By introducing hydrophilic polymers into silicone medical devices, highly beneficial biomedical properties can be realized. An established solution to introduce hydrophilic polymers is to form an interpenetrating polymer network (IPN) by performing the hydrogel synthesis in the presence of silicone swollen in supercritical carbon dioxide. The precise distribution of the two polymers is not known, and determining this is the goal of this study. Neutron scattering and microscopy were used to determine the distribution of the hydrophilic guest polymer. Atomic force microscopy revealed that the important length scale on the surface of these materials is 10–100 nm, and spin-echo small-angle neutron scattering (SESANS) on IPNs submerged in D₂O revealed structures of the same scale within the interior and enabled quantification of their size. SESANS with hydration by D₂O proved to be the only scattering technique that could determine the structure of the bulk of these types of materials, and it should be used as an important tool for characterizing polymer medical devices.

Interactions between graphene oxide (GO) and organic molecules play a role in processes such as environmental remediation and water treatment. However, little is known about underlying molecular level processes with the presence of ions. In this study, we utilized atomic force microscopy (AFM) in chemical force mapping (CFM) mode to directly probe their adhesion interactions. AFM tips were functionalised to serve as models for nonpolar and polar organic molecules, i.e. with alkyl, -CH₃, and carboxyl, -COO(H). For experiments with -COO(H) tips, adhesion between GO and tips decreased in the order: Ba²⁺ > Ca²⁺ > Mg²⁺ > Na⁺, whereas for the -CH₃ tips, ion dependent adhesion was relatively low but followed the same: Ba²⁺ > Ca²⁺ > Mg²⁺ ≈ Na⁺. Calculations with Derjaguin-Landau-Verwey-Overbeek (DLVO) theory and the Schulze-Hardy rule could not account for the observations. We propose that ion bridging plays a definitive role in adhesion between -COO(H) tips and the GO surface. This is consistent with proposed models with density functional theory (DFT) calculations. Adhesion of -CH₃ tips is a response to the hydrophilic interactions and the ion dependent part is suggested to arise from ion bridging between slightly negative charged -CH₃ tips and the GO surface. High pH had a notable influence on the adhesion of the -COO(H) tip but a negligible effect on the -CH₃ tip. These results offer important insights into interactions between solutions and mineral surfaces with adsorbed organic molecules.

The unambiguous determination of the chemical functionality over graphene oxide (GO) is important to unleash its potential applications. However, the mapping of oxygen functionalities distribution remains to be unequivocally determined because of highly inhomogeneous non-stoichiometric structures and ultra-thin layers of GO. In this study, we report an experimental observation of the spatial distribution of oxygen functional groups on monolayer and multilayer GO using AFM-IR, atomic force microscopy coupled with infrared spectroscopy. Overcoming conventional IR diffraction limit for several micrometers, the novel AFM-IR reaches high spatial resolution ∼20 nm and could detect IR absorption on ∼1 nm thickness of monolayer GO. With nanoscale chemical mapping, the distribution of different oxygen functional groups is distinguished with AFM-IR over the GO surface. It allows us to observe that these oxygen functional groups prefer to sit on the fold areas, in discrete domains and on the edges of GO, which gave more insights into its chemical nature. The determination of the position of functional groups through precise imaging contributes to our understanding of GO structure-properties relations and paves the way for targeted tethering of polymers, biomaterials, and other nanostructures.