Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation

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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 p...

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Autores principales: Calvo, E.J., Battaglini, F., Danilowicz, C., Wolosiuk, A., Otero, M.
Formato: JOUR
Materias:
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
Acceso en línea:http://hdl.handle.net/20.500.12110/paper_13596640_v116_n_p47_Calvo
Aporte de:
Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires
id todo:paper_13596640_v116_n_p47_Calvo
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spelling todo:paper_13596640_v116_n_p47_Calvo2023-10-03T16:10:39Z Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation Calvo, E.J. Battaglini, F. Danilowicz, C. Wolosiuk, A. Otero, M. 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 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. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_13596640_v116_n_p47_Calvo
institution Universidad de Buenos Aires
institution_str I-28
repository_str R-134
collection Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
topic 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
spellingShingle 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
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
topic_facet 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
description 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.
format JOUR
author Calvo, E.J.
Battaglini, F.
Danilowicz, C.
Wolosiuk, A.
Otero, M.
author_facet Calvo, E.J.
Battaglini, F.
Danilowicz, C.
Wolosiuk, A.
Otero, M.
author_sort Calvo, E.J.
title Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation
title_short Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation
title_full Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation
title_fullStr Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation
title_full_unstemmed Layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation
title_sort layer-by-layer electrostatic deposition of biomolecules on surfaces for molecular recognition, redox mediation and signal generation
url http://hdl.handle.net/20.500.12110/paper_13596640_v116_n_p47_Calvo
work_keys_str_mv AT calvoej layerbylayerelectrostaticdepositionofbiomoleculesonsurfacesformolecularrecognitionredoxmediationandsignalgeneration
AT battaglinif layerbylayerelectrostaticdepositionofbiomoleculesonsurfacesformolecularrecognitionredoxmediationandsignalgeneration
AT danilowiczc layerbylayerelectrostaticdepositionofbiomoleculesonsurfacesformolecularrecognitionredoxmediationandsignalgeneration
AT wolosiuka layerbylayerelectrostaticdepositionofbiomoleculesonsurfacesformolecularrecognitionredoxmediationandsignalgeneration
AT oterom layerbylayerelectrostaticdepositionofbiomoleculesonsurfacesformolecularrecognitionredoxmediationandsignalgeneration
_version_ 1807322062716403712

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