Highly Hydrated Thin Films Obtained via Templating of the Polyelectrolyte Multilayer Internal Structure with Proteins
(2020) ACS Applied Polymer Materials — Vol. 2, n° 7, p. 2602-2611 (2020)
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- Authors
vander Straeten, Aurélien 
- Abstract
- Controlling the sequencein which macromoleculesinteract allows creating self-assemblies that only exist because of theconstruction path that was followed. Because structure correlates withfunction, exploring paths of self-assembly holds the potential to confervarious functionalities to the assembly. In this paper, lysozyme (Lyz) wasused as a templating agent in the layer-by-layer (LbL) self-assembly ofpoly(allylamine hydrochloride) (PAH) with poly(styrenesulfonate)(PSS). To do so, Lyz was complexed with PSS, and the resultingcomplex was alternately adsorbed with PAH. By carrying the LbLassembly at low pH and in pure water, PAH adsorption causes thesubsequent release of Lyz. The result is that even though it was used forassembly, only a very small fraction of Lyz is present in the resultingfilm.Using quartz crystal microbalance with dissipation monitoring mountedwith a humidity module, the swelling/deswelling behavior and the composition of these polyelectrolyte multilayers (PEMs) wereinvestigated. It appears that such PEMs obtained via a complex adsorption sequence are much thicker and trapped in anonequilibrium state. Their dehydration is irreversible as it causes their collapse into denser PEMs. After dehydration, the PEMsshare a common composition with the ones constructed without the use of Lyz as a templating agent. Fitting the Flory−Hugginsequation to the data suggests that both PEM types separate into a polymer-rich phase and a water-rich phase when exposed toincreasing water vapor pressure. Nevertheless, the presence of a swelling hysteresis in the PEMs templated with Lyz suggests thatthey possess a different internal structure or that trace amounts of Lyz affect the polymer relaxation kinetics. The use of proteins astemplating elements thus allows to construct PEMs that are thick, highly hydrated, and gel-like at the nanoscale level rather than thindense PE blends, which is topical for biomedical applications.
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Citations
vander Straeten, A., & Dupont, C. (2020). Highly Hydrated Thin Films Obtained via Templating of the Polyelectrolyte Multilayer Internal Structure with Proteins. ACS Applied Polymer Materials, 2(7), 2602-2611. https://doi.org/10.1021/acsapm.0c00243 (Original work published 2020)