This preliminary study explores the development of a 3D printed PVDF-PLA70:30 piezoelectric scaffold to support bone tissue regeneration. By utilizing the piezoelectric properties of PVDF, the scaffold creates an electrical microenvironment conducive to bone repair. The incorporation of BaTiO3 nanoparticles enhanced the nucleation of the ß-phase in PVDF, a critical factor in improving its piezoelectric performance. To ensure better dispersion of these nanoparticles, a polydopamine coating was applied. In addition, PEG-coated magnesium peroxide (PEG-MPO) was incorporated into the scaffold to provide sustained release of oxygen, addressing the challenge of cell survival under low-oxygen conditions. Key analytical techniques, including Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD), confirmed an increase in ß-phase with nanoparticle incorporation up to 0.5% w/w. Furthermore, oxygen release from the scaffold followed a continuous profile over 14 days, with 1% w/w PEG-MPO contributing to this effect. Cell assays demonstrated improved cell adhesion and growth due to the enhanced electrical cues provided by ultrasound stimulation and confirmed cell survival even in hypoxic environments. In conclusion, this innovative oxygen-releasing piezoelectric scaffold has significant potential to advance bone repair using 3D printing technology.
TajvarSHadjizadehASamandariSS. Scaffold degradation in bone tissue engineering: an overview. Int Biodeterior Biodegrad2023; 180: 105599.
2.
LinXPatilSGaoYG, et al.The bone extracellular matrix in bone formation and regeneration. Front Pharmacol2020; 11: 757–835.
3.
WongSKYeeMMFChinKY, et al.A review of the application of natural and synthetic scaffolds in bone regeneration. J Funct Biomater2023; 14(5): 286.
4.
El-FiqiA. Three-dimensional printing of biomaterials for bone tissue engineering: a review. Front Mater Sci2023; 17(2): 230644.
5.
ZhangXWangTZhangZ, et al.Electrical stimulation system based on electroactive biomaterials for bone tissue engineering. Mater Today2023; 68: 177–203.
6.
SharmaTNaikSGopalA, et al.Emerging trends in bioenergy harvesters for chronic powered implants. MRS Energy Sustain2015; 2(1): 7.
7.
SilvaCAFernandesMMRibeiroC, et al.Two- and three-dimensional piezoelectric scaffolds for bone tissue engineering. Colloids Surf B Biointerfaces2022; 218(12): 112708–112725.
8.
MacielMMRibeiroSRibeiroC, et al.Relation between fiber orientation and mechanical properties of nano-engineered poly(vinylidene fluoride) electrospun composite fiber mats. Composites Part B2018; 139: 146–154.
9.
TaibNAABRahmanMRHudaD, et al.A review on poly lactic acid (PLA) as a biodegradable polymer. Polym Bull2023; 80(2): 1179–1213.
10.
AgarwalTKazemiSCostantiniM, et al.Oxygen releasing materials: towards addressing the hypoxia-related issues in tissue engineering. Mater Sci Eng C2021; 122: 111896.
11.
WangZChenTLiX, et al.Oxygen-releasing biomaterials for regenerative medicine. J Mater Chem B2023; 11(31): 7300–7320.
12.
Seyyed NasrollahSAKarimi-SoflouRKarkhanehA. PEG-coated magnesium peroxide nanosheets with tunable microstructure: effect of microstructure on concurrent oxygen and magnesium ion release. Mater Lett2021; 291(56): 129550–129578.
13.
AnPZuoFWuYP, et al.Fast synthesis of dopamine-coated Fe 3O 4 nanoparticles through ligand-exchange method. Chin Chem Lett2012; 23(9): 1099–1102.
14.
SuYLiWYuanL, et al.Piezoelectric fiber composites with polydopamine interfacial layer for self-powered wearable biomonitoring. Nano Energy2021; 89: 106321.
15.
MishraSSahooRUnnikrishnanL, et al.Enhanced structural and dielectric behaviour of PVDF-PLA binary polymeric blend system. Mater Today Commun2021; 26: 101958.
16.
BouadVOhnoKAddadA, et al.Surface-initiated reversible addition fragmentation chain transfer of fluoromonomers: an efficient tool to improve interfacial adhesion in piezoelectric composites. Polym Chem2022; 13(42): 6061–6072.
17.
de OliveiraPCMarangoniRFreitasVF, et al.Fused filaments of PVDF/PLA blends for biomedical applications. Ferroelectrics2023; 611(1): 60–66.
18.
Shabani SamghabadiMKarkhanehAKatbabAA. Synthesis and characterization of biphasic layered structure composite with simultaneous electroconductive and piezoelectric behavior as a scaffold for bone tissue engineering. Polym Adv Technol2023; 34: 1367–1380.
19.
SalehiyanRRaySSOjijoV. Processing-Driven morphology development and crystallization behavior of immiscible Polylactide/Poly(Vinylidene fluoride) blends. Macromol Mater Eng2018; 303: 1800349.
20.
XieQKeKJiangW, et al.Role of poly(lactic acid) in the phase transition of poly(vinylidene fluoride) under uniaxial stretching. J Appl Polym Sci2013; 129: 1686–1696.
21.
HosseiniSZarei-HanzakiAAbediHR, et al.Effect of crystallization process on the electrical, and piezoelectric properties of PLA scaffolds. J Mater Res Technol2023; 27: 3815–3824.
22.
WangBHuangHX. Incorporation of halloysite nanotubes into PVDF matrix: nucleation of electroactive phase accompany with significant reinforcement and dimensional stability improvement. Compos Part A Appl Sci Manuf2014; 66: 16–24.
23.
ChenJLiSJiaoY, et al.In vitro study on the piezodynamic therapy with a BaTiO3-Coating titanium scaffold under low-intensity pulsed ultrasound stimulation. ACS Appl Mater Interfaces2021; 13(41): 49542–49555.
24.
ShuaiCLiuGYangY, et al.Functionalized BaTiO3 enhances piezoelectric effect towards cell response of bone scaffold. Colloids Surf B Biointerfaces2020; 185(12): 110587.
25.
KimHJohnsonJChavezLA, et al.Enhanced dielectric properties of three phase dielectric MWCNTs/BaTiO3/PVDF nanocomposites for energy storage using fused deposition modeling 3D printing. Ceram Int2018; 44(8): 9037–9044.
26.
LiCCChangSJLeeJT, et al.Efficient hydroxylation of BaTiO3 nanoparticles by using hydrogen peroxide. Colloids Surfaces A Physicochem Eng Asp2010; 361(1–3): 143–149.
27.
HuJLiuYZhangS, et al.Novel designed core–shell nanofibers constituted by single element-doped BaTiO3 for high-energy–density polymer nanocomposites. Chem Eng J2022; 428: 131046.
28.
ChenXChaoXYangZ. Submicron barium calcium zirconium titanate ceramic for energy storage synthesised via the co-precipitation method. Mater Res Bull2019; 111: 259–266.
29.
LiPHeZLuoC, et al.α-Fe 2 O 3 @dopamine core-shell nanocomposites and their highly enhanced photoacoustic performance. Appl Surf Sci2019; 466: 185–192.
30.
XieYYuYFengY, et al.Fabrication of stretchable nanocomposites with high energy density and low loss from cross-linked PVDF filled with poly(dopamine) encapsulated BaTiO3. ACS Appl Mater Interfaces2017; 9(3): 2995–3005.
31.
MalekiMKarimi-SoflouRKarkhanehA. Raspberry-like PLA/PGS biodegradable microparticles with urethane linkages: unlocking tailored release of magnesium ions and oxygen for bone tissue engineering. Int J Pharm2024; 651: 123760.
32.
AliMFarooqULyuS, et al.Synthesis of controlled release calcium peroxide nanoparticles (CR-nCPs): characterizations, H2O2 liberate performances and pollutant degradation efficiency. Sep Purif Technol2020; 241: 116729.
33.
ZhangXZhangCLinY, et al.Nanocomposite membranes enhance bone regeneration through restoring physiological electric microenvironment. ACS Nano2016; 10(8): 7279–7286.
34.
WuLJinZLiuY, et al.Recent advances in the preparation of PVDF-Based piezoelectric materials. Nanotechnol Rev2022; 11(1): 1386–1407.
35.
ChernozemRVSurmenevaMASurmenevRA. Hybrid biodegradable scaffolds of piezoelectric polyhydroxybutyrate and conductive polyaniline: piezocharge constants and electric potential study. Mater Lett2018; 220(11): 257–260.
36.
KarEBoseNDasS, et al.Enhancement of electroactive β phase crystallization and dielectric constant of PVDF by incorporating GeO2 and SiO2 nanoparticles. Phys Chem Chem Phys2015; 17(35): 22784–22798.
37.
MartinsPLopesACLanceros-MendezS. Electroactive phases of poly(vinylidene fluoride): determination, processing and applications. Prog Polym Sci2014; 39(4): 683–706.
38.
SurmenevRAOrlovaTChernozemRV, et al.Hybrid lead-free polymer-based nanocomposites with improved piezoelectric response for biomedical energy-harvesting applications: a review. Nano Energy2019; 62: 475–506.
39.
YuanXYanALaiZ, et al.A poling-free PVDF nanocomposite via mechanically directional stress field for self-powered pressure sensor application. Nano Energy2022; 98: 107340.
40.
BarrulasRVCorvoMC. Rheology in product development: an insight into 3D printing of hydrogels and aerogels. Gels2023; 9(12): 986.
41.
MayeenAM SKJayalakshmyMS, et al.Dopamine functionalization of BaTiO3: an effective strategy for the enhancement of electrical, magnetoelectric and thermal properties of BaTiO3-PVDF-TrFE nanocomposites. Dalton Trans2018; 47(6): 2039–2051.
42.
FadzilAFAPramanikABasakAK, et al.Role of surface quality on biocompatibility of implants - a review. Annals of 3D Printed Medicine2022; 8: 100082.
43.
YangYHeCDianyu E, et al.Mg bone implant: features, developments and perspectives. Mater Des2020; 185: 108259.
44.
SuJZhangJ. Comparison of rheological, mechanical, electrical properties of HDPE filled with BaTiO 3 with different polar surface tension. Appl Surf Sci2016; 388: 531–538.
45.
CuiJZhouZXieA, et al.Bio-inspired fabrication of superhydrophilic nanocomposite membrane based on surface modification of SiO2 anchored by polydopamine towards effective oil-water emulsions separation. Sep Purif Technol2019; 209(12): 434–442.
46.
WillemenNGAHassanSGurianM, et al.Enzyme-mediated alleviation of peroxide toxicity in self-oxygenating biomaterials. Adv Healthcare Mater2022; 11(13): e2102697.
47.
MilenkovicSSlavkovicVFragassaC, et al.Effect of the raster orientation on strength of the continuous fiber reinforced PVDF/PLA composites, fabricated by hand-layup and fused deposition modeling. Compos Struct2021; 270: 114063.
48.
AliFKalvaSNKoçM. Additive manufacturing of Polymer/mg-based composites for porous tissue scaffolds. Polymers2022; 14(24): 5460.
49.
AroraGSSaxenaKKMohammedKA, et al.Manufacturing techniques for Mg-Based metal matrix composite with different reinforcements. Crystals2022; 12(7): 945.
