light irradiation reduces the local electric potential on the GOM following a carrier diffusion mechanism. When the illumination is applied to an off-center position, an electric potential difference is built that can drive the transport of ionic species. We further develop photonic ion switches, photonic ion diodes, and photonic ion transistors as the fundamental elements for active ion sieving and artificial photosynthesis on synthetic nanofluidic circuits.

SUBMITTER: Yang J

PROVIDER: S-EPMC6414642 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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Photo-induced ultrafast active ion transport through graphene oxide membranes.

Yang Jinlei J Hu Xiaoyu X Kong Xian X Jia Pan P Ji Danyan D Quan Di D Wang Lili L Wen Qi Q Lu Diannan D Wu Jianzhong J Jiang Lei L Guo Wei W

Nature communications 20190312 1

Layered graphene oxide membranes (GOM) with densely packed sub-nanometer-wide lamellar channels show exceptional ionic and molecular transport properties. Mass and charge transport in existing materials follows their concentration gradient, whereas attaining anti-gradient transport, also called active transport, remains a great challenge. Here, we demonstrate a coupled photon-electron-ion transport phenomenon through the GOM. Upon asymmetric light illumination, cations are able to move thermodyn ...[more]

PMID: 30862778

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Project description:In 2014, it was reported that protons can traverse between aqueous phases separated by nominally pristine monolayer graphene and hexagonal boron nitride (h-BN) films (membranes) under ambient conditions. This intrinsic proton conductivity of the one-atom-thick crystals, with proposed through-plane conduction, challenged the notion that graphene is impermeable to atoms, ions, and molecules. More recent evidence points to a defect-facilitated transport mechanism, analogous to transport through conventional ion-selective membranes based on graphene and h-BN. Herein, local ion-flux imaging is performed on chemical vapor deposition (CVD) graphene|Nafion membranes using an "electrochemical ion (proton) pump cell" mode of scanning electrochemical cell microscopy (SECCM). Targeting regions that are free from visible macroscopic defects (e.g., cracks, holes, etc.) and assessing hundreds to thousands of different sites across the graphene surfaces in a typical experiment, we find that most of the CVD graphene|Nafion membrane is impermeable to proton transport, with transmission typically occurring at ≈20-60 localized sites across a ≈0.003 mm2 area of the membrane (>5000 measurements total). When localized proton transport occurs, it can be a highly dynamic process, with additional transmission sites "opening" and a small number of sites "closing" under an applied electric field on the seconds time scale. Applying a simple equivalent circuit model of ion transport through a cylindrical nanopore, the local transmission sites are estimated to possess dimensions (radii) on the (sub)nanometer scale, implying that rare atomic defects are responsible for proton conductance. Overall, this work reinforces SECCM as a premier tool for the structure-property mapping of microscopically complex (electro)materials, with the local ion-flux mapping configuration introduced herein being widely applicable for functional membrane characterization and beyond, for example in diagnosing the failure mechanisms of protective surface coatings.

Dataset Information

Photo-induced ultrafast active ion transport through graphene oxide membranes.

Publications

Photo-induced ultrafast active ion transport through graphene oxide membranes.

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