Fabrication of Antibacterial, Osteo-Inductor 3D Printed Aerogel-Based Scaffolds by Incorporation of Drug Laden Hollow Mesoporous Silica Microparticles into the Self-Assembled Silk Fibroin Biopolymer

resumo

In this study, the novel biomimetic aerogel-based composite scaffolds through a synergistic combination of wet chemical synthesis and advanced engineering approaches have successfully designed. To this aim, initially the photo-crosslinkable methacrylated silk fibroin (SF-MA) biopolymer and methacrylated hollow mesoporous silica microcapsules (HMSC-MA) as the main constituents of the novel composite aerogels were synthesized. Afterward, by incorporation of drug-loaded HMSC-MA into the self-assembled SF-MA, printable gel-based composite inks are developed. By exploiting micro-extrusion-based three-dimensional (3D) printing, SF-MA-HMSC composite gels are printed by careful controlling their viscosity to provide a means to control the shape fidelity of the resulted printed gel constructs. The developed scaffold has shown a multitude of interesting biophysical and biological performances. Namely, thanks to the photo-crosslinking of the gel components during the 3D printing, the scaffolds become mechanically more stable than the pristine SF scaffolds. Also, freeze-casting the printed constructs generates further interconnectivity in the printed pore struts resulting in the scaffolds with hierarchically organized porosities necessary for cell infiltration and growth. Importantly, HMSC incorporated scaffolds promote antibacterial drug delivery, cellular ingrowth and proliferation, promoting osteoblastic differentiation by inducing the expression of osteogenic markers and matrix mineralization. Finally, the osteoconductive, -inductive, and anti-infective composite aerogels are expected to act as excellent bone implanting materials with an extra feature of local and sustained release of drug for efficient therapy of bone-related diseases.

palavras-chave

DIFFERENTIATION; TISSUE; OSTEOGENESIS; STIMULATION; DELIVERY; IONS

categoria

Biochemistry & Molecular Biology; Materials Science; Polymer Science

autores

Ng, P; Pinho, AR; Gomes, MC; Demidov, Y; Krakor, E; Grume, D; Herb, M; Le, K; Mano, J; Mathur, S; Maleki, H

nossos autores

agradecimentos

N. and A.R.P. contributed equally to this work. H.M. acknowledges the support of the Geramn Research Foundation (Projektnummer 467116484) Association of the Chemical Industry, the Chemical Industry Fund for the financial supports. This work was developed within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020 & UIDP/50011/2020, financed by national funds through the FCT/MEC and when appropriate co-financed by FEDER under the PT2020 Partnership Agreement. H.M. acknowledges the support of Michael Schramm and Prof. Martin Kronke for conducting antibacterial tests and Jaqueline Auer for micro and nanoCT analyses.; Open access funding enabled and organized by Projekt DEAL.

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