Abstract
Colloidal drug delivery systems are one of the most promising tools for the treatment of several diseases. We present a synthesis route based on four steps involving mesoporous silica-coated magnetite nanoparticles (MNPs) capped by polyelectrolyte (PE) assembling. The morphology and physical properties of the different components of the system were investigated. The magnetite phase of the iron oxide nanoparticles was identified by X-ray diffraction before their incorporation into the mesoporous silica matrix by a sol–gel process. A MCM-41-like organized hexagonal mesoporous (≈4.2 nm) structure was achieved, as ensured by the αS-plot model. Polyethylenimine PEI and sodium alginate (ALG) PE layer-by-layer capping were successfully performed by simple successive dispersions of nanoparticles in the PE solution bath. TEM images confirmed a well-organized structure, as also supported by DLS and XPS analyses, which present an increase in diameter size and distinct chemical surface composition after each step of the synthesis. The two successive coatings of the MNPs induced a significative decrease of the magnetic susceptibility but kept sufficient intensity for drug delivery assisted by an external magnetic field. To validate the system as drug delivery, in vitro tetracycline hydrochloride (TCH) loading and release studies were performed in PBS solution for 48 h. It was found that the TCH-loaded uncapped mesoporous silica NPs released more than 90% of TCH after 48 h. Meanwhile, when capped by the PEs, only 30% of the total drug amount was released, due to a hindrance of the drug diffusion by the PE layer. The present work suggests that the combination of the low cost and non-toxic hybrid system proposed has potential use in nanomedicine as a drug delivery vehicle.
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References
Ahmad A, Bae H, Rhee I (2018) Highly stable silica-coated manganese ferrite nanoparticles as high-efficacy T2 contrast agents for magnetic resonance imaging. AIP Adv 10(1063/1):5027898
Ahmadi A, Sedaghat T, Azadi R, Motamedi H (2020) Magnetic mesoporous silica nanocomposite functionalized with palladium schiff base complex: synthesis, characterization, catalytic efficacy in the Suzuki–Miyaura reaction and α-amylase immobilization. Catal Lett. https://doi.org/10.1007/s10562-019-02913-5
Alahmadi NS, Betts JW, Cheng F et al (2017) Synthesis and antibacterial effects of cobalt-cellulose magnetic nanocomposites. RSC Adv. https://doi.org/10.1039/C7RA00920H
Andrade GF, Faria JAQA, Gomes DA et al (2018) Mesoporous silica SBA-16/hydroxyapatite-based composite for ciprofloxacin delivery to bacterial bone infection. J Sol Gel Sci Technol. https://doi.org/10.1007/s10971-017-4557-y
Anirudhan TS, Vasantha CS, Sasidharan AV (2017) Layer-by-layer assembly of hyaluronic acid/carboxymethylchitosan polyelectrolytes on the surface of aminated mesoporous silica for the oral delivery of 5-fluorouracil. Eur Polym J. https://doi.org/10.1016/j.eurpolymj.2017.06.033
Askari P, Zahedi P, Rezaeian I (2016) Three-layered electrospun PVA/PCL/PVA nanofibrous mats containing tetracycline hydrochloride and phenytoin sodium: a case study on sustained control release, antibacterial, and cell culture properties. J Appl Polym Sci. https://doi.org/10.1002/app.43309
Bharti C, Gulati N, Nagaich U, Pal A (2015) Mesoporous silica nanoparticles in target drug delivery system: a review. Int J Pharm Investig. https://doi.org/10.4103/2230-973x.160844
Bish DL, Howard SA (1988) Quantitative phase analysis using the Rietveld method. J Appl Crystallogr 21:86–91. https://doi.org/10.1107/S0021889887009415
Brigante M, Pecini E, Avena M (2016) Magnetic mesoporous silica for water remediation: synthesis, characterization and application as adsorbent of molecules and ions of environmental concern. Microporous Mesoporous Mater. https://doi.org/10.1016/j.micromeso.2016.04.032
Castle JE, Baker MA (1999) The feasibility of an XPS expert system demonstrated by a rule set for carbon contamination. J Electron Spectros Relat Phenomena 105:245–256. https://doi.org/10.1016/S0368-2048(99)00065-1
Chen H, Wang Y (2002) Preparation of MCM-41 with high thermal stability and complementary textural porosity. Ceram Int. https://doi.org/10.1016/S0272-8842(02)00007-X
Chen X, Sun H, Hu J et al (2017a) Transferrin gated mesoporous silica nanoparticles for redox-responsive and targeted drug delivery. Colloids Surf B Biointerfaces. https://doi.org/10.1016/j.colsurfb.2017.01.010
Chen Z, Du Y, Li Z et al (2017b) Controllable synthesis of magnetic Fe3O3 particles with different morphology by one-step hydrothermal route. J Magn Magn Mater. https://doi.org/10.1016/j.jmmm.2016.11.
Coelho AA, Evans J, Evans I et al (2011) The TOPAS symbolic computation system. Powder Diffr 26:S22–S25. https://doi.org/10.1154/1.3661087
Dhal JP, Dash T, Hota G (2019) Iron oxide impregnated mesoporous MCM-41: synthesis, characterization and adsorption studies. J Porous Mater. https://doi.org/10.1007/s10934-019-00803-0
Dunn AW, Zhang Y, Mast D et al (2016) In-vitro depth-dependent hyperthermia of human mammary gland adenocarcinoma. Mater Sci Eng C. https://doi.org/10.1016/j.msec.2016.06.026
Feng W, Nie W, He C et al (2014) Effect of pH-responsive alginate/chitosan multilayers coating on delivery efficiency, cellular uptake and biodistribution of mesoporous silica nanoparticles based nanocarriers. ACS Appl Mater Interfaces. https://doi.org/10.1021/am501337s
Fleet ME (1981) The structure of magnetite. Acta Crystallogr Sect B Struct Crystallogr Cryst Chem 37:917–920. https://doi.org/10.1107/S0567740881004597
Ghaznavi H, Hosseini-Nami S, Kamrava SK et al (2018) Folic acid conjugated PEG coated gold–iron oxide core–shell nanocomplex as a potential agent for targeted photothermal therapy of cancer. Artif Cells Nanomed Biotechnol. https://doi.org/10.1080/21691401.2017.1384384
Gounani Z, Asadollahi MA, Pedersen JN et al (2019) Mesoporous silica nanoparticles carrying multiple antibiotics provide enhanced synergistic effect and improved biocompatibility. Colloids Surf B Biointerfaces. https://doi.org/10.1016/j.colsurfb.2018.12.035
Greaves C (1983) A powder neutron diffraction investigation of vacancy ordering and covalence in γ-Fe2O3. J Solid State Chem 49:325–333. https://doi.org/10.1016/S0022-4596(83)80010-3
Gupta A, Saleh NM, Das R, et al (2017) Synergistic antimicrobial therapy using nanoparticles and antibiotics for the treatment of multidrug-resistant bacterial infection. Nano Futur. https://doi.org/10.1088/2399-1984/aa69fb
Gür E, Altinisik A, Yurdakoc K (2017) Preparation and characterization of chitosan/sepiolite bionanocomposites for tetracycline release. Polym Compos. https://doi.org/10.1002/pc.23751
Hamzehloo M, Karimi J, Aghapoor K et al (2018) The synergistic cooperation between MCM-41 and azithromycin: a pH responsive system for drug adsorption and release. J Porous Mater. https://doi.org/10.1007/s10934-017-0538-3
Hegazy M, Zhou P, Wu G et al (2017) Construction of polymer coated core-shell magnetic mesoporous silica nanoparticles with triple responsive drug delivery. Polym Chem. https://doi.org/10.1039/c7py01179b
Higuchi T (1963) Mechanism of sustained-action medication. Theoretical analysis of rate of release of solid drugs dispersed in solid matrices. J Pharm Sci. https://doi.org/10.1002/jps.2600521210
Hu Y, Dong X, Ke L et al (2017) Polysaccharides/mesoporous silica nanoparticles hybrid composite hydrogel beads for sustained drug delivery. J Mater Sci. https://doi.org/10.1007/s10853-016-0597-x
Jadhav SV, Kim BM, Lee HY et al (2018) Induction heating and in vitro cytotoxicity studies of MnZnFe2O4 nanoparticles for self-controlled magnetic particle hyperthermia. J Alloys Compd. https://doi.org/10.1016/j.jallcom.2018.02.174
Ji Y, Li W, Fu W et al (2019) Development of boronic acid-functionalized mesoporous silica-coated core/shell magnetic microspheres with large pores for endotoxin removal. J Chromatogr A. https://doi.org/10.1016/j.chroma.2019.06.004
Koneru B, Shi Y, Wang YC et al (2015) Tetracycline-containing MCM-41 mesoporous silica nanoparticles for the treatment of Escherichia coli. Molecules. https://doi.org/10.3390/molecules201119650
Le Ouay B, Stellacci F (2015) Antibacterial activity of silver nanoparticles: a surface science insight. Nano Today 10(3):339–354 https://doi.org/10.1016/j.nantod.2015.04.002
Li J, Li Q, Ma X et al (2016) Biosynthesis of gold nanoparticles by the extreme bacterium Deinococcus radiodurans and an evaluation of their antibacterial properties. Int J Nanomed. https://doi.org/10.2147/IJN.S119618
Liu G, Ma J, Li Y et al (2017) Core-interlayer-shell Fe3O4@mSiO2@lipid-PEG-methotrexate nanoparticle for multimodal imaging and multistage targeted chemo-photodynamic therapy. Int J Pharm. https://doi.org/10.1016/j.ijpharm.2017.01.068
Lowman AM (2004) Biomaterials in drug delivery. In: Shi D (ed) Biomedical devices and their applications. Springer, Berlin, pp 1–31
Męczyńska-Wielgosz S, Piotrowska A, Majkowska-Pilip A et al (2016) Effect of surface functionalization on the cellular uptake and toxicity of nanozeolite A. Nanoscale Res Lett. https://doi.org/10.1186/s11671-016-1334-8
Mohseni M, Gilani K, Mortazavi SA (2015) Preparation and characterization of rifampin loaded mesoporous silica nanoparticles as a potential system for pulmonary drug delivery. Iran J Pharm Res. https://doi.org/10.22037/ijpr.2015.1616
Moreira AF, Dias DR, Correia IJ (2016) Stimuli-responsive mesoporous silica nanoparticles for cancer therapy: A review. Microporous Mesoporous Mater. 236:141–157
Ortiz-Bustos J, Martín A, Morales V et al (2017) Surface-functionalization of mesoporous SBA-15 silica materials for controlled release of methylprednisolone sodium hemisuccinate: influence of functionality type and strategies of incorporation. Microporous Mesoporous Mater. https://doi.org/10.1016/j.micromeso.2016.11.021
Palo E, Salomäki M, Lastusaari M (2017) Surface modification of upconverting nanoparticles by layer-by-layer assembled polyelectrolytes and metal ions. J Colloid Interface Sci. https://doi.org/10.1016/j.jcis.2017.08.038
Pourjavadi A, Tehrani ZM (2016) Mesoporous silica nanoparticles with bilayer coating of poly(acrylic acid-co-itaconic acid) and human serum albumin (HSA): a pH-sensitive carrier for gemcitabine delivery. Mater Sci Eng C 61:782–790. https://doi.org/10.1016/j.msec.2015.12.096
Rietveld HM (1967) Line profiles of neutron powder-diffraction peaks for structure refinement. Acta Crystallogr 22:151–152. https://doi.org/10.1107/S0365110X67000234
Rietveld HM (1969) A profile refinement method for nuclear and magnetic structures. J Appl Crystallogr 2:65–71. https://doi.org/10.1107/S0021889869006558
Rotello VM, Gupta A, Landis RF (2016) Nanoparticle-based antimicrobials: surface functionality is critical. F1000Research. https://doi.org/10.12688/f1000research.7595.1
Schmaljohann D (2006) Thermo- and pH-responsive polymers in drug delivery. Adv Drug Deliv Rev 58:1655–1670
Seabra AB, Durán N (2015) Nanotoxicology of metal oxide nanoparticles. Metals (Basel) 5(2):934–975
Shankar S, Rhim JW (2019) Effect of Zn salts and hydrolyzing agents on the morphology and antibacterial activity of zinc oxide nanoparticles. Environ Chem Lett. https://doi.org/10.1007/s10311-018-00835-z
Sing KSW (1982) Reporting physisorption data for gas/solid systems. Pure Appl Chem. https://doi.org/10.1351/pac198254112201
Talavera-Pech WA, Esparza-Ruiz A, Quintana-Owen P et al (2018) Synthesis of pH-sensitive poly($β$-amino ester)-coated mesoporous silica nanoparticles for the controlled release of drugs. Appl Nanosci 8:853–866. https://doi.org/10.1007/s13204-018-0716-x
Thommes M (2010) Physical adsorption characterization of nanoporous materials. Chem Ing Tech. https://doi.org/10.1002/cite.201000064
Wang S, Zhao X, Qian J, He S (2016) Polyelectrolyte coated BaTiO3 nanoparticles for second harmonic generation imaging-guided photodynamic therapy with improved stability and enhanced cellular uptake. RSC Adv. https://doi.org/10.1039/c6ra05289d
Wani A, Muthuswamy E, Savithra GHL et al (2012) Surface functionalization of mesoporous silica nanoparticles controls loading and release behavior of mitoxantrone. Pharm Res. https://doi.org/10.1007/s11095-012-0766-9
Xiong L, Bi J, Tang Y, Qiao SZ (2016) Magnetic core-shell silica nanoparticles with large radial mesopores for siRNA delivery. Small. https://doi.org/10.1002/smll.201600531
Yao X, Niu X, Ma K et al (2017) Graphene quantum dots-capped magnetic mesoporous silica nanoparticles as a multifunctional platform for controlled drug delivery, magnetic hyperthermia, and photothermal therapy. Small. https://doi.org/10.1002/smll.201602225
Zhao W, Shi JL, Chen H, Zhang L (2006) Particle size, uniformity, and mesostructure control of magnetic core/mesoporous silica shell nanocomposite spheres. J Mater Res. https://doi.org/10.1557/jmr.2006.0381
Zhao K, Wu C, Deng Z et al (2015) Preparation of silver decorated silica nanocomposite rods for catalytic and surface-enhanced Raman scattering applications. RSC Adv 5:52726–52736. https://doi.org/10.1039/C5RA08076B
Acknowledgements
This project was financially supported by FAPESP (Proc. no. 2014/50983-3). The authors also thank the financial support provided by CNPq (proc. nos. 305601/2019-9 and 428333/2018-4) and the Multiuser Experimental Center (CEM-UFABC) for access to its facilities.
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Alavarse, A.C., de Castro, C.E., dos Santos Andrade, L. et al. Synthesis of nanostructured mesoporous silica-coated magnetic nuclei with polyelectrolyte layers for tetracycline hydrochloride control release. Appl Nanosci 10, 3693–3702 (2020). https://doi.org/10.1007/s13204-020-01482-z
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DOI: https://doi.org/10.1007/s13204-020-01482-z