Nanocelluloses can be used to stabilize oil–water
surfaces,
forming so-called Pickering emulsions. In this work, we compare the
organization of native and mercerized cellulose nanocrystals (CNC-I
and CNC-II) adsorbed on the surface of hexadecane droplets dispersed
in water at different CNC concentrations. Both types of CNCs have
an elongated particle morphology and form a layer strongly adsorbed
at the interface. However, while the layer thickness formed with CNC-I
is independent of the concentration at 7 nm, CNC-II forms a layer
ranging from 9 to 14 nm thick with increasing concentration, as determined
using small-angle neutron scattering with contrast-matched experiments.
Molecular dynamics (MD) simulations showed a preferred interacting
crystallographic plane for both crystalline allomorphs that exposes
the CH groups (100 and 010) and is therefore considered hydrophobic.
Furthermore, this study suggests that whatever the allomorph, the
migration of CNCs to the oil–water interface is spontaneous
and irreversible and is driven by both enthalpic and entropic processes.