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:

Layer-by-layer supramolecular structures composed of alternate layers of negatively charged enzymes and cationic redox polyelectrolyte have been assembled. Glucose oxidase (GOx), lactate oxidase (LOx) and soybean peroxidase (SBP) have been electrically wired to the underlying electrode by means of poly(allylamine) with [Os(bpy)2CIPyCOH]+ covalently attached (PAA-Os) in organized structures with high spatial resolution. Biotinylated glucose oxidase has also been used to assemble step-by-step on antibiotin goat immunoglobulin (IgG) layers and the enzyme was electrically wired by PAA-Os. These spatially organized multilayers with mono- and bienzymatic schemes can work efficiently in molecular recognition, redox mediation and generation of an electrical signal. The concentration of redox mediator integrated into the multilayers, obtained from the voltammetric charge and an estimation of the layer thickness, exceeds by 100-fold the amount of deposited enzyme assessed by quartz crystal microbalance. Differences in GOx electrical wiring efficiency have been detected with the different assembling strategies. The surface concentration of electrically wired enzyme represents a small proportion of all the enzyme molecules present in the multilayers which can be oxidized by the soluble mediator [Os(bpy)2Cl PyCOOH]Cl. This proportion, as well as the rate of FADH2 oxidation by PAA-Os, increases with the number of electrically wired enzyme layers and with the spatial accessibility of the Os moiety to the enzyme active center.

Registro:

Documento: Artículo
Título:Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation
Autor:Calvo, E.J.; Battaglini, F.; Danilowicz, C.; Wolosiuk, A.; Otero, M.
Filiación:INQUIMAE-Fac. de Cie. Exact. y Nat., Universidad de Buenos Aires, Ciudad Universitaria, AR-1428, Buenos Aires, Argentina
CONICET, Argentina
Facultad de Farmacia y Bioquimica, Universidad de Buenos Aires, Junin 956, AR-1113, Buenos Aires, Argentina
Palabras clave:immobilized enzyme; adsorption; article; chemistry; oxidation reduction reaction; physical chemistry; signal processing; surface property; Adsorption; Chemistry, Physical; Enzymes, Immobilized; Oxidation-Reduction; Signal Processing, Computer-Assisted; Surface Properties
Año:2000
Volumen:116
Página de inicio:47
Página de fin:65
DOI: http://dx.doi.org/10.1039/b001665i
Título revista:Faraday Discussions
Título revista abreviado:Faraday Discuss.
ISSN:13596640
CAS:Enzymes, Immobilized
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_13596640_v116_n_p47_Calvo

Referencias:

  • Rajagopalan, R., Heller, A., (1997) Molecular Electronics, p. 241. , ed. J. Jortner and M. Ratner, Blackwell Science, Oxford
  • Degani, Y., Heller, A., (1989) J. Am. Chem. Soc., 111, p. 2357
  • Gregg, B.A., Heller, A., (1991) J. Phys. Chem., 95, p. 5970
  • Gregg, B.A., Heller, A., (1991) J. Phys. Chem., 95, p. 5976
  • Heller, A., (1992) Acc. Chem. Res., 23, p. 128
  • Pishko, M.V., Katakis, I., Lindquist, S.E., Ye, L., Gregg, B.A., Heller, A., (1992) J. Phys. Chem., 96, p. 3579
  • Willner, J., Riklin, A., Shoham, B., Rivenzon, D., Katz, E., (1993) Adv. Mater., 5 (12), p. 912
  • Anicet, N., Anne, A., Moiroux, J., Savéant, J.M., (1998) J. Am. Chem. Soc., 120, p. 7115
  • Hodak, J., Etchenique, R., Calvo, E.J., Singhal, K., Bartlett, P.N., (1997) Langmuir, 13, p. 2716
  • Murray, R.W., (1992) Molecular Design of Electrode Surfaces, p. 1. , ed. R. W. Murray, John Wiley & Sons, New York
  • Ulmann, A., (1991) An Introduction to Ultrathin Ogranic Films: From Langmuir-Blodgett to Self-Assembly, , Academic Press, Boston
  • Willner, I., Riklin, A., (1994) Anal. Chem., 66, p. 1535
  • Willner, I., Lapidot, N., Riklin, A., Kasher, R., Zahavy, E., Katz, E., (1994) J. Am. Chem. Soc., 116, p. 1428
  • Decher, G., Hong, J.D., Schmitt, J., (1992) Thin Solid Films, 210-211, p. 831
  • Decher, G., Hong, J.D., (1991) Ber. Bunsen-Ges. Phys. Chem., 95, p. 1430
  • Lvov, Y., Decher, G., Sukhorukov, G., (1993) Macromolecules, 26, p. 5396
  • Decher, G., (1997) Science, 277, p. 1232
  • Lvov, Y., Decher, G., Mohwald, H., (1993) Langmuir, 9, p. 481
  • Lvov, Y., Ariga, K., Ichinose, I., Kunitake, T., (1995) J. Am. Chem. Soc., 117, p. 6117
  • Sun, S., Ho-Si, P.H., Harrison, D.J., (1991) Langmuir, 7, p. 727
  • Mizutani, F., Sato, Y., Yabuki, S., Hirata, Y., (1996) Chem. Lett., p. 251
  • Kinnear, K.T., Monbouquette, H.G., (1993) Langmuir, 9, p. 2255
  • Guiomar, A.J., Guthrie, J.T., Evans, S.D., (1999) Langmuir, 15, p. 1198
  • Onda, M., Lvov, Y., Ariga, K., Kunitake, T., (1996) J. Ferment. Bioeng., 82, p. 502
  • Lvov, Y., (2000) Protein Architecture, p. 125. , ed. Y. Lvov and H. Mohwald, Marcel Dekker, New York, ch. 6
  • Lvov, Y., Ariga, K., Ichinose, I., Kunitake, T., (1995) J. Am. Chem. Soc., 117, p. 6117
  • Blonder, R., Katz, E., Cohen, Y., Itzhak, N., Riklin, A., Wilner, I., (1996) Anal. Chem., 68, p. 3151
  • Bourdillon, C., Demaille, C., Gueris, J., Moiroux, J., Savéant, J.M., (1993) J. Am. Chem. Soc., 115, p. 1264
  • Bourdillon, C., Demaille, C., Moiroux, J., Savéant, J.M., (1994) J. Am. Chem. Soc., 116, p. 10328
  • Bourdillon, C., Demaille, C., Moiroux, J., Savéant, J.M., (1995) J. Am. Chem. Soc., 117, p. 11499
  • Bourdillon, C., Demaille, C., Moiroux, J., Savéant, J.M., (1996) Acc. Chem. Res., 29, p. 529
  • Anicet, N., Bourdillon, C., Moiroux, J., Savéant, J.M., (1998) J. Phys. Chem. B, 102, p. 9844
  • Bourdillon, C., Demaille, C., Moiroux, J., Savéant, J.M., (1999) J. Phys. Chem. B, 103, p. 8532
  • Rusling, J.F., (1998) Acc. Chem. Res., 31, p. 363
  • Rusling, J.M., (2000) Protein Architecture, p. 337. , ed. Y. Lvov and H. Mohwald, Marcel Dekker, New York, ch. 13
  • Franchina, J.G., Lackowski, W.M., Dermody, D.L., Crooks, R.M., Bergbreiter, D.E., Sirkar, K., Russell, R.J., Pishko, M.V., (1999) Anal. Chem., 71, p. 3133
  • Danilowicz, C., Corton, E., Battaglini, F., (1998) J. Electroanal. Chem., 445, p. 89
  • Weibel, M., Bright, H.J., (1971) Biochem. J., 124, p. 801
  • Finklea, H.O., Snider, D.A., Fedyk, J., (1990) Langmuir, 6, p. 371
  • Calvo, E.J., Danilowicz, C., Etchenique, R., (1995) J. Chem. Soc., Faraday Trans., 91, p. 4083
  • Wilson, R., Turner, A.P.F., (1992) Biosens. Bioelectron., 7, p. 165
  • Danilowicz, C., Cortón, E., Battaglini, F., Calvo, E.J., (1998) Electrochim, Acta, 43, p. 3525
  • Calvo, E.J., Danilowicz, C., Etchenique, R.A., Pietrasanta, L., Wolosiuk, A., Anal. Chem., , submitted
  • Hecht, H.J., Kalisz, H.M., Hendle, H., Schmid, R.D., Schomburg, D., (1993) J. Mol. Biol., 229, p. 153
  • Rickert, J., Brecht, A., Göpel, W., (1997) Anal. Chem., 69, p. 1441
  • Wolosiuk, A., Calvo, E.J., J. Phys. Chem., , submitted
  • Szucs, A., Hitchens, G.D., Bockris, J.O., (1989) J. Electrochem. Soc., 136, p. 3748
  • Danilowicz, C., Manrique, J.M., (1999) Electrochem. Commun., 1, p. 22
  • Calvo, E.J., Danilowicz, C.D., Lagier, C., Manrique, J., Otero, M., Anal. Chem., , submitted
  • Caruso, F., Nikura, K., Furlong, D., Okata, Y., (1997) Langmuir, 13, p. 3427
  • Amit, A.G., Mariuzza, R.A., Phillips, S.E., Poljak, R., (1986) Science, 233, p. 747
  • Kulys, J.J., Pesliakinese, M.V., Samalius, A.S., (1981) Bioelectrochem. Bioenerg., 8, p. 81
  • Kenausis, G., Chen, Q., Heller, A., (1997) Anal. Chem., 69, p. 1054
  • Scheller, F., Pfeiffer, D., (1980) Anal. Chim. Acta, 117, p. 383
  • Laurent, D., Schlenoff, J.B., (1997) Langmuir, 13, p. 1552
  • Baur, J.W., Rubner, M.F., Reynolds, J.R., Kim, S., (1999) Langmuir, 15, p. 6460
  • Battaglini, F., Bartlett, P.N., Wang, J.H., (2000) Anal. Chem., 72, p. 502
  • Calvo, E.J., Etchenique, R., (1999) J. Phys. Chem. B, 103, p. 8944
  • Bartlett, P.N., Pratt, K.F.E., (1995) J. Electroanal. Chem., 397, p. 61

Citas:

---------- APA ----------
Calvo, E.J., Battaglini, F., Danilowicz, C., Wolosiuk, A. & Otero, M. (2000) . Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation. Faraday Discussions, 116, 47-65.
http://dx.doi.org/10.1039/b001665i
---------- CHICAGO ----------
Calvo, E.J., Battaglini, F., Danilowicz, C., Wolosiuk, A., Otero, M. "Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation" . Faraday Discussions 116 (2000) : 47-65.
http://dx.doi.org/10.1039/b001665i
---------- MLA ----------
Calvo, E.J., Battaglini, F., Danilowicz, C., Wolosiuk, A., Otero, M. "Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation" . Faraday Discussions, vol. 116, 2000, pp. 47-65.
http://dx.doi.org/10.1039/b001665i
---------- VANCOUVER ----------
Calvo, E.J., Battaglini, F., Danilowicz, C., Wolosiuk, A., Otero, M. Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation. Faraday Discuss. 2000;116:47-65.
http://dx.doi.org/10.1039/b001665i