Nanocarriers of Eu<sup>3+</sup> doped silica nanoparticles modified by APTES for luminescent monitoring of cloxacillin

João Otávio Donizette Malafatti; Thamara Machado de Oliveira Ruellas; Mariana Rodrigues Meirelles; Adriana Coatrini Thomazi; Carmen Greice Renda; Elaine Cristina Paris; João Otávio Donizette Malafatti; Thamara Machado de Oliveira Ruellas; Mariana Rodrigues Meirelles; Adriana Coatrini Thomazi; Carmen Greice Renda; Elaine Cristina Paris

doi:10.3934/matersci.2021046

AIMS Materials Science

2021, Volume 8, Issue 5: 760-775. doi: 10.3934/matersci.2021046

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Nanocarriers of Eu³⁺ doped silica nanoparticles modified by APTES for luminescent monitoring of cloxacillin

João Otávio Donizette Malafatti ^1,2,
Thamara Machado de Oliveira Ruellas ^1,2,
Mariana Rodrigues Meirelles ^2,4,
Adriana Coatrini Thomazi ²,
Carmen Greice Renda ³,
Elaine Cristina Paris ^{2
,
,}

1.
Federal University of São Carlos, Chemistry Department, Rod. Washington Luís, Km 235-C. P.676, zip code: 13.565-905, São Carlos-SP, Brazil
2.
Nanotechnology National Laboratory for Agriculture (LNNA), Embrapa Instrumentação, XV de Novembro St., 1452, zip code: 13560-970, São Carlos, SP, Brazil
3.
Federal University of São Carlos, Department of Materials Engineering, Rod. Washington Luís, Km 235-C. P.676, zip code: 13.565-905, São Carlos-SP, Brazil
4.
Institute of Chemistry, University of São Paulo, Av. Trab. São Carlense, 400, zip code: 13566-590, São Carlos-SP, Brazil

Received: 14 May 2021 Accepted: 08 October 2021 Published: 14 October 2021

Drug nanocarriers have been continuously improved to promote satisfactory release control. In this sense, luminescent materials have become an alternative option in clinical trials due to their ability to monitor drug delivery. Among the nanocarriers, silica stands out for structural stability, dispersibility, and surface reactivity. When using ceramic nanocarriers, one of the challenges is their interaction and selectivity capability for organic molecules, such as drugs. In order to overcome such adversity, superficial modifications can be carried out to enable a higher affinity for the desired drug. Thus, the present study aimed to obtain silica nanoparticles (NPs) doped with low concentrations of europium (III) superficially modified by (3-aminopropyl)triethoxysilane (APTES) to assess their interaction with the model drug cloxacillin benzathine. This drug was chosen because it is part of the ampicillin family and is commonly used in several treatments. Near-spherical and homogeneous silica NPs were obtained via sol-gel synthesis, with particle sizes of approximately 21 nm. It was possible to verify the fluorescence capacity of the silica NPs when doped with europium (III) in a mole percent that varied from 0.5 to 3.0%. A 10% volume percent of APTES caused the silica nanoparticles to increase the degree of hydrophobicity, with a shift in the contact angle from 8° to 51°. After surface modification by APTES, the silica nanocarrier (10 g·L^-1) achieved a satisfactory degree of CLOX incorporation (25 g·L^-1), increasing the adsorptive capacity to values above 50%. Therefore, silica NPs doped with europium (III) in a low percent of 0.5% (mole) modified by APTES showed promising results as an alternative option for trials and clinical studies of drug incorporation.
- silica,
- nanoparticles,
- europium,
- surface modification,
- nanocarriers
Citation: João Otávio Donizette Malafatti, Thamara Machado de Oliveira Ruellas, Mariana Rodrigues Meirelles, Adriana Coatrini Thomazi, Carmen Greice Renda, Elaine Cristina Paris. Nanocarriers of Eu3+ doped silica nanoparticles modified by APTES for luminescent monitoring of cloxacillin[J]. AIMS Materials Science, 2021, 8(5): 760-775. doi: 10.3934/matersci.2021046

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Abstract

Drug nanocarriers have been continuously improved to promote satisfactory release control. In this sense, luminescent materials have become an alternative option in clinical trials due to their ability to monitor drug delivery. Among the nanocarriers, silica stands out for structural stability, dispersibility, and surface reactivity. When using ceramic nanocarriers, one of the challenges is their interaction and selectivity capability for organic molecules, such as drugs. In order to overcome such adversity, superficial modifications can be carried out to enable a higher affinity for the desired drug. Thus, the present study aimed to obtain silica nanoparticles (NPs) doped with low concentrations of europium (III) superficially modified by (3-aminopropyl)triethoxysilane (APTES) to assess their interaction with the model drug cloxacillin benzathine. This drug was chosen because it is part of the ampicillin family and is commonly used in several treatments. Near-spherical and homogeneous silica NPs were obtained via sol-gel synthesis, with particle sizes of approximately 21 nm. It was possible to verify the fluorescence capacity of the silica NPs when doped with europium (III) in a mole percent that varied from 0.5 to 3.0%. A 10% volume percent of APTES caused the silica nanoparticles to increase the degree of hydrophobicity, with a shift in the contact angle from 8° to 51°. After surface modification by APTES, the silica nanocarrier (10 g·L^-1) achieved a satisfactory degree of CLOX incorporation (25 g·L^-1), increasing the adsorptive capacity to values above 50%. Therefore, silica NPs doped with europium (III) in a low percent of 0.5% (mole) modified by APTES showed promising results as an alternative option for trials and clinical studies of drug incorporation.

References

[1]	McNamara K, Tofail SAM (2017) Nanoparticles in biomedical applications. Adv Phys X 2: 54-88.
[2]	Becaro AA, Puti FC, Correa DS, et al. (2014) Polyethylene films containing silver nanoparticles for applications in food packaging: Characterization of physico-chemical and anti-microbial properties. J Nanosci Nanotechnol 15: 2148-2156. doi: 10.1166/jnn.2015.9721
[3]	Malafatti JOD, Bernardo MP, Moreira FKV, et al. (2020) Electrospun poly(lactic acid) nanofibers loaded with silver sulfadiazine/[Mg-Al]-layered double hydroxide as an antimicrobial wound dressing. Polym Adv Technol 31: 1377-1387.
[4]	Florek J, Caillard R, Kleitz F (2017) Evaluation of mesoporous silica nanoparticles for oral drug delivery-current status and perspective of MSNs drug carriers. Nanoscale 9: 15252-15277. doi: 10.1039/C7NR05762H
[5]	Li Z, Zhang Y, Feng N (2019) Mesoporous silica nanoparticles: synthesis, classification, drug loading, pharmacokinetics, biocompatibility, and application in drug delivery. Expert Opin Drug Del 16: 219-237. doi: 10.1080/17425247.2019.1575806
[6]	Gómez-Vallejo V, Puigivila M, Plaza-García S, et al. (2018) PEG-copolymer-coated iron oxide nanoparticles that avoid the reticuloendothelial system and act as kidney MRI contrast agents. Nanoscale 10: 14153-14164. doi: 10.1039/C8NR03084G
[7]	Shin K, Choi JW, Ko G, et al. (2017) Multifunctional nanoparticles as a tissue adhesive and an injectable marker for image-guided procedures. Nat Commun 8: 1-12. doi: 10.1038/s41467-016-0009-6
[8]	Touloumes GJ, Ardoña HAM, Casalino EK, et al. (2020) Mapping 2D- and 3D-distributions of metal/metal oxide nanoparticles within cleared human ex vivo skin tissues. NanoImpact 17: 100208. doi: 10.1016/j.impact.2020.100208
[9]	Liao H, Jiang C, Liu W, et al. (2015) Fluorescent nanoparticles from several commercial beverages: Their properties and potential application for bioimaging. J Agr Food Chem 63: 8527-8533. doi: 10.1021/acs.jafc.5b04216
[10]	Liu C, Hou Y, Gao M (2014) Are rare-earth nanoparticles suitable for in vivo applications? Adv Mater 26: 6922-6932.
[11]	Yang B, Chen H, Zheng Z, et al. (2020) Application of upconversion rare earth fluorescent nanoparticles in biomedical drug delivery system. J Lumin 223: 117226. doi: 10.1016/j.jlumin.2020.117226
[12]	Lima RC, Espinosa JWM, Gurgel MFC, et al. (2006) Photoluminescence in disordered Sm-doped PbTiO₃: Experimental and theoretical approach. J Appl Phys 100: 034917. doi: 10.1063/1.2230122
[13]	Lima RC, Paris EC, Leite ER, et al. (2007) Structural order-disorder transformations monitored by X-ray diffraction and photoluminescence. J Chem Educ 84: 814-817. doi: 10.1021/ed084p814
[14]	Gurgel MFC, Paris EC, Souza G, et al. (2007) Jahn-Teller effect on the structure of the Sm-doped PbTiO₃: A theoretical approach. J Mol Struc-Theochem 813: 33-37. doi: 10.1016/j.theochem.2007.02.017
[15]	Paris EC, Gurgel MFC, Joya MR, et al. (2010) Structural deformation monitored by vibrational properties and orbital modeling in (Pb, Sm)TiO₃ systems. J Phys Chem Solids 71: 12-17. doi: 10.1016/j.jpcs.2009.09.012
[16]	Paris EC, Gurgel MFC, Boschi TM, et al. (2008) Investigation on the structural properties in Er-doped PbTiO₃ compounds: A correlation between experimental and theoretical results. J Alloy Compd 462: 157-163. doi: 10.1016/j.jallcom.2007.07.107
[17]	Mendes AC, Maia LJQ, Paris EC, et al. (2013) Solvent effect on the optimization of 1.54 μm emission in Er-doped Y₂O₃-Al₂O₃-SiO₂ powders synthesized by a modified Pechini method. Curr Appl Phys 13: 1558-1565.
[18]	Croissant JG, Butler KS, Zink JI, et al. (2020) Synthetic amorphous silica nanoparticles: Toxicity, biomedical and environmental implications. Nat Rev Mater 5: 886-909. doi: 10.1038/s41578-020-0230-0
[19]	Li Z, Barnes JC, Bosoy A, et al. (2012) Mesoporous silica nanoparticles in biomedical applications. Chem Soc Rev 41: 2590-2605. doi: 10.1039/c1cs15246g
[20]	Crucho CIC, Baleiza C, Farinha JPS (2017) Functional group coverage and conversion quantification in nanostructured silica by ¹H NMR. Anal Chem 89: 681-687. doi: 10.1021/acs.analchem.6b03117
[21]	Davidowski SK, Holland GP (2016) Solid-state NMR characterization of mixed phosphonic acid ligand binding and organization on silica nanoparticles. Langmuir 32: 3253-3261. doi: 10.1021/acs.langmuir.5b03933
[22]	Araújo VD, Avansi W, Paris EC, et al. (2011) Influence of pH on the incorporation and growth of Pb₂CrO₅ crystallites in silica matrix. J Sol-gel Sci Technol 59: 488-494. doi: 10.1007/s10971-011-2517-5
[23]	Thanh NTK, Green LAW (2010) Functionalisation of nanoparticles for biomedical applications. Nano Today 5: 213-230. doi: 10.1016/j.nantod.2010.05.003
[24]	Gao P, Nie X, Zou M, et al. (2011) Recent advances in materials for extended-release antibiotic delivery system. J Antibiot 64: 625-634. doi: 10.1038/ja.2011.58
[25]	Silva R, Martins G, Mario J, et al. (2019) Cloxacillin benzathine-loaded polymeric nanocapsules: Physicochemical characterization, cell uptake, and intramammary antimicrobial effect. Mater Sci Eng C-Mater 104: 110006. doi: 10.1016/j.msec.2019.110006
[26]	Hälleberg Nyman M, Johansson JE, Persson K, et al. (2011) A prospective study of nosocomial urinary tract infection in hip fracture patients. J Clin Nurs 20: 2531-2539. doi: 10.1111/j.1365-2702.2011.03769.x
[27]	Bru JP, Garraffo R (2012) Role of intravenous cloxacillin for inpatient infections. Med Mal Infect 42: 241-246. doi: 10.1016/j.medmal.2011.10.015
[28]	Tuomela A, Hirvonen J, Peltonen L (2016) Stabilizing agents for drug nanocrystals : Effect on bioavailability. Pharmaceutics 8: 16. doi: 10.3390/pharmaceutics8020016
[29]	Javed R, Zia M, Naz S, et al. (2020) Role of capping agents in the application of nanoparticles in biomedicine and environmental remediation : Recent trends and future prospects. J Nanobiotechnol 18: 1-15. doi: 10.1186/s12951-020-00704-4
[30]	Stöber W, Fink A, Bohn E (1968) Controlled growth of monodisperse silica spheres in the micron size range. J Colloid Interf Sci 26: 62-69. doi: 10.1016/0021-9797(68)90272-5
[31]	Kresge CT, Leonowicz ME, Roth WJ, et al. (1992) Ordered mesoporous molecular sieves synthesized by a liquid-crystal template mechanism. Nature 359: 710-712. doi: 10.1038/359710a0
[32]	Malta OL, Brito HF, Menezes JFS, et al. (1998) Experimental and theoretical emission quantum yield in the compound Eu(thenoyltrifluoroacetonate)_3.2(dibenzyl sulfoxide). Chem Phys Lett 282: 233-238.
[33]	Ibrahim IA, Zikry AAF, Sharaf MA (2010) Preparation of spherical silica nanoparticles: Stober silica. J Am Sci 6: 985-989.
[34]	onacchi S, Genovese D, Juris R, et al. (2011) Luminescent silica nanoparticles: Extending the frontiers of brightness. Angew Chemie Int Edit 50: 4056-4066. doi: 10.1002/anie.201004996
[35]	Sayadi K, Rahdar A, Hajinezhad MR, et al. (2020) Atorvastatin-loaded SBA-16 nanostructures: Synthesis, physical characterization, and biochemical alterations in hyperlipidemic rats. J Mol Struct 1202: 127296. doi: 10.1016/j.molstruc.2019.127296
[36]	Koshida N (2008) Device Applications of Silicon Nanocrystals and Nanostructures, Springer Science & Business Media.
[37]	Abadi MHS, Delbari A, Fakoor Z, et al. (2015) Effects of annealing temperature on infrared spectra of SiO₂ extracted from rice husk. J Ceram Sci Technol 46: 41-46.
[38]	Ay F, Aydinli A (2004) Comparative investigation of hydrogen bonding in silicon based PECVD grown dielectrics for optical waveguides. Opt Mater 26: 33-46. doi: 10.1016/j.optmat.2003.12.004
[39]	Bange JP, Patil LS, Gautam DK (2008) Growth and characterization of SiO₂ films deposited by flame hydrolysis deposition system for photonic device application. PIER M 3: 165-175. doi: 10.2528/PIERM08060401
[40]	Moore C, Perova TS, Kennedy BJ, et al. (2003) Study of structure and quality of different silicon oxides using FTIR and Raman microscopy, Opto-Ireland 2002: Optics and Photonics Technologies and Applications, International Society for Optics and Photonics, 4876: 1247-1256.
[41]	Selvan ST, Hayakawa T, Nogami M (2001) Enhanced fluorescence from Eu³⁺-doped silica gels by adsorbed CdS nanoparticles. J Non-Cryst Solids 291: 137-141. doi: 10.1016/S0022-3093(01)00859-6
[42]	Shi M, Xia L, Chen Z, et al. (2017) Europium-doped mesoporous silica nanosphere as an immune-modulating osteogenesis/angiogenesis agent. Biomaterials 144: 176-187. doi: 10.1016/j.biomaterials.2017.08.027
[43]	Volanti DP, Rosa IL V, Paris EC, et al. (2009) The role of the Eu³⁺ ions in structure and photoluminescence properties of SrBi₂Nb₂O₉ powders. Opt Mater 31: 995-999. doi: 10.1016/j.optmat.2008.11.006
[44]	André RS, Paris EC, Gurgel MFC, et al. (2012) Structural evolution of Eu-doped hydroxyapatite nanorods monitored by photoluminescence emission. J Alloy Compd 531: 50-54. doi: 10.1016/j.jallcom.2012.02.053
[45]	Molkenova A, Oteulina Z, Atabaev TS (2021) Europium (Ⅲ)-doped mesoporous silica nanoparticles (SiO₂-Eu NPs) prepared via the soaking method. Results Mater 11: 100209-100213. doi: 10.1016/j.rinma.2021.100209
[46]	Rahman IA, Jafarzadeh M, Sipaut CS (2009) Synthesis of organo-functionalized nanosilica via a co-condensation modification using γ-aminopropyltriethoxysilane (APTES). Ceram Int 35: 1883-1888. doi: 10.1016/j.ceramint.2008.10.028
[47]	Bourkaib MC, Gaudin P, Vibert F, et al. (2021) APTES modified SBA15 and meso-macro silica materials for the immobilization of aminoacylases from Streptomyces ambofaciens. Micropor Mesopor Mater 323: 111226. doi: 10.1016/j.micromeso.2021.111226
[48]	Kulkarni SA, Ogale SB, Vijayamohanan KP (2008) Tuning the hydrophobic properties of silica particles by surface silanization using mixed self-assembled monolayers. J Colloid Interf Sci 318: 372-379. doi: 10.1016/j.jcis.2007.11.012
[49]	Wang Y, Sun Y, Wang J, et al. (2016) Charge-reversal APTES-modi fied mesoporous silica nanoparticles with high drug loading and release controllability. ACS Appl Mater Inter 8: 17166-17175. doi: 10.1021/acsami.6b05370
[50]	Yagub MT, Sen TK, Afroze S, et al. (2014) Dye and its removal from aqueous solution by adsorption: A review. Adv Colloid Interfac 209: 172-184. doi: 10.1016/j.cis.2014.04.002

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