Highly oriented,
layered, and mechanically resilient films of polydopamine
(PDA) have been synthesized from the air/water interface. The films
show a unique layered structure, as shown by scanning and transmission
electron studies (SEM/TEM) and X-ray diffraction analysis (XRD), which
resemble that of 2D layered materials. The films exhibit a composition
typical of PDA-based materials, as evidenced by X-ray photoelectron
spectroscopy (XPS); moreover, the samples present the distinctive
resonance modes of PDA-based nanomaterials in Raman and infrared spectroscopy
(FTIR) experiments. The presence of highly ordinated 3–4 protomolecule
stacking, taking place at the air/water interface, with a unique eumelanin-like
supramolecular arrangement is presented. Moreover, the films show
superior mechanical resilience with
E
= 13 ±
4 GPa and
H
= 0.21 ± 0.03 GPa, as revealed by
nanoindentation experiments, making them highly resilient and easily
transferable. Finally, the ordering induced by the interface opens
many possibilities for further studies, including those regarding
the supramolecular structure on PDA due to their similarity to 2D
layered materials.