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. 2020 Dec 13;12(12):1208.
doi: 10.3390/pharmaceutics12121208.

Carbon Nano-Onions Reinforced Multilayered Thin Film System for Stimuli-Responsive Drug Release

Narsimha Mamidi  1 , Ramiro Manuel Velasco Delgadillo  1 , Aldo Gonzáles Ortiz  1 , Enrique V Barrera  2
Affiliations

Carbon Nano-Onions Reinforced Multilayered Thin Film System for Stimuli-Responsive Drug Release

Narsimha Mamidi et al. Pharmaceutics. .

Abstract

Herein, poly (N-(4-aminophenyl) methacrylamide))-carbon nano-onions (PAPMA-CNOs = f-CNOs) and anilinated-poly (ether ether ketone) (AN-PEEK) have synthesized, and AN-PEEK/f-CNOs composite thin films were primed via layer-by-layer (LbL) self-assembly for stimuli-responsive drug release. The obtained thin films exhibited pH-responsive drug release in a controlled manner; pH 4.5 = 99.2% and pH 6.5 = 59.3% of doxorubicin (DOX) release was observed over 15 days. Supramolecular π-π stacking interactions between f-CNOs and DOX played a critical role in controlling drug release from thin films. Cell viability was studied with human osteoblast cells and augmented viability was perceived. Moreover, the thin films presented 891.4 ± 8.2 MPa of the tensile strength (σult), 43.2 ± 1.1 GPa of Young's modulus (E), and 164.5 ± 1.7 Jg-1 of toughness (K). Quantitative scrutiny revealed that the well-ordered aligned nanofibers provide critical interphase, and this could be responsible for augmented tensile properties. Nonetheless, a pH-responsive and mechanically robust biocompatible thin-film system may show potential applications in the biomedical field.

Keywords: Young’s modulus; cell viability; layer-by-layer assembly; nanocomposite thin films; pH-responsive drug release; strength; toughness.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Scheme 1
Scheme 1
(A) Synthetic route of PAPMA-CNOs (f-CNOs) from p-phenylenediamine. (B) Synthetic route of anilinated-poly (ether ether ketone) (AN-PEEK) from PEEK and aniline (AN). (i) AN, CH2Cl2/CF3COOH, BF3.Et2O, 48 h, (ii) NaBH3CN, DMSO, 130 °C, 24 h.
Figure 1
Figure 1
(a) UV-vis spectra of AN-PEEK/f-CNOs LbL films as a function of the number of layers. (b) Absorbance at 340 nm as a function of the number of layers and thickness of AN-PEEK/f-CNOs thin films measured by profilometry. (c) Cross-sectional, and (d,e) side-view of the SEM images of AN-PEEK/f-CNOs nanocomposite thin film with 5 wt% of f-CNOs.
Figure 2
Figure 2
(a) FTIR of AN-PEEK and AN-PEEK/f-CNOs composite films. (b) Molecular structure of AN-PEEK/f-CNOs complex presenting the possible π–π-stacking between AN-PEEK, and f-CNOs and hydrogen bonding interactions between AN-PEEK, and PAPMA moiety. (c) Raman, and (d) TGA curves of AN-PEEK and AN-PEEK/f-CNOs nanocomposite films. The percentage fractions in the plots denotes wt% of the f-CNOs content in the AN-PEEK.
Figure 3
Figure 3
Quantitative mechanical characterization of AN-PEEK/f-CNOs composite films. (a) Stress–strain, (b) ultimate strength-Young’s modulus, (c) toughness-strain curves for nanocomposite thin films obtained from uniaxial tensile. (d) SEM images of fracture surfaces of AN-PEEK/f-CNOs with 5 wt% of f-CNOs, prepared from tearing tests on notched samples. The weight fraction in the x-axis (b) and the percentage in plots (a,c) represent the wt% of f-CNOs content in the AN-PEEK.
Figure 4
Figure 4
Drug release results of DOX-loaded AN-PEEK and AN-PEEK/f-CNOs thin films: (a) pH 4.5, (b) pH 6.5, and (c) pH 7.4 at 37 °C in DMEM solution. (d) Cell viability of thin films.
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