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Article Dans Une Revue Nature Communications Année : 2024

Staggered structural dynamic-mediated selective adsorption of H2O/D2O on flexible graphene oxide nanosheets

Ryusuke Futamura
Takahiro Ueda
Ayumi Furuse
Hideki Tanaka
Katsumi Kaneko

Résumé

Graphene oxide (GO) is the one of the most promising family of materials as atomically thin membranes for water-related molecular separation technologies due to its amphipathic nature and layered structure. Here, we show important aspects of GO on water adsorption from molecular dynamics (MD) simulations, in-situ X-ray diffraction (XRD) measurements, and ex-situ nuclear magnetic resonance (NMR) measurements. Although the MD simulations for GO and the reduced GO models revealed that the flexibility of the interlayer spacing could be attributed to the oxygen-functional groups of GO, the ultra-large GO model cannot well explain the observed swelling of GO from XRD experiments. Our MD simulations propose a realistic GO interlayer structure constructed by staggered stacking of flexible GO sheets, which can explain very well the swelling nature upon water adsorption. The transmission electron microscopic (TEM) observation also supports the non-regular staggered stacking structure of GO. Furthermore, we demonstrate the existence of the two distinct types of adsorbed water molecules in the staggered stacking: water bonded with hydrophilic functional groups and “free” mobile water. Finally, we show that the staggered stacking of GO plays a crucial role in H/D isotopic recognition in water adsorption, as well as the high mobility of water molecules.
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Origine : Publication financée par une institution
Licence : CC BY - Paternité

Dates et versions

hal-04561878 , version 1 (28-04-2024)

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Ryusuke Futamura, Taku Iiyama, Takahiro Ueda, Patrick A Bonnaud, François-Xavier Coudert, et al.. Staggered structural dynamic-mediated selective adsorption of H2O/D2O on flexible graphene oxide nanosheets. Nature Communications, 2024, 15 (1), pp.3585. ⟨10.1038/s41467-024-47838-9⟩. ⟨hal-04561878⟩
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