Characterization of synthesized nanomaterials
Figure 2 has been confirmed and demonstrated of surface morphologies and also the determination of particle sizes of (a) Fe3O4 nanospheres (b) Fe3O4@LDH multicore-shell nanostructure and (c) Fe3O4@LDH-ibuprofen. Figure 2a and Fig. 2b obviously display the Monodispersed structure Fe3O4 nanospheres and Fe3O4@LDH multicore-shell nanostructure. The diameter of the Fe3O4 nanospheres is determined 80–130 nm, and the thickness of the LDH nanoflakes shell is about 70–110 nm. Furthermore, as it is shown in Fig. 2c, the Fe3O4@LDH-ibuprofen, for instance, has a similar structure, even after loading of drug into the LDH layer structure.
The TEM was used to prove the core-shell structures and to show the porous and multicore nanoparticles created by the Ostwald ripening method, as well as to calculate their size. With regard to Fig. (3a) Fe3O4@LDH multicore-shell nanostructure and (3b) Fe3O4@LDH-ibuprofen, as the drug-loading nanostructure, the multicore, and core-shell structure are fully visible.
The Fourier transform infrared spectra of (a) Fe3O4 nanospheres (b) Fe3O4@LDH multicore-shell nanostructure (c) Fe3O4@LDH-ibuprofen and (d) Fe3O4@LDH-diclofenac are shown in Fig. 4. The FT-IR spectrum of Fe3O4 Nanospheres(Fig. 4a), two highest peaks linked to metal-oxygen bonds were shown. The first band detected in the range 385–540 cm− 1, is normally apportioned to octahedral–metal stretching, whereas the highest one detected in the range 500–600 cm− 1 is consistent with basic stretching vibrations of the metal at the tetrahedral site. The higher frequency band at 574 cm− 1 and lower frequency band at 448 cm− 1are assigned to the tetrahedral and octahedral, respectively. Additionally, the peak at ~ 3360 cm− 1 is attributed to the stretching vibrations of hydroxyl that is allocated to hydroxyl absorbed by magnetic nanospheres and the existence of water is evidenced by the appearance of the bending mode at 1645 cm− 1 and the stretching mode at 3476 cm− 1. In Fig. 4c and 4d, compared with the spectrum of Fe3O4@LDH multicore-shell nanostructure with Fe3O4@LDH-ibuprofen and Fe3O4@LDH-diclofenac there are particular similar peaks in their spectra. The principal peaks were between 2800 and 3000 cm− 1 due to the alkyl stretching of drugs, especially in ibuprofen due to the existence of many methyl groups in its structure than diclofenac. And also two peaks appeared at approximately 1421 and 1576 cm− 1 that were recognized to the symmetric and asymmetric stretch of the carboxyl group, respectively. The interaction between the metal atom and the carboxylate groups was classified as three types: monodentate, bridging and chelating [16, 17], which the major difference (200–320 cm− 1) was related to the monodentate interaction and the lowest difference (< 110 cm− 1) was for the chelating bidentate. The medium-range difference (140–190 cm− 1) was for the bridging bidentate. In this research, the Δ (1576– 1421 = 155 cm− 1) was ascribed bridging bidentate. Moreover, the peaks at 1440 and 1519 cm− 1 are related to C–C stretching vibration in benzene rings. These outcomes provided subsequent assistance that ibuprofen and diclofenac have been loaded into the layered double hydroxide nanoflakes in the anionic form.
The XRD patterns of the Fe3O4 nanospheres (5a) in the 2θ range of 2–70° is shown in Fig. 5. Besides, with loading the drugs, the regenerated matrix indicates representative diffraction peaks of the LDH-drugs representing two sharp basal reflections that were indexed (003) and (006) reflections agree to the well-crystallized lamellar construction in synthesized nanocarrier with 3R rhombic proportion. The important diffraction peaks of Fe3O4@LDH-ibuprofen (5b) and Fe3O4@LDH-diclofenac (5c) are achieved at 2θ value of 7.6° and 7.8°. The d003 spacing of Fe3O4@LDH-ibuprofen and Fe3O4@LDH-diclofenac were found to be 2.62 nm and 2.22 nm, respectively.
The magnetic properties of magnetic nanospheres (Fig. 6a) and Fe3O4@LDH multicore-shell nanostructure (Fig. 6b) were specify using a vibrating sample magnetometer (VSM). The magnetic saturation values of the magnetic nanospheres and Fe3O4@LDH multicore-shell nanostructure were 59 and 32 emu g− 1, respectively. After the LDH shell packing of Fe3O4 (curve (b)), the saturated magnetization of the Fe3O4@LDH multicore-shell nanostructure decreases because of the shield of the LDH nanoflakes.
In this study, inhibition zones for the two pathogen bacteria including Klebsiella pneumonia PTCC10031T and Bacillus cereus ATCC11778T (Fig. 7) were obsoreved in the presence of the nanoparticles. This results indicated that the nanoparticle can be a good candidate as an antimicrobial particle. Most of nanoparticles and nanostructures with different mechanisms such as destruction of bacterial membranes, inhibition of biofilm formation, or other multiple mechanisms exert their antibacterial properties [18].
MTT assay analysis showed that Fe3O4@LDH multicore-shell nanostructure in 0.001 g concentration had a less negative effect on C2C12 cells as upon 90% of the cells treated viable in comparison to the control group (Fig. 8). Also, we did not observe any valuable difference between 0.001 and 0.005 g concentrations of Fe3O4@LDH on cell viability. However, we observed that in the presence of the high concentration of the nanostructure (0.05 and 0.01 g) the viability of about 20%-30% of cells are decreased.
UV-Vis spectrum of ibuprofen and diclofenac release assay
Drug release is specified as the speed of mass transport from a solid phase into the broth media under normal conditions. The major phase in drug delivery is an interaction between the drug carrier and PBS (pH = 7.4) that happen at the interface of carrier and buffer solution and absorption was measured via UV-Vis Spectrophotometer in specified intervals. According to Fig. 9, Drug release was determined at intervals between 15 min and 72 h in the wavelength of 264 nm for ibuprofen and wavelength of 276 nm for diclofenac. Both Drug releases were gently increasing between 15 min to 6 h interval and concentration of drug was fixed between 6 h to 72 h interval. The release rate of ibuprofen was 90% within 24 hours, 94% in 48 hours and 96% in 72 hours. The values for diclofenac in 24 hours 78%, within 48 hours of 81% in 72 hours and 82%, respectively, indicating the release of less diclofenac than ibuprofen per unit of time. This can be due to lower solubility in water [19], highly lipophilicity [20] of diclofenac as well as small size and more sterile effect of diclofenac compared to ibuprofen [21] that is not able to release easily between layers. Comparing to the old and industrial methods, drug loading between LDH layers lead to the different release rate of drug and enhance the solubility of the drug and also, reduce a side effect of it.