Significant
developments have been proposed over the past decade in the synthesis
of aluminosilicate and aluminogermanate imogolite-like nanotubes.
But, while liquid phase synthesis is well-controlled, it is not the
case for the nanotube arrangement in the dry state. In particular,
nanotubes are found to self-assemble in bundles of various sizes,
which may impact the properties of the final product. Here, we investigate
the effect of ionic strength on bundling of aluminogermanate single-walled
imogolite nanotubes (Ge-SWINT) in aqueous suspensions and in the resulting
powders after solvent evaporation. The nanotube arrangement as a function
of salt concentration was studied by X-ray scattering experiments
and simulations. In aqueous suspension, nanotubes bundling occurs
only at high ionic strength (IS > 8 × 10–2 mol·L–1), while beyond this threshold, the
increase of electrostatic repulsions induces a complete stabilization
of individual nanotubes. After solvent evaporation, nanotube arrangement
is shown to be dictated principally by the initial concentration of
salt. Beyond an ionic strength of ∼10–3 mol·L–1 in the starting suspension, all Ge-SWINT samples
tend to form large bundles in powder, whose lattice parameters are
independent of the initial salt concentrations. These experimental
results clearly show that the positive surface charge of imogolite
can be used to control nanotubes bundling by anion condensation.