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Article Dans Une Revue Nanoscale Advances Année : 2020

Solid wetting-layers in inorganic nano-reactors: the water in imogolite nanotube case

Résumé

Solid wetting-layers in inorganic nano-reactors: the water in imogolite nanotube case In 2016, 'isolated' water molecules trapped inside beryl nanochannels provided the fi rst fi rm experimental evidence of the dipole ordering of water molecules and a new 'quantum tunneling' state was evidenced. We have discovered a new phase of 'isolated' water molecules at the inner surface of inorganic nanotubes and we have investigated their associated dynamical properties. Our fi ndings are signifi cant to the emerging fi eld of 'isolated' nanoconfi ned water and to the areas of water science, nanoreactors and nanofl uidics. Inelastic neutron scattering and DFT-MD techniques are used in association with new methods of analysis which may be of interest to other fi elds of physics and nanosciences. By combined use of wide-angle X-ray scattering, thermo-gravimetric analysis, inelastic neutron scattering, density functional theory and density functional theory molecular dynamics simulations, we investigate the structure, dynamics and stability of the water wetting-layer in single-walled aluminogermanate imogolite nanotubes (SW Ge-INTs): an archetypal system for synthetically controllable and monodisperse nano-reactors. We demonstrate that the water wetting-layer is strongly bound and solid-like up to 300 K under atmospheric pressure, with dynamics markedly different from that of bulk water. Atomic-scale characterisation of the wetting-layer reveals organisation of the H 2 O molecules in a curved triangular sublattice stabilised by the formation of three H-bonds to the nanotube's inner surface, with covalent interactions sufficiently strong to promote energetically favourable decoupling of the H 2 O molecules in the adlayer. The evidenced changes in the local composition, structure, electrostatics and dynamics of the Ge-INT's inner surface upon the formation of the solid wetting-layer demonstrate solvent-mediated functionalisation of the nanotube's cavity at room temperature and pressure, suggesting new strategies for the design of nano-rectors towards potential control of chemical reactivity in nano-confined volumes.
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Dates et versions

hal-02613870 , version 1 (28-05-2020)

Identifiants

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Geoffrey Monet, Erwan Paineau, Ziwei Chai, Mohamed Amara, Andrea Orecchini, et al.. Solid wetting-layers in inorganic nano-reactors: the water in imogolite nanotube case. Nanoscale Advances, 2020, 2 (5), pp.1869-1877. ⟨10.1039/d0na00128g⟩. ⟨hal-02613870⟩
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