abstract
Piezoelectricity is considered to be one of the key functionalities in biomaterials to boost bone tissue regeneration, however, integrating biocompatibility, biodegradability and 3D structure with pronounced piezoresponse remains a material challenge. Herein, novel hybrid biocompatible 3D scaffolds based on biodegradable poly(3-hydroxybutyrate) (PHB) and reduced graphene oxide (rGO) flakes have been developed. Nanoscale insights revealed a more homogenous distribution and superior surface potential values of PHB fibers (33 +/- 29 mV) with increasing rGO content up to 1.0 wt% (314 +/- 31 mV). The maximum effective piezoresponse was detected at 0.7 wt% rGO content, demonstrating 2.5 and 1.7 times higher out-of-plane and in-plane values, respectively, than that for pure PHB fibers. The rGO addition led to enhanced zigzag chain formation between paired lamellae in PHB fibers. In contrast, a further increase in rGO content reduced the alpha-crystal size and prevented zigzag chain conformation. A corresponding model explaining structural and molecular changes caused by rGO addition in electrospun PHB fibers is proposed. In addition, finite element analysis revealed a negligible vertical piezoresponse compared to lateral piezoresponse in uniaxially oriented PHB fibers based on alpha-phase (P2(1)2(1)2(1) space group). Thus, the present study demonstrates promising results for the development of biodegradable hybrid 3D scaffolds with an enhanced piezoresponse for various tissue engineering applications.
keywords
PIEZOELECTRIC PROPERTIES; ULTRASOFT PSEUDOPOTENTIALS; CHEMICAL-REDUCTION; RAMAN-SPECTROSCOPY; ELASTIC PROPERTIES; POLY(3-HYDROXYBUTYRATE); CRYSTALLINITY; BIOMATERIALS; DEGRADATION; COMPOSITES
subject category
Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied
authors
Chernozem, RV; Romanyuk, KN; Grubova, I; Chernozem, PV; Surmeneva, MA; Mukhortova, YR; Wilhelm, M; Ludwig, T; Mathur, S; Kholkin, AL; Neyts, E; Parakhonskiy, B; Skirtach, AG; Surmenev, RA
our authors
Andrei Kholkin
Principal Researcher
Konstantin Nikolaevich Romanyuk
Junior ResearcherProjects
CICECO - Aveiro Institute of Materials (UIDB/50011/2020)
CICECO - Aveiro Institute of Materials (UIDP/50011/2020)
Collaboratory for Emerging Technologies, CoLab (EMERGING TECHNOLOGIES)
acknowledgements
This research was performed at Tomsk Polytechnic University within the framework of the Tomsk Polytechnic University Competitiveness Enhancement Program grant. The work was also supported by the Special Research Fund (BOF) of Ghent University [grant numbers BOF16/FJD/029 (RVC and AGS) 01IO3618, BAS094-18 and BOF14/IOP/003 (AGS) ] and Research Foundation Flanders (FWO) , Belgium [G043219 and I002620N (AGS) ] . In addition, this study was supported by the scholarship of the President of the Russia Federation for PhD students training abroad, the Russian President's grant MK-330.2020.8 and Russian Science Foundation (20-63-47096, materials purchase, SEM, XRD studies) . The PFM study was supported by the Ministry of Science and Higher Education (#075-15-2021-588 from 1.06.2021) . This work was carried out within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020 & UIDP/50011/2020, financed by national funds through the Portuguese Foundation for Science and Technology/MCTE, and by national funds (OE) through FCT - Fundacao para a Ciencia e a Tecnologia, I.P., in the scope of the framework contract foreseen in the numbers 4, 5 and 6 of the article 23, of the Decree-Law 57/2016, of August 29, changed by Law 57/2017, of July 19. The computational part of this work was carried out in part using the Turing HPC infrastructure of the CalcUA core facility of the Universiteit Antwerpen (UAntwerp) , a division of the Flemish Super-computer Centre (VSC) , funded by the Hercules Foundation, the Flemish Government (department EWI) and the UAntwerp, Belgium. The sup-port from the Alexander von Humboldt Foundation is acknowledged.