Abstract:
Self-assembled multilayers comprised of alternate layers of polyphenol oxidase (PPO) and poly(allylamine) (PAH) or PPO and poly(diallyldimethylamine) (PDDA), deposited on a 3-mercaptopropanesulfonic acid (MPS)-modified gold surface, were studied "in-situ" (under water) by means of ellipsometry and quartz crystal microbalance (QCM), and "ex-situ" (in open air) by ellipsometry and fourier transform infrared reflection-absorption spectroscopy (FT-IRRAS). Optical ellipsometric properties of (PAH n(PPO)n and (PDDA)n(PPO)n multilayers were obtained at two wavelengths, employing an isotropic single-layer model with the substrate parameters measured after thiol adsorption. Film thickness as well as ellipsometric mass values based on the de Feijter equation were also evaluated. The quartz crystal impedance analysis showed that self-assembled multilayers behaved as acoustically thin films, and therefore, the shifts observed in the film inductive impedance parameter were interpreted in terms of gravimetric mass. The enzyme mass uptake in each adsorption step was determined on PAH or on PDDA topmost layer. A comparative study between the ellipsometric thickness and acoustic mass values allowed us to obtain average values of "apparent" densities of (2.1 ± 0.1) and (2.4 ± 0.1) g cm-3 for (PAH)n(PPO n and (PDDA)n(PPO)n multilayers, respectively. The content of water included in the open polymer-enzyme structure was evaluated by comparison of QCM and ellipsometric mass values. FT-IRRAS spectra of each layer in (PAH)n(PPO n and (PDDA)n(PPO)n films were recorded, and the intensity ratio of the amide bands was evaluated to obtain information about layer-by-layer enzyme conformation. An enzyme/polycation distribution model for (PAH)n-(PPO)n and (PDDA)n(PPO)n multilayer structures is presented on the basis of combined ellipsometric, QCM, and FT-IRRAS results.
Registro:
Documento: |
Artículo
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Título: | Effect of the polycation nature on the structure of layer-by-layer electrostatically self-assembled multilayers of polyphenol oxidase |
Autor: | Forzani, E.S.; López Teijelo, M.; Nart, F.; Calvo, E.J.; Solís, V.M. |
Filiación: | INQUIMAE, Departamento de Quimica Inorganica, Ciudad Universitaria, Pabellón 2, AR-1428 Buenos Aires, Argentina INFIQC, Departmento de Fisicoquímica, Universidad Nacional de Cordoba, Pabellón Argentina, AR-5000 Córdoba, Argentina Instituto de Quimica de Sao Carlos, Universidad de Sao Paulo, C.P. 780, 13560-970 Sao Carlos, SP, Brazil
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Palabras clave: | Absorption spectroscopy; Electric impedance; Enzymes; Fourier transform infrared spectroscopy; Positive ions; Self assembly; Polycations; Macromolecules; 3 mercaptopropanesulfonic acid; catechol oxidase; enzyme; gold; poly(allylamine); poly(diallyldimethylamine); polycation; polymer; silicon dioxide; sulfonic acid derivative; thiol; unclassified drug; water; absorption; article; calculation; chemical structure; comparative study; controlled study; density; electricity; ellipsometry; enzyme structure; enzyme substrate; film; gravimetry; impedance; infrared spectroscopy; molecular model; priority journal; surface property; thickness; water content; Catechol Oxidase; Electrostatics; Gold; Microchemistry; Polyamines; Quartz; Spectroscopy, Fourier Transform Infrared; Sulfonic Acids; Surface Properties |
Año: | 2003
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Volumen: | 4
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Número: | 4
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Página de inicio: | 869
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Página de fin: | 879
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DOI: |
http://dx.doi.org/10.1021/bm0256855 |
Título revista: | Biomacromolecules
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Título revista abreviado: | Biomacromolecules
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ISSN: | 15257797
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CODEN: | BOMAF
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CAS: | gold, 7440-57-5; silicon dioxide, 10279-57-9, 14464-46-1, 14808-60-7, 15468-32-3, 60676-86-0, 7631-86-9; water, 7732-18-5; Catechol Oxidase, EC 1.10.3.1; Gold, 7440-57-5; polyallylamine, 30551-89-4; Polyamines; polycations; Quartz, 14808-60-7; Sulfonic Acids
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Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_15257797_v4_n4_p869_Forzani |
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Citas:
---------- APA ----------
Forzani, E.S., López Teijelo, M., Nart, F., Calvo, E.J. & Solís, V.M.
(2003)
. Effect of the polycation nature on the structure of layer-by-layer electrostatically self-assembled multilayers of polyphenol oxidase. Biomacromolecules, 4(4), 869-879.
http://dx.doi.org/10.1021/bm0256855---------- CHICAGO ----------
Forzani, E.S., López Teijelo, M., Nart, F., Calvo, E.J., Solís, V.M.
"Effect of the polycation nature on the structure of layer-by-layer electrostatically self-assembled multilayers of polyphenol oxidase"
. Biomacromolecules 4, no. 4
(2003) : 869-879.
http://dx.doi.org/10.1021/bm0256855---------- MLA ----------
Forzani, E.S., López Teijelo, M., Nart, F., Calvo, E.J., Solís, V.M.
"Effect of the polycation nature on the structure of layer-by-layer electrostatically self-assembled multilayers of polyphenol oxidase"
. Biomacromolecules, vol. 4, no. 4, 2003, pp. 869-879.
http://dx.doi.org/10.1021/bm0256855---------- VANCOUVER ----------
Forzani, E.S., López Teijelo, M., Nart, F., Calvo, E.J., Solís, V.M. Effect of the polycation nature on the structure of layer-by-layer electrostatically self-assembled multilayers of polyphenol oxidase. Biomacromolecules. 2003;4(4):869-879.
http://dx.doi.org/10.1021/bm0256855