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Nano Lett. 2018 Jun 13;18(6):3962-3968. doi: 10.1021/acs.nanolett.8b01429. Epub 2018 May 7.

Pore-Size-Tuned Graphene Oxide Frameworks as Ion-Selective and Protective Layers on Hydrocarbon Membranes for Vanadium Redox-Flow Batteries.

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Department of Chemical and Biomolecular Engineering, KAIST Institute for the Nanocentury , Korea Advanced Institute of Science and Technology , 291 Daehak-ro , Yuseong-gu, Daejeon , 34141 Republic of Korea.
Center for Membrane , Korea Research Institute of Chemical Technology , 141 Gajeong-ro , Yuseong-gu, Daejeon , 34114 Republic of Korea.


The laminated structure of graphene oxide (GO) membranes provides exceptional ion-separation properties due to the regular interlayer spacing ( d) between laminate layers. However, a larger effective pore size of the laminate immersed in water (∼11.1 Å) than the hydrated diameter of vanadium ions (>6.0 Å) prevents its use in vanadium redox-flow batteries (VRFB). In this work, we report an ion-selective graphene oxide framework (GOF) with a d tuned by cross-linking the GO nanosheets. Its effective pore size (∼5.9 Å) excludes vanadium ions by size but allows proton conduction. The GOF membrane is employed as a protective layer to address the poor chemical stability of sulfonated poly(arylene ether sulfone) (SPAES) membranes against VO2+ in VRFB. By effectively blocking vanadium ions, the GOF/SPAES membrane exhibits vanadium-ion permeability 4.2 times lower and a durability 5 times longer than that of the pristine SPAES membrane. Moreover, the VRFB with the GOF/SPAES membrane achieves an energy efficiency of 89% at 80 mA cm-2 and a capacity retention of 88% even after 400 cycles, far exceeding results for Nafion 115 and demonstrating its practical applicability for VRFB.


Graphene oxide framework membranes; chemical stabilities; hydrocarbon membranes; pore-size exclusions; vanadium redox-flow batteries

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