Artículo

Estamos trabajando para incorporar este artículo al repositorio
Consulte el artículo en la página del editor
Consulte la política de Acceso Abierto del editor

Abstract:

Silica matrices synthesized from a pre-hydrolysis step in ethanol followed by alcohol removal at low pressure distillation, and condensation in water, are suitable for encapsulation of biomolecules and microorganisms and building bioactive materials with optimized optical properties. Here we analyze the microstructure of these hydrogels from the dependence of I(q) data acquired from SAXS experiments over a wide range of silica concentration and pH employed in the condensation step. From the resulting data it is shown that there is a clear correlation between the microscopic parameters-cluster fractal dimension (D), elementary particle radius (a) and cluster gyration radius (R)-with the attenuation of visible light when the condensation step proceeds at pH < 6. At higher pHs, there is a steep dependence of the cluster density (~R D-3 ) with the condensation pH, and non-monotonous changes of attenuance are less than 20%, revealing the complexity of the system. These results, which were obtained for a wide pH and silica concentration range, reinforce the idea that the behavior of gels determined in a restricted interval of synthesis variables cannot be extrapolated, and comparison of gelation times is not enough for predicting their properties. © 2011 Springer Science+Business Media, LLC.

Registro:

Documento: Artículo
Título:Effect of synthesis conditions on the microstructure of TEOS derived silica hydrogels synthesized by the alcohol-free sol-gel route
Autor:Perullini, M.; Jobbágy, M.; Bilmes, S.A.; Torriani, I.L.; Candal, R.
Filiación:INQUIMAE-DQIAQF, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Pab. II, Buenos Aires C1428EHA, Argentina
ECyT, Universidad Nacional de San Martín, Campus Miguelete, San Martín, Buenos Aires, Argentina
Institute of Physics Gleb Wataghin, State University of Campinas, Campinas, SP, Brazil
Palabras clave:Optical quality; SAXS microstructure characterization; Silica hydrogels; TEOS alcohol-free; Bioactive material; Cluster densities; Gyration radii; Low pressures; Optical qualities; SAXS microstructure characterization; Silica concentrations; Silica matrix; Sol-gel routes; Synthesis conditions; TEOS alcohol-free; Visible light; Coagulation; Condensation; Distillation; Elementary particles; Ethanol; Fractal dimension; Gelation; Gels; Hydrogels; Optical properties; Pressure effects; Silica; Sol-gel process; Microstructure
Año:2011
Volumen:59
Número:1
Página de inicio:174
Página de fin:180
DOI: http://dx.doi.org/10.1007/s10971-011-2478-8
Título revista:Journal of Sol-Gel Science and Technology
Título revista abreviado:J Sol Gel Sci Technol
ISSN:09280707
CODEN:JSGTE
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_09280707_v59_n1_p174_Perullini

Referencias:

  • Brinker, C.J., Scherer, G., (1990) Sol Gel Science, , Academic Press San Diego
  • Gill, I., Ballesteros, A., Encapsulation of biologicals within silicate, siloxane, and hybrid sol- gel polymers: An efficient and generic approach (1998) Journal of the American Chemical Society, 120 (34), pp. 8587-8598. , DOI 10.1021/ja9814568
  • Avnir, D., Brown, S., Lev, O., Ottolenghi, M., Enzymes and other proteins entrapped in sol-gel materials (1994) Chem Mater, 6 (10), pp. 1605-1614. , 10.1021/cm00046a008 1:CAS:528:DyaK2cXlvF2rsLo%3D
  • Avnir, D., Lev, O., Livage, J., Recent bio-applications of sol-gel materials (2006) Journal of Materials Chemistry, 16 (11), pp. 1013-1030. , DOI 10.1039/b512706h
  • Livage, J., Coradin, T., Living cells in oxide glasses (2006) Rev Mineral Geochem, 64 (1), pp. 315-332. , 10.2138/rmg.2006.64.10 1:CAS:528:DC%2BD2sXkslKnsw%3D%3D
  • Soltmann, U., Böttcher, H., Utilization of sol-gel ceramics for the immobilization of living microorganisms (2008) J Sol-Gel Sci Technol, 342, p. 211
  • Meunier, C.F., Dandoy, P., Su, B.-L., Encapsulation of cells within silica matrixes: Towards a new advance in the conception of living hybrid materials (2010) J Colloid Interface Sci, 48, pp. 66-72
  • Premkumar, J.R., Lev, O., Marks, R.S., Polyak, B., Rosen, R., Belkin, S., Antibody-based immobilization of bioluminescent bacterial sensor cells (2001) Talanta, 55 (5), pp. 1029-1038. , DOI 10.1016/S0039-9140(01)00533-1, PII S0039914001005331
  • Perullini, M., Rivero, M.M., Jobbagy, M., Mentaberry, A., Bilmes, S.A., Plant cell proliferation inside an inorganic host (2007) Journal of Biotechnology, 127 (3), pp. 542-548. , DOI 10.1016/j.jbiotec.2006.07.024, PII S0168165606006365
  • Fiedler, D., Hager, U., Franke, H., Soltmann, U., Bottcher, H., Algae biocers: Astaxanthin formation in sol-gel immobilised living microalgae (2007) Journal of Materials Chemistry, 17 (3), pp. 261-266. , DOI 10.1039/b613455f
  • Kuncova, G., Podrazky, O., Ripp, S., Trögl, J., Sayler, G.S., Demnerova, K., Vankova, R., Monitoring of the viability of cells immobilized by sol-gel process (2004) J Sol-Gel Sci Technol, 31, pp. 1-8. , 10.1023/B:JSST.0000048013.64235.c8
  • Nguyen-Ngoc, H., Durrieu, C., Tran-Minh, C., Synchronous-scan fluorescence of algal cells for toxicity assessment of heavy metals and herbicides (2009) Ecotoxicol Environ Saf, 72, pp. 316-320. , 10.1016/j.ecoenv.2008.04.016 1:CAS:528:DC%2BD1cXhtlaqtbbN
  • Sicard, C., Perullini, M., Spedalieri, C., Coradin, T., Brayner, R., Livage, J., Jobbagy, M., Bilmes, S.A., CeO2 nanoparticles for the protection of photosynthetic organisms immobilized in silica gels (2011) Chem Mater, 23 (6), pp. 1374-1378. , 1:CAS:528:DC%2BC3MXit1WjsLw%3D
  • Perullini, M., Jobbagy, M., Moretti, M.B., Garcia, S.C., Bilmes, S.A., Optimizing silica encapsulation of living cells: In situ evaluation of cellular stress (2008) Chemistry of Materials, 20 (9), pp. 3015-3021. , DOI 10.1021/cm703075b
  • Brumberger, H., Modern aspects of small-angle scattering (1993) Proceedings of the NATO Advanced Study Institutes, , Como, Italy
  • Schmidt, P.W., Höhr, A., Neumann, H.-B., Kaiser, H., Avnir, D., Lin, J.S., Small angle X-ray scattering study of the fractal morphology of porous silicas (1989) J Chem Phys, 90 (9), pp. 5016-5023. , 10.1063/1.456544 1:CAS:528:DyaL1MXlt1WnsLk%3D
  • Vollet, D.R., Donatti, D.A., Ibãez Ruiz, A., De Vicente, F.S., Dynamical scaling in fractal structures in the aggregation of tetraethoxysilane-derived sonogels (2010) J Appl Cryst, 43 (5), pp. 949-954. , 10.1107/S0021889810025161 1:CAS:528:DC%2BC3cXhtFOqsbjM
  • Zarzycki, J., Fractal properties of gels (1987) J Non-Cryst Solids, 9596 (1), pp. 173-184. , 10.1016/S0022-3093(87)80108-4
  • Schaefer, D.W., Keefer, K.D., Fractal geometry of silica condensation polymers (1984) Phys Rev Lett, 53 (14), pp. 1383-1386. , 10.1103/PhysRevLett.53.1383 1:CAS:528:DyaL2MXjtVKmsw%3D%3D
  • Mandelbrot, B.B., (1983) The Fractal Geometry of Nature, , Freeman San Francisco
  • Kim, S., Lee, K.-S., Zachariah, M.R., Lee, D., Three-dimensional off-lattice Monte Carlo simulations on a direct relation between experimental process parameters and fractal dimension of colloidal aggregates (2010) J Colloid Interface Sci, 344, pp. 353-361. , 10.1016/j.jcis.2010.01.008 1:CAS:528:DC%2BC3cXjtFKjsbs%3D
  • Schaefer, D.W., Martin, J.E., Wiltzius, P., Cannell, D.S., Fractal geometry of colloidal aggregates (1984) Phys Rev Lett, 52 (26), pp. 2371-2374. , 10.1103/PhysRevLett.52.2371 1:CAS:528:DyaL2cXks1Skt7c%3D
  • Vollet, D.R., Donatti, D.A., Ibanez Ruiz, A., A SAXS study of kinetics of aggregation of TEOS-derived sonogels at different temperatures (2001) Journal of Non-Crystalline Solids, 288 (1-3), pp. 81-87. , DOI 10.1016/S0022-3093(01)00607-X, PII S002230930100607X
  • Brinker, C.J., Keefer, K.D., Schaefer, D.W., Assink, R.A., Kay, B.D., Ashley, C.S., Sol gel transition in simple silicates (1984) J Non-Cryst Solids, 63, pp. 45-59. , 10.1016/0022-3093(84)90385-5 1:CAS:528:DyaL2cXhs1Srsr4%3D
  • Strawbridge, I., Craievich, A.F., James, P.F., Effect of the h 2 o/teos ratio on the structure of gels derived by the acid catalysed hydrolysis of tetraethoxysilane (1985) Journal of Non-Crystalline Solids, 72 (1), pp. 139-157. , DOI 10.1016/0022-3093(85)90170-X
  • Himmel, B., Gerber, Th., Burger, H., WAXS- and SAXS-investigations of structure formation in alcoholic SiO 2 solutions (1990) Journal of Non-Crystalline Solids, 119 (1), pp. 1-13. , DOI 10.1016/0022-3093(90)90234-D
  • Reichenauer, G., Thermal aging of silica gels in water (2004) J Non-Cryst Solids, 350, pp. 189-195. , 10.1016/j.jnoncrysol.2004.07.073 1:CAS:528:DC%2BD2cXhtVGkur%2FF
  • Bhatia, R.B., Brinker, C.J., Gupta, A.K., Singh, A.K., Aqueous sol-gel process for protein encapsulation (2000) Chem Mater, 12, pp. 2434-2441. , 10.1021/cm000260f 1:CAS:528:DC%2BD3cXltVOjt7g%3D
  • Coiffier, A., Coradin, T., Roux, C., Bouvet, O.M.M., Livage, J., Sol-gel encapsulation of bacteria: A comparison between alkoxide and aqueous routes (2001) Journal of Materials Chemistry, 11 (8), pp. 2039-2044. , DOI 10.1039/b101308o
  • Nassif, N., Roux, C., Coradin, T., Rager, M.N., Bouvet, O., Livage, J., A sol-gel matrix to preserve the viability of encapsulated bacteria (2003) Mater Chem, 13, pp. 203-208. , 10.1039/b210167j 1:CAS:528:DC%2BD3sXps1Chsw%3D%3D
  • Gerberb, T., Himmel, B., Bürger, H., WAXS- and SAXS-investigations of structure formation of gels from sodium water glass (1994) J Non-Cryst Solids, 175, pp. 160-168. , 10.1016/0022-3093(94)90008-6
  • Perullini, M., Amoura, M., Roux, C., Coradin, T., Livage, J., Japas, M.L., Jobbagy, M., Bilmes, S.A., Improving silica matrices for encapsulation of Escherichia coli using osmoprotectors (2011) J Mater Chem, 21, pp. 4546-4552. , 10.1039/c0jm03948a 1:CAS:528:DC%2BC3MXivFygu70%3D
  • Ferrer, M.L., Del Monte, F., Levy, D., A novel and simple alcohol-free sol-gel route for encapsulation of labile proteins (2002) Chem Mater, 14, pp. 3619-3621. , 10.1021/cm025562r 1:CAS:528:DC%2BD38XmtVymu7s%3D
  • Ferrer, M.L., Yuste, L., Rojo, F., Del Monte, F., Biocompatible sol-gel route for encapsulation of living bacteria in organically modified silica matrixes (2003) Chem Mater, 15, pp. 3614-3618. , 10.1021/cm034372t 1:CAS:528:DC%2BD3sXmsVOnsrk%3D
  • Ferrer, M.L., García-Carbajal, Z.Y., Yuste, L., Rojo, F., Del Monte, F., Bacteria viability in sol-gel materials revisited: Cryo-SEM as a suitable tool to study the structural integrity of encapsulated bacteria (2006) Chem Mater, 18, pp. 1458-1463. , 10.1021/cm0522275 1:CAS:528:DC%2BD28Xhtlekurw%3D
  • Cavalcanti, L.P., Torriani, I.L., Plivelic, T.S., Oliveira, C.L.P., Kellermann, G., Neuenschwander, R., Two new sealed sample cells for small angle x-ray scattering from macromolecules in solution and complex fluids using synchrotron radiation (2004) Review of Scientific Instruments, 75 (11), pp. 4541-4546. , DOI 10.1063/1.1804956
  • http://kur.web.psi.ch/sans1/SANSSoft/sasfit.html; Vinogradova, E., Moreno, A., Lara, V.H., Bosch, P., Multi-fractal imaging and structural investigation of silica hydrogels and aerogels (2003) Silicon Chem, 2, pp. 247-254. , 10.1007/s11201-005-3391-1
  • Vinogradova, E., Moreno, A., Lara, V.H., Bosch, P., Multi-fractal imaging and structural investigation of silica hydrogels and aerogels (2003) Silicon Chem, 2, pp. 247-254. , 10.1007/s11201-005-3391-1
  • Avnir, D., Biham, O., Lidar, D., Malcai, O., Is the geometry of nature fractal? (1998) Science, 279 (5347), pp. 39-40. , DOI 10.1126/science.279.5347.39
  • Sorensen, C.M., Wang, G.M., Size distribution effect on the power law regime of the structure factor of fractal aggregates (1999) Physical Review E - Statistical Physics, Plasmas, Fluids, and Related Interdisciplinary Topics, 60 (6 B), pp. 7143-7148
  • Knoblich, B., Gerber, Th., Aggregation in SiO 2 sols from sodium silicate solutions (2001) Journal of Non-Crystalline Solids, 283 (1-3), pp. 109-113. , DOI 10.1016/S0022-3093(01)00356-8, PII S0022309301003568
  • Boukari, H., Lin, J.S., Harris, M.T., Small-angle X-ray scattering study of the formation of colloidal silica particles from alkoxides: Primary particles or not? (1997) Journal of Colloid and Interface Science, 194 (2), pp. 311-318. , DOI 10.1006/jcis.1997.5112
  • Knoblich, B., Gerber, Th., The arrangement of fractal clusters dependent on the pH value in silica gels from sodium silicate solutions (2001) Journal of Non-Crystalline Solids, 296 (1-2), pp. 81-87. , DOI 10.1016/S0022-3093(01)00871-7, PII S0022309301008717
  • Beelen, T.P.M., Pwjg, W., Vonk, C.G., Van Santen, R.A., (1989) Catal Lett, 3, p. 209. , 10.1007/BF00766395 1:CAS:528:DyaL1MXmsVSqs7Y%3D
  • Bohren, C.G., Huffmann, D.F., (1983) Absorption and Scattering of Light by Small Particles, , Wiley New York

Citas:

---------- APA ----------
Perullini, M., Jobbágy, M., Bilmes, S.A., Torriani, I.L. & Candal, R. (2011) . Effect of synthesis conditions on the microstructure of TEOS derived silica hydrogels synthesized by the alcohol-free sol-gel route. Journal of Sol-Gel Science and Technology, 59(1), 174-180.
http://dx.doi.org/10.1007/s10971-011-2478-8
---------- CHICAGO ----------
Perullini, M., Jobbágy, M., Bilmes, S.A., Torriani, I.L., Candal, R. "Effect of synthesis conditions on the microstructure of TEOS derived silica hydrogels synthesized by the alcohol-free sol-gel route" . Journal of Sol-Gel Science and Technology 59, no. 1 (2011) : 174-180.
http://dx.doi.org/10.1007/s10971-011-2478-8
---------- MLA ----------
Perullini, M., Jobbágy, M., Bilmes, S.A., Torriani, I.L., Candal, R. "Effect of synthesis conditions on the microstructure of TEOS derived silica hydrogels synthesized by the alcohol-free sol-gel route" . Journal of Sol-Gel Science and Technology, vol. 59, no. 1, 2011, pp. 174-180.
http://dx.doi.org/10.1007/s10971-011-2478-8
---------- VANCOUVER ----------
Perullini, M., Jobbágy, M., Bilmes, S.A., Torriani, I.L., Candal, R. Effect of synthesis conditions on the microstructure of TEOS derived silica hydrogels synthesized by the alcohol-free sol-gel route. J Sol Gel Sci Technol. 2011;59(1):174-180.
http://dx.doi.org/10.1007/s10971-011-2478-8