Mechanically Strong Silica-Silk Fibroin Bioaerogel: A Hybrid Scaffold with Ordered Honeycomb Micromorphology and Multiscale Porosity for Bone Regeneration

Hajar Maleki, Mohammad-Ali Shahbazi*, Susan Montes, Seyed Hojjat Hosseini, Mohammad Reza Eskandari, Stefan Zaunschirm, Thomas Verwanger, Sanjay Mathur, Barbara Milow, Barbara Krammer, Nicola Hüsing

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Due to the synergic feature of individual components in hybrid (nano)biomaterials, their application in regenerative medicine has drawn significant attention. Aiming to address all the current challenges of aerogel as a potent scaffold in bone tissue engineering application, we adopted a novel synthesis approach to synergistically improve the pore size regime and mechanical strength in the aerogel. The three-dimensional aerogel scaffold in this study has been synthesized through a versatile one-pot aqueous-based sol-gel hybridization/assembly of organosilane (tetraethyl orthosilicate) and silk fibroin (SF) biopolymer, followed by unidirectional freeze-casting of the as-prepared hybrid gel and supercritical drying. The developed ultralight silica-SF aerogel hybrids demonstrated a hierarchically organized porous structure with interesting honeycomb-shaped micromorphology and microstructural alignment (anisotropy) in varied length scales. The average macropore size of the hybrid aerogel lied in ∼0.5-18 μm and was systematically controlled with freeze-casting conditions. Together with high porosity (91-94%), high Young's modulus (∼4-7 MPa, >3 order of magnitude improvement compared to their pristine aerogel counterparts), and bone-type anisotropy in the mechanical compressive behavior, the silica-SF hybrid aerogel of this study acted as a very competent scaffold for bone tissue formation. The results of in vitro assessments revealed that the silica-SF aerogel is not only cytocompatible and nonhemolytic but also acted as an open porous microenvironment to trigger osteoblast cell attachment, growth, and proliferation on its surface within 14 days of incubation. Moreover, to support the in vitro results, in vivo bone formation within the aerogel implant in the bone defect site was studied. The X-ray radiology and microcomputed tomography analyses confirmed that a significant new bone tissue density formed in the defect site within 25 days of implantation. Also, in vivo toxicology studies showed a zero-toxic impact of the aerogel implant on the blood biochemical and hematological parameters. Finally, the study clearly shows the potential of aerogel as a bioactive and osteoconductive open porous cellular matrix for a successful osseointegration process.
Original languageEnglish
JournalACS Applied Materials and Interfaces
Volume11
Issue number19
Pages (from-to)17256-17269
ISSN1944-8244
DOIs
Publication statusPublished - 2019

Keywords

  • Silica
  • Silk fibroin
  • Hybrid aerogel
  • Sol−gel
  • Bone tissue engineering

Cite this

Maleki, Hajar ; Shahbazi, Mohammad-Ali ; Montes, Susan ; Hosseini, Seyed Hojjat ; Eskandari, Mohammad Reza ; Zaunschirm, Stefan ; Verwanger, Thomas ; Mathur, Sanjay ; Milow, Barbara ; Krammer, Barbara ; Hüsing, Nicola. / Mechanically Strong Silica-Silk Fibroin Bioaerogel: A Hybrid Scaffold with Ordered Honeycomb Micromorphology and Multiscale Porosity for Bone Regeneration. In: ACS Applied Materials and Interfaces. 2019 ; Vol. 11, No. 19. pp. 17256-17269.
@article{a7cca79c83b44ffb94e694231f100cbd,
title = "Mechanically Strong Silica-Silk Fibroin Bioaerogel: A Hybrid Scaffold with Ordered Honeycomb Micromorphology and Multiscale Porosity for Bone Regeneration",
abstract = "Due to the synergic feature of individual components in hybrid (nano)biomaterials, their application in regenerative medicine has drawn significant attention. Aiming to address all the current challenges of aerogel as a potent scaffold in bone tissue engineering application, we adopted a novel synthesis approach to synergistically improve the pore size regime and mechanical strength in the aerogel. The three-dimensional aerogel scaffold in this study has been synthesized through a versatile one-pot aqueous-based sol-gel hybridization/assembly of organosilane (tetraethyl orthosilicate) and silk fibroin (SF) biopolymer, followed by unidirectional freeze-casting of the as-prepared hybrid gel and supercritical drying. The developed ultralight silica-SF aerogel hybrids demonstrated a hierarchically organized porous structure with interesting honeycomb-shaped micromorphology and microstructural alignment (anisotropy) in varied length scales. The average macropore size of the hybrid aerogel lied in ∼0.5-18 μm and was systematically controlled with freeze-casting conditions. Together with high porosity (91-94{\%}), high Young's modulus (∼4-7 MPa, >3 order of magnitude improvement compared to their pristine aerogel counterparts), and bone-type anisotropy in the mechanical compressive behavior, the silica-SF hybrid aerogel of this study acted as a very competent scaffold for bone tissue formation. The results of in vitro assessments revealed that the silica-SF aerogel is not only cytocompatible and nonhemolytic but also acted as an open porous microenvironment to trigger osteoblast cell attachment, growth, and proliferation on its surface within 14 days of incubation. Moreover, to support the in vitro results, in vivo bone formation within the aerogel implant in the bone defect site was studied. The X-ray radiology and microcomputed tomography analyses confirmed that a significant new bone tissue density formed in the defect site within 25 days of implantation. Also, in vivo toxicology studies showed a zero-toxic impact of the aerogel implant on the blood biochemical and hematological parameters. Finally, the study clearly shows the potential of aerogel as a bioactive and osteoconductive open porous cellular matrix for a successful osseointegration process.",
keywords = "Silica, Silk fibroin, Hybrid aerogel, Sol−gel, Bone tissue engineering",
author = "Hajar Maleki and Mohammad-Ali Shahbazi and Susan Montes and Hosseini, {Seyed Hojjat} and Eskandari, {Mohammad Reza} and Stefan Zaunschirm and Thomas Verwanger and Sanjay Mathur and Barbara Milow and Barbara Krammer and Nicola H{\"u}sing",
year = "2019",
doi = "10.1021/acsami.9b04283",
language = "English",
volume = "11",
pages = "17256--17269",
journal = "A C S Applied Materials and Interfaces",
issn = "1944-8244",
publisher = "American Chemical Society",
number = "19",

}

Maleki, H, Shahbazi, M-A, Montes, S, Hosseini, SH, Eskandari, MR, Zaunschirm, S, Verwanger, T, Mathur, S, Milow, B, Krammer, B & Hüsing, N 2019, 'Mechanically Strong Silica-Silk Fibroin Bioaerogel: A Hybrid Scaffold with Ordered Honeycomb Micromorphology and Multiscale Porosity for Bone Regeneration', ACS Applied Materials and Interfaces, vol. 11, no. 19, pp. 17256-17269. https://doi.org/10.1021/acsami.9b04283

Mechanically Strong Silica-Silk Fibroin Bioaerogel: A Hybrid Scaffold with Ordered Honeycomb Micromorphology and Multiscale Porosity for Bone Regeneration. / Maleki, Hajar; Shahbazi, Mohammad-Ali; Montes, Susan; Hosseini, Seyed Hojjat; Eskandari, Mohammad Reza; Zaunschirm, Stefan; Verwanger, Thomas; Mathur, Sanjay; Milow, Barbara; Krammer, Barbara; Hüsing, Nicola.

In: ACS Applied Materials and Interfaces, Vol. 11, No. 19, 2019, p. 17256-17269.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Mechanically Strong Silica-Silk Fibroin Bioaerogel: A Hybrid Scaffold with Ordered Honeycomb Micromorphology and Multiscale Porosity for Bone Regeneration

AU - Maleki, Hajar

AU - Shahbazi, Mohammad-Ali

AU - Montes, Susan

AU - Hosseini, Seyed Hojjat

AU - Eskandari, Mohammad Reza

AU - Zaunschirm, Stefan

AU - Verwanger, Thomas

AU - Mathur, Sanjay

AU - Milow, Barbara

AU - Krammer, Barbara

AU - Hüsing, Nicola

PY - 2019

Y1 - 2019

N2 - Due to the synergic feature of individual components in hybrid (nano)biomaterials, their application in regenerative medicine has drawn significant attention. Aiming to address all the current challenges of aerogel as a potent scaffold in bone tissue engineering application, we adopted a novel synthesis approach to synergistically improve the pore size regime and mechanical strength in the aerogel. The three-dimensional aerogel scaffold in this study has been synthesized through a versatile one-pot aqueous-based sol-gel hybridization/assembly of organosilane (tetraethyl orthosilicate) and silk fibroin (SF) biopolymer, followed by unidirectional freeze-casting of the as-prepared hybrid gel and supercritical drying. The developed ultralight silica-SF aerogel hybrids demonstrated a hierarchically organized porous structure with interesting honeycomb-shaped micromorphology and microstructural alignment (anisotropy) in varied length scales. The average macropore size of the hybrid aerogel lied in ∼0.5-18 μm and was systematically controlled with freeze-casting conditions. Together with high porosity (91-94%), high Young's modulus (∼4-7 MPa, >3 order of magnitude improvement compared to their pristine aerogel counterparts), and bone-type anisotropy in the mechanical compressive behavior, the silica-SF hybrid aerogel of this study acted as a very competent scaffold for bone tissue formation. The results of in vitro assessments revealed that the silica-SF aerogel is not only cytocompatible and nonhemolytic but also acted as an open porous microenvironment to trigger osteoblast cell attachment, growth, and proliferation on its surface within 14 days of incubation. Moreover, to support the in vitro results, in vivo bone formation within the aerogel implant in the bone defect site was studied. The X-ray radiology and microcomputed tomography analyses confirmed that a significant new bone tissue density formed in the defect site within 25 days of implantation. Also, in vivo toxicology studies showed a zero-toxic impact of the aerogel implant on the blood biochemical and hematological parameters. Finally, the study clearly shows the potential of aerogel as a bioactive and osteoconductive open porous cellular matrix for a successful osseointegration process.

AB - Due to the synergic feature of individual components in hybrid (nano)biomaterials, their application in regenerative medicine has drawn significant attention. Aiming to address all the current challenges of aerogel as a potent scaffold in bone tissue engineering application, we adopted a novel synthesis approach to synergistically improve the pore size regime and mechanical strength in the aerogel. The three-dimensional aerogel scaffold in this study has been synthesized through a versatile one-pot aqueous-based sol-gel hybridization/assembly of organosilane (tetraethyl orthosilicate) and silk fibroin (SF) biopolymer, followed by unidirectional freeze-casting of the as-prepared hybrid gel and supercritical drying. The developed ultralight silica-SF aerogel hybrids demonstrated a hierarchically organized porous structure with interesting honeycomb-shaped micromorphology and microstructural alignment (anisotropy) in varied length scales. The average macropore size of the hybrid aerogel lied in ∼0.5-18 μm and was systematically controlled with freeze-casting conditions. Together with high porosity (91-94%), high Young's modulus (∼4-7 MPa, >3 order of magnitude improvement compared to their pristine aerogel counterparts), and bone-type anisotropy in the mechanical compressive behavior, the silica-SF hybrid aerogel of this study acted as a very competent scaffold for bone tissue formation. The results of in vitro assessments revealed that the silica-SF aerogel is not only cytocompatible and nonhemolytic but also acted as an open porous microenvironment to trigger osteoblast cell attachment, growth, and proliferation on its surface within 14 days of incubation. Moreover, to support the in vitro results, in vivo bone formation within the aerogel implant in the bone defect site was studied. The X-ray radiology and microcomputed tomography analyses confirmed that a significant new bone tissue density formed in the defect site within 25 days of implantation. Also, in vivo toxicology studies showed a zero-toxic impact of the aerogel implant on the blood biochemical and hematological parameters. Finally, the study clearly shows the potential of aerogel as a bioactive and osteoconductive open porous cellular matrix for a successful osseointegration process.

KW - Silica

KW - Silk fibroin

KW - Hybrid aerogel

KW - Sol−gel

KW - Bone tissue engineering

U2 - 10.1021/acsami.9b04283

DO - 10.1021/acsami.9b04283

M3 - Journal article

VL - 11

SP - 17256

EP - 17269

JO - A C S Applied Materials and Interfaces

JF - A C S Applied Materials and Interfaces

SN - 1944-8244

IS - 19

ER -