Pathway-Driven Peptide–Bioglass Nanocomposites as the Dynamic and Self-Healable Matrix

Abstract

Peptide hydrogels have recently emerged as potential biomaterials for designing synthetic scaffolds in tissue engineering. We demonstrate pathway-controlled self-assembly of peptide amphiphile 1 to furnish kinetically controlled nanofibers (1 NF ) and thermodynamically stable twisted helical bundles (1 TB ). These supramolecular nanostructures with varied persistence lengths promote in situ mineralization to yield templated bioactive glass composites, 1 NF BG and 1 TB BG − resorbable, mesoporous, and degradable biomaterials as bone scaffolds. The structural features of the hydrogel composites are investigated extensively with microscopic characterization, energydispersive X-ray spectroscopy, Raman spectroscopy, and XPS to conclude 1 TB BG as the superior material with higher percentage of open network structures as obtained from ratios of nonbridging and bridging oxygen. The hydrogel composites show excellent dynamic and self-healing behavior from rheological studies, especially the elastic modulus of 1 TB BG being almost comparable to natural bone. Upon incubation in simulated body fluid, the bioglass composites illustrate tunable bioactive response mediated by the structural and topological control to induce the deposition of multiphasic calcium phosphate along with octacalcium phosphate and carbonate hydroxyapatite. Finally, such spatiotemporal composites facilitate stiffness-controlled osteoblast cellular interactions to support U2OS subsistence in the hydrogel matrix, highlighting their potential as a substrate for osteoblast growth for prolonged culture periods and in 3D bone tissue modeling.

Bio‐Inspired Synthesis of Hollow Mesoporous Bioactive Glass Nanoparticles Using Calcium Carbonate as Solid Template

“…We have previously carried out synthesis of mesoporous bioactive glass nanoparticles in presence of structure directing templates like Calf Thymus (CT) DNA, [15] gelatin, [16] normal and grafted cellulose, [17] pectin‐collagen composites, [18] self‐assembling peptides, [19] etc. under ambient conditions mostly without involving organic solvents and surfactants.…”

Modulation of flexo-rigid balance in photoresponsive thymine grafted copolymers towards designing smart healable coating

“… 5 As compared to the extrinsic self-healing mechanism involving the breakage of microcapsule to release the stored healing agents for single time healing, intrinsic self-healing has the advantages of reduced costs and multiple cycles of healings. Such intrinsic mechanism entails reversible interactions such as hydrogen bonding, 6 host–guest interactions, 7 metal–ligand complexations, 8 ionic interactions, 9 π–π stacking interactions, 10 dynamic covalent chemistry 11 to efficiently mend the damage. Further, control over such interactions by the intervention of external stimuli renders the self-healing processes autonomic or non-autonomic.…”

Mechanical Integrity in a Dynamic Interpenetrating Hydrogel Network of Supramolecular Peptide–Polysaccharide Supports Enhanced Chondrogenesis

“…Collagen type 2 (COL2A1) and aggrecan (ACAN) that are the main markers for hyaline cartilage were found to consistently increase with culture time, indicating that the hydrogels supported the production of the cartilage-specific extracellular matrix (Figure A,B) . The expression levels of these biomolecules were comparatively higher in P2 than in P0 , which might be ascribed to the presence of the ECM mimic, peptide 1 NF . Likewise, SOX9, one of the transcription factors known to be a regulator of chondrogenic differentiation, induces the production of cartilage-specific ECM.…”

“…The mechanical strength of the above network was further reinforced by the introduction of the supramolecular engineered minimalistic peptide sequence, 1 . The kinetically controlled, robust self-assembled fibers , were incorporated through the Schiff base mediated polysaccharide network to render an interpenetrating network of supramolecular peptide fibers within the polysaccharide hydrogel network. The supramolecular peptide fibers associated with the dynamic covalent imine bond served as sacrificial bonds resulting in the efficient dissipation of energy and fast recovery of the hydrogel network.…”