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Internal Structure of Matrix-Type Multilayer Capsules Templated on Porous Vaterite CaCO3 Crystals as Probed by Staining with a Fluorescence Dye

Robert Schuman University Institute of Technology (IUT Robert Schuman), University of Strasbourg, 72 Route Du Rhin, 67411 Illkirch CEDEX, France
School of Science and Technology, Nottingham Trent University, Clifton Lane, Nottingham NG11 8NS, UK
Department of Chemistry, Lomonosov Moscow State University, Leninskiye Gory 1-3, 119991 Moscow, Russia
Department Cellular Biotechnology & Biochips, Branch Bioanalytics and Bioprocesses (Fraunhofer IZI-BB), Fraunhofer Institute for Cell Therapy and Immunology, Am Mühlenberg 13, 14476 Potsdam-Golm, Germany
Author to whom correspondence should be addressed.
Micromachines 2018, 9(11), 547;
Received: 28 September 2018 / Revised: 19 October 2018 / Accepted: 23 October 2018 / Published: 25 October 2018
(This article belongs to the Special Issue Self-Assembly of Polymers)
PDF [3653 KB, uploaded 25 October 2018]


Multilayer capsules templated on decomposable vaterite CaCO3 crystals are widely used as vehicles for drug delivery. The capsule represents typically not a hollow but matrix-like structure due to polymer diffusion into the porous crystals during multilayer deposition. The capsule formation mechanism is not well-studied but its understanding is crucial to tune capsule structure for a proper drug release performance. This study proposes new approach to noninvasively probe and adjust internal capsule structure. Polymer capsules made of poly(styrene-sulfonate) (PSS) and poly(diallyldimethylammonium chloride) (PDAD) have been stained with fluorescence dye rhodamine 6G. Physical-chemical aspects of intermolecular interactions required to validate the approach and adjust capsule structure are addressed. The capsules consist of a defined shell (typically 0.5–2 µm) and an internal matrix of PSS-PDAD complex (typically 10–40% of a total capsule volume). An increase of ionic strength and polymer deposition time leads to the thickening of the capsule shell and formation of a denser internal matrix, respectively. This is explained by effects of a polymer conformation and limitations in polymer diffusion through the crystal pores. We believe that the design of the capsules with desired internal structure will allow achieving effective encapsulation and controlled/programmed release of bioactives for advanced drug delivery applications. View Full-Text
Keywords: layer-by-layer; self-assembly; mesoporous; calcium carbonate; fluorescence layer-by-layer; self-assembly; mesoporous; calcium carbonate; fluorescence

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Jeannot, L.; Bell, M.; Ashwell, R.; Volodkin, D.; Vikulina, A.S. Internal Structure of Matrix-Type Multilayer Capsules Templated on Porous Vaterite CaCO3 Crystals as Probed by Staining with a Fluorescence Dye. Micromachines 2018, 9, 547.

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