1. De Novo Design of Functional Coassembling Organic–Inorganic Hydrogels for Hierarchical Mineralization and Neovascularization
- Author
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Delali K. Boccorh, Babatunde O. Okesola, Alvaro Mata, Richard O.C. Oreffo, Sherif Elsharkawy, Yuanhao Wu, Jonathan I. Dawson, Dave J. Adams, David Osuna de la Peña, Ana Karen Mendoza-Martinez, Dafna Knani, Alastair W. Wark, Gianluca Cidonio, and Burak Derkus
- Subjects
Nanofibers ,Supramolecular chemistry ,General Physics and Astronomy ,02 engineering and technology ,Matrix (biology) ,010402 general chemistry ,01 natural sciences ,Article ,Adsorption ,Amphiphile ,coassembly ,Humans ,QD ,General Materials Science ,multicomponent biomaterials ,Chemistry ,nanocomposite hydrogels ,General Engineering ,Hydrogels ,Mesenchymal Stem Cells ,biomineralization ,021001 nanoscience & nanotechnology ,peptide amphiphiles ,0104 chemical sciences ,laponite ,Durapatite ,Chemical engineering ,Nanofiber ,Self-healing hydrogels ,Nanorod ,Rheology ,0210 nano-technology ,supramolecular ,Biomineralization - Abstract
Synthetic nanostructured materials incorporating both organic and inorganic components offer a unique, powerful, and versatile class of materials for widespread applications due to the distinct, yet complementary, nature of the intrinsic properties of the different constituents. We report a supramolecular system based on synthetic nanoclay (Laponite,bLap/b) and peptide amphiphiles (PAs,bPAH3/b) rationally designed to coassemble into nanostructured hydrogels with high structural integrity and a spectrum of bioactivities. Spectroscopic and scattering techniques and molecular dynamic simulation approaches were harnessed to confirm thatbPAH3/bnanofibers electrostatically adsorbed and conformed to the surface ofbLap/bnanodisks. Electron and atomic force microscopies also confirmed an increase in diameter and surface area ofbPAH3/bnanofibers after coassembly withbLap/b. Dynamic oscillatory rheology revealed that the coassembledbPAH3-Lap/bhydrogels displayed high stiffness and robust self-healing behavior while gas adsorption analysis confirmed a hierarchical and heterogeneous porosity. Furthermore, this distinctive structure within the three-dimensional (3D) matrix provided spatial confinement for the nucleation and hierarchical organization of high-aspect ratio hydroxyapatite nanorods into well-defined spherical clusters within the 3D matrix. Applicability of the organic-inorganicbPAH3-Lap/bhydrogels was assessediin vitro/iusing human bone marrow-derived stromal cells (hBMSCs) andiex vivo/iusing a chick chorioallantoic membrane (CAM) assay. The results demonstrated that the organic-inorganicbPAH3-Lap/bhydrogels promote human skeletal cell proliferation and, upon mineralization, integrate with the CAM, are infiltrated by blood vessels, stimulate extracellular matrix production, and facilitate extensive mineral deposition relative to the controls.
- Published
- 2021