Tuning protein delivery from different architectures of layer-by-layer assemblies on polymer films

Delechiave, Giovanne; Naves, Alliny F.; Kolanthai, Elayaraja; Silva, Rubens Alexandre da; Vlasman, Raphael C.; Petri, Denise Freitas Siqueira; Torresi, Roberto Manuel; Catalani, Luiz H.

doi:10.1039/d0ma00432d

Cited by 12 publications

(9 citation statements)

References 40 publications

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“…155,156 Adsorption of proteins onto LbL-assembled films has been studied widely, and a kinetic model of protein adsorption has been described. 157,158 PLL/ DNA bilayers have been used to enhance protein adsorption and biomimetic mineralisation on the surface of titanium implants for osteoblast cell culture experiments. PLL is a positively charged polyelectrolyte that is biocompatible and can be easily conjugated with bioactive molecules.…”

Section: Cell Interactions and Protein Adhesionmentioning

confidence: 99%

Advancing bone tissue engineering one layer at a time: a layer-by-layer assembly approach to 3D bone scaffold materials

et al. 2022

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Section: Cell Interactions and Protein Adhesionmentioning

confidence: 99%

Advancing bone tissue engineering one layer at a time: a layer-by-layer assembly approach to 3D bone scaffold materials

et al. 2022

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“…Exponentially growing (chitosan/Hep) 10 films with thicknesses of 34 and 98 nm were also obtained when the surfaces were dried under a stream of N 2 after each rinsing step. 23 , 24 As has been reported for several types of LbL films, the drying process leads to the reorganization of the polyelectrolyte molecules, including reorientation of unneutralized sites with unsaturated charges in the upper surface layer in the air. Such reorganization of macromolecules facilitates film growth, leading to thicker films.…”

Section: Resultsmentioning

confidence: 86%

“…Chitosan/Hep LbL films, which have anticoagulant and antithrombotic properties, − have primarily been investigated as coatings for cardiovascular implants and grafts and can promote the proliferation of endothelial cells. − Although these polyelectrolyte assemblies have also been tested for the delivery of antimalarial drugs, FGF-2, or the model proteins albumin and lysozyme, , their preparation is limited to deposition at pH levels lower than physiological conditions because of poor chitosan solubility at pH 7.4. Alternatively, the modification of chitosan by quaternary amine groups results in water-soluble derivatives, which allows further processing under physiological pH, i.e., nondenaturing conditions for proteins.…”

Section: Introductionmentioning

confidence: 99%

Quaternized Chitosan/Heparin Polyelectrolyte Multilayer Films for Protein Delivery

et al. 2022

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Layer-by-layer (LbL) polyelectrolyte coatings are intensively studied as reservoirs of bioactive proteins for modulating interactions between biomaterial surfaces and cells. Mild conditions for the incorporation of growth factors into delivery systems are required to maintain protein bioactivity. Here, we present LbL films composed of water-soluble N- [(2-hydroxy-3trimethylammonium)propyl] chitosan chloride (HTCC), heparin (Hep), and tannic acid (TA) fabricated under physiological conditions with the ability to release heparin-binding proteins. Surface plasmon resonance analysis showed that the films formed on an anchoring HTCC/TA bilayer, with TA serving as a physical crosslinker, were more stable during their assembly, leading to increased film thickness and increased protein release. X-ray reflectivity measurements confirmed intermixing of the deposited layers. Protein release also increased when the proteins were present as an integral part of the Hep layers rather than as individual protein layers. The 4-week release pattern depended on the protein type; VEGF, CXCL12, and TGF-β1 exhibited a typical high initial release, whereas FGF-2 was sustainably released over 4 weeks. Notably, the films were nontoxic, and the released proteins retained their bioactivity, as demonstrated by the intensive chemotaxis of T-lymphocytes in response to the released CXCL12. Therefore, the proposed LbL films are promising biomaterial coating candidates for stimulating cellular responses.

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“…Since Decher et al’s first report, the LbL method has been extended to a wide range of deposited materials such as clay minerals, , viruses, dendrimers, , gold colloids, silica particles, and proteins. − Interestingly, this versatile method enables the assembly of multicomponent protein films, which open a way to construct multifunctional systems . This is topical for various fields of research such as biomaterials, drug release, tissue engineering, and regenerative medicine.…”

Section: Introductionmentioning

confidence: 99%

Layer-by-Layer Nanoarchitectonics Using Protein–Polyelectrolyte Complexes toward a Generalizable Tool for Protein Surface Immobilization

et al. 2022

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Layer-by-layer (LbL) self-assembly is an attractive method for the immobilization of macromolecules at interfaces. Integrating proteins in LbL thin films is however challenging due to their polyampholyte nature. Recently, we developed a method to integrate lysozyme into multilayers using protein−polyelectrolytes complexes (PPCs). In this work, we extended this method to a wide range of protein−polyelectrolyte combinations. We demonstrated the robustness and versatility of PPCs as building blocks. LL-37, insulin, lysozyme, and glucose oxidase were complexed with alginate, poly(styrenesulfonate), heparin, and poly(allylamine hydrochloride). The resulting PPCs were then LbL self-assembled with chitosan, PAH, and heparin. We demonstrated that multilayers built with PPCs are thicker compared to the LbL selfassembly of bare protein molecules. This is attributed to the higher mass of protein in the multilayers and/or the more hydrated state of the assemblies. PPCs enabled the self-assembly of proteins that could otherwise not be LbL assembled with a PE or with another protein. Furthermore, the results also show that LbL with PPCs enabled the construction of multilayers combining different proteins, highlighting the formation of multifunctional films. Importantly, we show that the adsorption behavior and thus the multilayer growth strongly depend on the nature of the protein and polyelectrolyte used. In this work, we elaborated a rationale to help and guide the use of PPCs for protein LbL assembly. It will therefore be beneficial to the many scientific communities willing to modify interfaces with hard-to-immobilize proteins and peptides.

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Tuning protein delivery from different architectures of layer-by-layer assemblies on polymer films

Abstract: In the past two decades, the fabrication of nanolayer coatings on polymeric materials triggered considerable interest in the tissue-engineering field. Layer-by-Layer (LbL) assembly has attracted substantial attention for being a...

Cited by 12 publications

References 40 publications

Advancing bone tissue engineering one layer at a time: a layer-by-layer assembly approach to 3D bone scaffold materials

Advancing bone tissue engineering one layer at a time: a layer-by-layer assembly approach to 3D bone scaffold materials

Quaternized Chitosan/Heparin Polyelectrolyte Multilayer Films for Protein Delivery

Layer-by-Layer Nanoarchitectonics Using Protein–Polyelectrolyte Complexes toward a Generalizable Tool for Protein Surface Immobilization

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