Abstract
Cellprene™ is a recently developed polymeric blend based on poly(lactide-co-glycolide) (PLGA)/polyisoprene (PI) with good biological performance for biomedical applications. However, its potential as fiber scaffold in tissue engineering is still unknown, and the influence of processing parameters is yet to be understood. In this study, several compositions based on PLGA/PI blend mixed with hydroxyapatite (HAp) and polyethylene glycol (PEG) were prepared by solvent casting. Then, the membranes were used to produce micro/nanofibers by centrifugal spinning (CS) and electrospinning (ES). The viscosity’s effect was studied to find an ideal viscosity value to produce homogeneous micro/nanofibers. The in vitro bioactivity test was also performed. Rheological results showed that the best viscosity range was (0.105 Pa s > η > 0.138 Pa s) for CS; larger fibers of ES were produced with lower viscosities. The sample with the lowest HAp concentration exhibited thinner and more homogeneous non-beaded fibers and proved its bioactivity response.
Similar content being viewed by others
References
A. Asti and L. Gioglio: Natural and synthetic biodegradable polymers: Different scaffolds for cell expansion and tissue formation. Int. J. Artif. Organs 37, 187 (2014).
K. Wei, Y. Li, K.-O. Kim, Y. Nakagawa, B.-S. Kim, K. Abe, G.-Q. Chen, and I.-S. Kim: Fabrication of nano-hydroxyapatite on electrospun silk fibroin nanofiber and their effects in osteoblastic behavior. J. Biomed. Mater. Res. A 97A, 272 (2011).
J. Liuyun, L. Yubao, and X. Chengdong: Preparation and biological properties of a novel composite scaffold of nano-hydroxyapatite/chitosan/carboxymethyl cellulose for bone tissue engineering. J. Biomed. Sci. 16, 65 (2009).
T. Prasad, E.A. Shabeena, D. Vinod, T.V. Kumary, and P.R. Anil Kumar: Characterization and in vitro evaluation of electrospun chitosan/polycaprolactone blend fibrous mat for skin tissue engineering. J. Mater. Sci. Mater. Med. 26, 5352 (2015).
C. Dong and Y. Lv: Application of collagen scaffold in tissue engineering: Recent advances and new perspectives. Polymers 8, 42 (2016).
S.H. Xia, S.H. Teng, and P. Wang: Synthesis of bioactive polyvinyl alcohol/silica hybrid fibers for bone regeneration. Mater. Lett. 213, 181 (2018).
B.N. Singh and K. Pramanik: Development of novel silk fibroin/polyvinyl alcohol/sol-gel bioactive glass composite matrix by modified layer by layer electrospinning method for bone tissue construct generation. Biofabrication 9, 015028 (2017).
M. Abbasian, B. Massoumi, R. Mohammad-Rezaei, H. Samadian, and M. Jaymand: Scaffolding polymeric biomaterials: Are naturally occurring biological macromolecules more appropriate for tissue engineering? Int. J. Biol. Macromol. 134, 673 (2019).
D.R. Marques, L.A. dos Santos, V.C. Sousa, P.R.S. Sanches, and A.V. Macedo Neto: Blendas Poliméricas de Poli (Ácido Láctico-co-Glicólico) e Poliisopreno. BR Patent registration number: 0000221010682444, 2011.
_Universidade Federal do Rio Grande do Sul. Pedido de Registro de Marca de Produto (Nominativa). BR Patent registration number: 906982910, 2013.
D.R. Marques, L.A. dos Santos, L.F. Schopf, and J.C.S. de Fraga: Analysis of poly(lactic-co-glycolic acid)/poly(isoprene) polymeric blend for application as biomaterial. Polímeros 2, 579 (2013).
H.Y. Mi, S.M. Palumbo, X. Jing, L.-S. Turng, W.-J. Li, and X.-F. Peng: Thermoplastic polyurethane/hydroxyapatite electrospun scaffolds for bone tissue engineering: Effects of polymer properties and particle size. J. Biomed. Mater. Res. B Appl. Biomater. 102, 1434 (2014).
S.I. Jeong, E.K. Ko, J. Yum, C.H. Jung, Y.M. Lee, and H. Shin: Nanofibrous poly(lactic acid)/hydroxyapatite composite scaffolds for guided tissue regeneration. Macromol. Biosci. 8, 328 (2008).
S.Y. Heo, J.W. Seol, and N.S. Kim: Characterisation and assessment of electrospun poly/hydroxyapatite nanofibres together with a cell adhesive for bone repair applications. Vet Med 59, 498 (2014).
D. Banerjee and S. Bose: Effects of polymer chemistry, concentration, and pH on doxorubicin release kinetics from hydroxyapatite-PCL-PLGA composite. J. Mater. Res. 34, 1692 (2019).
T. Hou, X. Li, Y. Lu, and B. Yang: Highly porous fibers prepared by centrifugal spinning. Mater. Des. 114, 303–311 (2017).
D. Salamon, S. Teixeira, S.M. Dutczak, and D.F. Stamatialis: Facile method of building hydroxyapatite 3D scaffolds assembled from porous hollow fibers enabling nutrient delivery. Ceram. Int. 40, 14793 (2014).
H.R. Pant, M.P. Neupane, B. Pant, G. Panthi, H.J. Oh, M.H. Lee, and H.Y. Kim: Fabrication of highly porous poly(e-caprolactone) fibers for novel tissue scaffold via water-bath electrospinning. Colloids Surf. B 88, 587 (2011).
D.E. Mogosanu, R. Verplancke, P. Dubruel, and J. Vanfleteren: Fabrication of 3-dimensional biodegradable microfluidic environments for tissue engineering applications. Mater. Des. 89, 1315 (2016).
H. Wu, J. Kong, X. Yao, C. Zhao, Y. Dong, and X. Lu: Polydopamine-assisted attachment of β-cyclodextrin on porous electrospun fibers for water purification under highly basic condition. Chem. Eng. J. 270, 101 (2015).
B. Wang, J.L. Cheng, Y.P. Wu, D. Wang, and D.N. He: Porous NiO fibers prepared by electrospinning as high performance anode materials for lithium ion batteries. Electrochem. Commun. 23, 5 (2012).
F. Dabirian, S.A. Hosseini Ravandi, A.R. Pishevar, and R.A. Abuzade: A comparative study of jet formation and nanofiber alignment in electrospinning and electrocentrifugal spinning systems. J. Electrostat. 69, 540 (2011).
G.M. Gonzalez, L.A. MacQueen, J.U. Lind, S.A. Fitzgibbons, C.O. Chantre, I. Huggler, H.M. Golecki, J.A. Goss, and K.K. Parker: Production of synthetic, para-aramid and biopolymer nanofibers by immersion rotary jet-spinning. Macromol. Mater. Eng. 302, 1600365 (2017).
H. Rodríguez-Tobías, G. Morales, and D. Grande: Comprehensive review on electrospinning techniques as versatile approaches toward antimicrobial biopolymeric composite fiber. Mater. Sci. Eng. C 101, 306 (2019).
G. Jin, R. He, B. Sha, W. Li, H. Qing, R. Teng, and F. Xu: Electrospun three-dimensional aligned nano fibrous scaffolds for tissue engineering. Mater. Sci. Eng. C 92, 995 (2018).
F.A. Vechietti, D. Marques, N.O. Muniz, and L.A. Santos: Fibers obtaining and characterization using poly(lactic-co-glycolic acid) and poly(isoprene) containing hydroxyapatite and α TCP calcium phosphate by electrospinning method. Key Eng. Mater. 631, 173 (2015).
L. Zhang, Z. Wang, Y. Xiao, P. Liu, S. Wang, Y. Zhao, M. Shen, and X. Shi: Electrospun PEGylated PLGA nanofibers for drug encapsulation and release. Mater. Sci. Eng. C 91, 255 (2018).
A.H. Touny, J.G. Lawrence, A.D. Jones, and S.B. Bhaduri: Effect of electrospinning parameters on the characterization of PLA/HNT nanocomposite fibers. J. Mater. Res. 25, 857 (2010).
J.J. Vázquez and E.S.M. Martínez: Collagen and elastin scaffold by electrospinning for skin tissue engineering applications. J. Mater. Res. 34, 2819 (2019).
R. Nayak, R. Padhye, I.L. Kyratzis, Y. Truong, and L. Arnold: Recent advances in nanofibre fabrication techniques. Text. Res. J. 82, 129 (2012).
X. Li, H. Chen, and B. Yang: Centrifugally spun starch-based fibers from amylopectin rich starches. Carbohydr. Polym. 137, 459 (2016).
P. Mellado, H.A. McIlwee, M.R. Badrossamay, J.A. Goss, L. Mahadevan, and K.K. Parker: A simple model for nanofiber formation by rotary jet-spinning. Appl. Phys. Lett. 99, 203107 (2011).
S. Ramakrishna, W. Teo, T. Lim, and Z. Ma: An Introduction to Electrospinning and Nanofibers (World Scientific Publishing Company, Singapore, 2005), p. 396.
S. Padron, A. Fuentes, D. Caruntu, and K. Lozano: Experimental study of nanofiber production through forcespinning. J. Appl. Phys. 113, 024318 (2013).
M.R. Badrossamay, H.A. McIlwee, J.A. Goss, and K.K. Parker: Nanofiber assembly by rotary jet-spinning. Nano Lett. 10, 2257 (2010).
G. Leng, X. Zhang, T. Shi, G. Chen, X. Wu, Y. Liu, M. Fang, X. Min, and Z. Huang: Preparation and properties of polystyrene/silica fibres flexible thermal insulation materials by centrifugal spinning. Polymer 185, 121964 (2019).
L. Wang, J. Shi, L. Liu, E. Secret, and Y. Chen: Fabrication of polymer fiber scaffolds by centrifugal spinning for cell culture studies. Microelectron. Eng. 88, 1718 (2011).
E. Stojanovska, E. Canbay, E.S. Pampal, M.D. Calisir, O. Agma, Y. Polat, R. Simsek, N.A.S. Gundogdu, Y. Akgul, and A. Kilic: A review on non-electro nanofibre spinning techniques. RSC Adv. 6, 83783 (2016).
S.P. Decent, A.C. King, M.J.H. Simmons, E.I. Parau, I.M. Wallwork, C.J. Gurney, and J. Uddin: The trajectory and stability of a spiralling liquid jet: Viscous theory. Appl. Math. Model. 33, 4283 (2009).
M.M. Machado-Paula, M.A.F. Corat, M. Lancellotti, G. Mi, F.R. Marciano, M.L. Vega, A.A. Hidalgo, T.J. Webster, and A.O. Lobo: A comparison between electrospinning and rotary-jet spinning to produce PCL fibers with low bacteria colonization. Mater. Sci. Eng. C 111, 110706 (2020).
F. Sun, J. Guo, Y. Liu, and Y. Yu: Preparation, characterizations and properties of sodium alginate grafted acrylonitrile/polyethylene glycol electrospun nanofibers. Int. J. Biol. Macromol. 137, 420 (2019).
R. Hobzova, Z. Hampejsova, T. Cerna, J. Hrabeta, K. Venclikova, J. Jedelska, U. Bakowsky, Z. Bosakova, M. Lhotka, S. Vaculin, M. Franek, M. Steinhart, J. Kovarova, J. Michalek, and J. Sirc: Poly(D,L-lactide)/polyethylene glycol micro/nanofiber mats as paclitaxel-eluting carriers: Preparation and characterization of fibers, in vitro drug release, antiangiogenic activity and tumor recurrence prevention. Mater. Sci. Eng. C 98, 982 (2019).
D.R. Marques: Fibras De Poli (Ácido Láctico-Co-Glicólico)/Poliisopreno Para Aplicação Em Engenharia De Tecidos. Ph.D. thesis, Universidade Federal do Rio Grande do Sul, 2015.
G.C. Pandey and P.B. Aswath: Synthesis of polylactic acid–polyglycolic acid blends using microwave radiation. J. Mech. Behav. Biomed. Mater. 1, 227 (2008).
B. Cengiz, Y. Gokce, N. Yildiz, Z. Aktas, and A. Calimli: Synthesis and characterization of hydroxyapatite nanoparticles. Colloids Surf. 322, 29 (2008).
L. Gan and R. Pilliar: Calcium phosphate sol–gel-derived thin films on porous-surfaced implants for enhanced osteoconductivity. Part I: Synthesis and characterization. Biomaterials 25, 5303 (2004).
C. Ilie, G. Stîngă, A. Iovescu, V. Purcar, D.F. Anghel, and D. Donescu: The influence of nonionic surfactants on the carbopol-peg interpolymer complexes. Rev. Roum. Chim. 55, 409 (2010).
S.R. Bhattarai, N. Bhattarai, P. Viswanathamurthi, H.K. Yi, P.H. Hwang, and H.Y. Kim: Hydrophilic nanofibrous structure of polylactide; fabrication and cell affinity. J. Biomed. Mater. Res. A 78, 247 (2006).
L.M. Buttaro, E. Drufva, and M.W. Frey: Phase separation to create hydrophilic yet non-water soluble PLA/PLA-b-PEG fibers via electrospinning. J. Appl. Polym. Sci. 131, 1 (2014).
V. Trakoolwannachai, P. Kheolamai, and S. Ummartyotin: Development of hydroxyapatite from eggshell waste and a chitosan-based composite: In vitro behavior of human osteoblast-like cell (Saos- 2) cultures. Int. J. Biol. Macromol. 134, 557 (2019).
S. Kar, T. Kaur, and A. Thirugnanam: Microwave-assisted synthesis of porous chitosan-modified montmorillonite–hydroxyapatite composite scaffolds. Int. J. Biol. Macromol. 82, 628 (2016).
L. Ren, V. Pandit, J. Elkin, T. Denman, J.A. Cooper, and S.P. Kotha: Large-scale and highly efficient synthesis of micro- and nano-fibers with controlled fiber morphology by centrifugal jet spinning for tissue regeneration. Nanoscale 5, 2337 (2013).
D. Quéré: Wetting and roughness. Annu. Rev. Mater. Res. 38, 71 (2008).
R. Junker, A. Dimakis, M. Thoneick, and J.A. Jansen: Effects of implant surface coatings and composition on bone integration: A systematic review. Clin. Oral Implants Res. 20, 185 (2009).
H.H. Lu, S.D. Subramony, M.K. Boushell, and X. Zhang: Tissue engineering strategies for the regeneration of orthopedic interfaces. Ann. Biomed. Eng. 38, 2142 (2010).
J. Costa-Rodrigues, A. Fernandes, M.A. Lopes, and M.H. Fernandes: Hydroxyapatite surface roughness: Complex modulation of the osteoclastogenesis of human precursor cells. Acta Biomater. 8, 1137 (2012).
L. Le Guéhennec, A. Soueidan, P. Layrolle, and Y. Amouriq: Surface treatments of titanium dental implants for rapid osseointegration. Dent. Mater. 23, 844 (2007).
C. Aparicio, A. Padrós, and F.-J. Gil: In vivo evaluation of micro-rough and bioactive titanium dental implants using histometry and pull-out tests. J. Mech. Behav. Biomed. Mater. 4, 1672 (2011).
J. Chen, M.A. Birch, and S.J. Bull: Nanomechanical characterization of tissue engineered bone grown on titanium alloy in vitro. J. Mater. Sci. Mater. Med. 21, 277–282 (2010).
N.B. Guerra: Obtenção e Avaliação Da Blenda Poliisopreno Epoxidado - Poli(Ácido Lático-Co-Glicólico) Para Engenharia de Tecidos. Ph.D. thesis, Universidade Federal do Rio Grande do Sul, 2018.
D.R. Marques, L.A.L. dos Santos, M.A. O'Brien, S.H. Cartmell, and J.E. Gough: In vitro evaluation of poly(lactic-co-glycolic acid)/polyisoprene fibers for soft tissue engineering. J. Biomed. Mater. Res. B 105, 2581 (2017).
K. Sungsanit, N. Kao, and S.N. Bhattacharya: Properties of linear poly(lactic acid)/polyethylene glycol blends. Polym. Eng. Sci. 52, 108 (2012).
A. Marcilla and M. Beltran: Handbook of Plasticizers (ChemTec Publishing, Toronto, 2004).
Y. Lu, Y. Li, S. Zhang, G. Xu, K. Fu, H. Lee, and X. Zhang: Parameter study and characterization for polyacrylonitrile nanofibers fabricated via centrifugal spinning process. Eur. Polym. J. 49, 3834 (2013).
R.T. Weitz, L. Harnau, S. Rauschenbach, M. Burghard, and K. Kern: Polymer nanofibers via nozzle-free centrifugal spinning. Nano Lett. 8, 1187 (2008).
Z. Zhang and J. Sun: Research on the development of the centrifugal spinning. MATEC Web Conf. 95, 07003 (2017).
Y. You, S.J. Lee, B.M. Min, and W.H. Park: Effect of solution properties on nanofibrous structure of electrospun poly(lactic-co-glycolic acid). J. Appl. Polym. Sci. 99, 1214 (2006).
H. Tan, R. Inai, M. Kotaki, and S. Ramakrishna: Systematic parameter study for ultra-fine fiber fabrication via electrospinning process. Polymer 46, 6128 (2005).
A.R. Faramarzi, J. Barzin, and H. Mobedi: Effect of solution and apparatus parameters on the morphology and size of electrosprayed PLGA microparticles. Fibers Polym. 17, 1806 (2016).
S.M. Troian, X.L. Wu, and S.A. Safran: Fingering instability in thin wetting films. Phys. Rev. Lett. 62, 1496 (1989).
H.E. Huppert: Flow and instability of a viscous current down a slope. Nature 300, 427 (1982).
F. Melo, J.F. Joanny, and S. Fauve: Fingering instability of spinning drops. Phys. Rev. Lett. 63, 1958 (1989).
C.B. Danoux, D. Barbieri, H. Yuan, J.D. de Bruijn, C.A. van Blitterswijk, and P. Habibovic: In vitro and in vivo bioactivity assessment of a polylactic acid/hydroxyapatite composite for bone regeneration. Biomatter 4, 1 (2014).
I. Rajzer: Fabrication of bioactive polycaprolactone/hydroxyapatite scaffolds with final bilayer nano-/micro-fibrous structures for tissue engineering application. J. Mater. Sci. 49, 5799 (2014).
M.H. Santos, M. De Oliveira, L.P.D.F. Souza, H.S. Mansur, and W.L. Vasconcelos: Synthesis control and characterization of hydroxyapatite prepared by wet precipitation process. Mater. Res. 7, 625 (2004).
H. Kim, T. Himeno, T. Kokubo, and T. Nakamura: Process and kinetics of bonelike apatite formation on sintered hydroxyapatite in a simulated body fluid. Biomaterials 26, 4366 (2005).
A. Olad and F.F. Azhar: The synergetic effect of bioactive ceramic and nanoclay on the properties of chitosan–gelatin/nanohydroxyapatite–montmorillonite scaffold for bone tissue engineering. Ceram. Int. 40, 10061 (2014).
L. Liverani, J. Lacina, J.A. Roether, E. Boccardi, M.S. Killian, P. Schmuki, D.W. Schubert, and A.R. Boccaccini: Incorporation of bioactive glass nanoparticles in electrospun PCL/chitosan fibers by using benign solvents. Bioact. Mater. 3, 55 (2018).
Z. Shahbazarab, A. Teimouri, A.N. Chermahini, and M. Azadi: Fabrication and characterization of nanobiocomposite scaffold of zein/chitosan/nanohydroxyapatite prepared by freeze-drying method for bone tissue engineering. Int. J. Biol. Macromol. 108, 1017 (2018).
Y. Tsuneizumi, M. Kuwahara, K. Okamoto, and S. Matsumura: Chemical recycling of poly(lactic acid) based polymer blends using environmentally benign catalysts. Polym. Degrad. Stab. 95, 1387 (2010).
S. Ramesh, C.Y. Tan, S.B. Bhaduri, and W.D. Teng: Rapid densification of nanocrystalline hydroxyapatite for biomedical applications. Ceram. Int. 33, 1363 (2007).
T. Kokubo and H. Takadama: How useful is SBF in predicting in vivo bone bioactivity? Biomaterials 27, 2907 (2006).
Acknowledgments
The authors gratefully acknowledge Coordination for the Improvement of Higher Education Personnel (CAPES–Brazil), National Council for Scientific and Technological Development (CNPQ–Brazil), Research Foundation of the State of Rio Grande do Sul (FAPERGS–Brazil), Funding Authority for Studies and Projects (FINEP–Brazil), and Erasmus for their financial support.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Muniz, N.O., Vechietti, F.A., Anesi, G.R. et al. Blend-based fibers produced via centrifugal spinning and electrospinning processes: Physical and rheological properties. Journal of Materials Research 35, 2905–2916 (2020). https://doi.org/10.1557/jmr.2020.189
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1557/jmr.2020.189