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Cited by 39Bone Tissue Engineering MaterialsAdvanced Cellulose Research Studiesbiodegradable polymer synthesis and properties

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Bioactive Cellulose Nanocrystal-Poly(ε-Caprolactone) Nanocomposites for Bone Tissue Engineering Applications

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Hong, Jung Ki, Cooke, Shelley L., Whittington, Abby R., Roman, Maren·2021·Frontiers in Bioengineering and Biotechnology
DOI 10.3389/fbioe.2021.605924PMC PMC7947866
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Abstract

3D-printed bone scaffolds hold great promise for the individualized treatment of critical-size bone defects. Among the resorbable polymers available for use as 3D-printable scaffold materials, poly(ε-caprolactone) (PCL) has many benefits. However, its relatively low stiffness and lack of bioactivity limit its use in load-bearing bone scaffolds. This study tests the hypothesis that surface-oxidized cellulose nanocrystals (SO-CNCs), decorated with carboxyl groups, can act as multi-functional scaffold additives that (1) improve the mechanical properties of PCL and (2) induce biomineral formation upon PCL resorption. To this end, an in vitro biomineralization study was performed to assess the ability of SO-CNCs to induce the formation of calcium phosphate minerals. In addition, PCL nanocomposites containing different amounts of SO-CNCs (1, 2, 3, 5, and 10 wt%) were prepared using melt compounding extrusion and characterized in terms of Young's modulus, ultimate tensile strength, crystallinity, thermal transitions, and water contact angle. Neither sulfuric acid-hydrolyzed CNCs (SH-CNCs) nor SO-CNCs were toxic to MC3T3 preosteoblasts during a 24 h exposure at concentrations ranging from 0.25 to 3.0 mg/mL. SO-CNCs were more effective at inducing mineral formation than SH-CNCs in simulated body fluid (1x). An SO-CNC content of 10 wt% in the PCL matrix caused a more than 2-fold increase in Young's modulus (stiffness) and a more than 60% increase in ultimate tensile strength. The matrix glass transition and melting temperatures were not affected by the SO-CNCs but the crystallization temperature increased by about 5.5°C upon addition of 10 wt% SO-CNCs, the matrix crystallinity decreased from about 43 to about 40%, and the water contact angle decreased from 87 to 82.6°. The abilities of SO-CNCs to induce calcium phosphate mineral formation and increase the Young's modulus of PCL render them attractive for applications as multi-functional nanoscale additives in PCL-based bone scaffolds.

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Crossref · 10.3389/fbioe.2021.605924

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Figures

Figure 1 Conductometric titration curves for (A) SH-CNC-I and (B) SO-CNC-I.
Figure 1 Conductometric titration curves for (A) SH-CNC-I and (B) SO-CNC-I.CC BY · PubMed Central
Figure 2 3D AFM height images of SH-CNCs (A,B) and SO-CNCs (C,D) before (A,C) and after (B,D) 400 h incubation in SBF at 37°C.
Figure 2 3D AFM height images of SH-CNCs (A,B) and SO-CNCs (C,D) before (A,C) and after (B,D) 400 h incubation in SBF at 37°C.CC BY · PubMed Central
Figure 3 Height changes of CNCs during the incubation in SBF at 37°C.
Figure 3 Height changes of CNCs during the incubation in SBF at 37°C.CC BY · PubMed Central
Figure 4 AFM phase images of SH-CNCs (A,B) and SO-CNCs (C,D) before (A,C) and after (B,D) 400 h incubation in SBF at 37°C. Scan size: 2 μm x 2 μm.
Figure 4 AFM phase images of SH-CNCs (A,B) and SO-CNCs (C,D) before (A,C) and after (B,D) 400 h incubation in SBF at 37°C. Scan size: 2 μm x 2 μm.CC BY · PubMed Central
Figure 5 Cytotoxicity of MC3T3 cells after 24 h exposure to SH-CNCs and SO-CNCs. Each data set mean value was normalized to the DI water control, data showed no significant difference in means (p < 0.05) compared to the control. Error bars represent one standard deviation.
Figure 5 Cytotoxicity of MC3T3 cells after 24 h exposure to SH-CNCs and SO-CNCs. Each data set mean value was normalized to the DI water control, data showed no significant difference in means (p < 0.05) compared to the control. Error bars represent one standard deviation.CC BY · PubMed Central
Figure 6 Mechanical properties of SO-CNC/PCL nanocomposite filaments. Insert: Stress-strain curves of the nanocomposite filaments.
Figure 6 Mechanical properties of SO-CNC/PCL nanocomposite filaments. Insert: Stress-strain curves of the nanocomposite filaments.CC BY · PubMed Central
Figure 7 DSC curves (2nd heating and 2nd cooling) of pure PCL and SO-CNC/PCL nanocomposite filament containing 10 wt% SO-CNC.
Figure 7 DSC curves (2nd heating and 2nd cooling) of pure PCL and SO-CNC/PCL nanocomposite filament containing 10 wt% SO-CNC.CC BY · PubMed Central

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Metadata

Authors
Hong, J. K., Cooke, S. L., Whittington, A. R., & Roman, M.
Affiliations
Virginia Tech (US)
Corresponding author
Roman, Maren
ORCID
Venue
Frontiers in Bioengineering and Biotechnology
Publisher
Frontiers Media SA
Published
2021-02-25
Volume
9
Pages
605924-605924
ISSN
2296-4185 (ISSN-L)
DOI
10.3389/fbioe.2021.605924
PMC
PMC7947866
OpenAlex
W3133428517
Cited by
39
References
50
Citations by year
2026: 7 · 2025: 4 · 2024: 6 · 2023: 9 · 2022: 9 · 2021: 4
FWCI
2.13
Type
journal article
Language
en
Open access
Licence
Locations
  • Frontiers in Bioengineering and Biotechnology (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
  • VTechWorks (Virginia Tech) (submittedVersion, cc-by)
Funders
  • National Science Foundation
  • U.S. Department of Agriculture
  • Virginia Agricultural Experiment Station, Virginia Polytechnic Institute and State University
  • Institute for Critical Technology and Applied Science
Topics
  • Physical Sciences › Engineering › Biomedical Engineering › Bone Tissue Engineering Materials
  • Physical Sciences › Materials Science › Biomaterials › Advanced Cellulose Research Studies
  • Physical Sciences › Materials Science › Biomaterials › biodegradable polymer synthesis and properties
Keywords
cellulose nanocrystals, polycaprolactone, bone tissue engineering, 3D-printed bone scaffolds, biomineralization, mechanical properties, Young's modulus, tensile strength, crystallinity, water contact angle, biocompatibility, critical-size bone defect, resorbable polymers

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