Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors

This work describes the synergistic combination of ionic self-assembly and recognition-directed assembly with the aim of creating highly functional bioelectrochemical interfaces compatible with the supramolecular design of a wide variety of biosensing platforms. A recently synthesized glycopolyelect...

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Autores principales:	Cortez, María Lorena, Pallarola, Diego Andrés, Battaglini, Fernando
Publicado:	2013
Materias:	Bio-electrochemical Bioelectrocatalytic currents Biosensing platforms Electrocatalytic properties Electrode surfaces Electron transfer Electron transfer process Electrostatic driving Glycosidic residues Grazing incidence small-angle X-ray scattering Horseradish peroxidase Interfacial architecture Interfacial configurations Ionic self-assembly ITS applications Mesostructured New dimensions Non-covalent interaction Osmium complexes Polyallylamine Redox-active Self assembled films Self assembled structures Self-assembled architectures Specific recognition Substrate inhibition Supramolecular thin film Synergistic combinations Electrodes Ions Organic compounds Self assembly Sodium dodecyl sulfate Sugars Supramolecular chemistry Synthesis (chemical) Electron transitions coordination compound electrolyte horseradish peroxidase lactose osmium polyallylamine polyamine article chemistry electrochemical analysis electrode electron transport enzyme specificity genetic procedures metabolism oxidation reduction reaction quartz crystal microbalance small angle scattering static electricity X ray diffraction Biosensing Techniques Coordination Complexes Electrochemical Techniques Electrolytes Electron Transport Horseradish Peroxidase Lactose Osmium Oxidation-Reduction Polyamines Quartz Crystal Microbalance Techniques Scattering, Small Angle Static Electricity Substrate Specificity X-Ray Diffraction
Acceso en línea:	https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00032700_v85_n4_p2414_Cortez http://hdl.handle.net/20.500.12110/paper_00032700_v85_n4_p2414_Cortez
Aporte de:	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires

id	paper:paper_00032700_v85_n4_p2414_Cortez
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spelling	paper:paper_00032700_v85_n4_p2414_Cortez2023-06-08T14:24:14Z Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors Cortez, María Lorena Pallarola, Diego Andrés Battaglini, Fernando Bio-electrochemical Bioelectrocatalytic currents Biosensing platforms Electrocatalytic properties Electrode surfaces Electron transfer Electron transfer process Electrostatic driving Glycosidic residues Grazing incidence small-angle X-ray scattering Horseradish peroxidase Interfacial architecture Interfacial configurations Ionic self-assembly ITS applications Mesostructured New dimensions Non-covalent interaction Osmium complexes Polyallylamine Redox-active Self assembled films Self assembled structures Self-assembled architectures Specific recognition Substrate inhibition Supramolecular thin film Synergistic combinations Electrodes Ions Organic compounds Self assembly Sodium dodecyl sulfate Sugars Supramolecular chemistry Synthesis (chemical) Electron transitions coordination compound electrolyte horseradish peroxidase lactose osmium polyallylamine polyamine article chemistry electrochemical analysis electrode electron transport enzyme specificity genetic procedures metabolism oxidation reduction reaction quartz crystal microbalance small angle scattering static electricity X ray diffraction Biosensing Techniques Coordination Complexes Electrochemical Techniques Electrodes Electrolytes Electron Transport Horseradish Peroxidase Lactose Osmium Oxidation-Reduction Polyamines Quartz Crystal Microbalance Techniques Scattering, Small Angle Static Electricity Substrate Specificity X-Ray Diffraction This work describes the synergistic combination of ionic self-assembly and recognition-directed assembly with the aim of creating highly functional bioelectrochemical interfaces compatible with the supramolecular design of a wide variety of biosensing platforms. A recently synthesized glycopolyelectrolyte constituted of polyallylamine bearing redox-active osmium complexes and glycosidic residues (lactose) is used to create a self-assembled structure with sodium dodecylsulfate. In turn, this supramolecular thin films bearing redox-active and biorecognizable carbohydrate units enable the facile assembly of functional lectins as well as the subsequent docking and "wiring" of glycoenzymes, like horseradish peroxidase (HRP) (an elusive enzyme to immobilize via noncovalent interactions). The assembly of this system was followed by quartz crystal microbalance and grazing-incidence small-angle X-ray scattering (GISAXS) studies confirming that spin-coated ionically self-assembled films exhibit mesostructured architectures according to the formation of self-organized lamellar structures. In-depth characterization of the electrocatalytic properties of the biosupramacromolecular assemblies confirmed the ability of this kind of interfacial architecture to efficiently mediate electron transfer processes between the glycoenzyme and the electrode surface. For instance, our experimental electrochemical evidence clearly shows that tailor-made interfacial configurations of the ionic self-assemblies can prevent the inhibition of the glycoenzyme (typically observed in HRP) leading to bioelectrocatalytic currents up to 0.1 mA cm-2. The presence of carbohydrate moieties in the ionic domains promotes the biorecognition-driven assembly of lectins adding a new dimension to the capabilities of ionic self-assembly. © 2013 American Chemical Society. Fil:Cortez, M.L. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Pallarola, D. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Battaglini, F. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. 2013 https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00032700_v85_n4_p2414_Cortez http://hdl.handle.net/20.500.12110/paper_00032700_v85_n4_p2414_Cortez
institution	Universidad de Buenos Aires
institution_str	I-28
repository_str	R-134
collection	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
topic	Bio-electrochemical Bioelectrocatalytic currents Biosensing platforms Electrocatalytic properties Electrode surfaces Electron transfer Electron transfer process Electrostatic driving Glycosidic residues Grazing incidence small-angle X-ray scattering Horseradish peroxidase Interfacial architecture Interfacial configurations Ionic self-assembly ITS applications Mesostructured New dimensions Non-covalent interaction Osmium complexes Polyallylamine Redox-active Self assembled films Self assembled structures Self-assembled architectures Specific recognition Substrate inhibition Supramolecular thin film Synergistic combinations Electrodes Ions Organic compounds Self assembly Sodium dodecyl sulfate Sugars Supramolecular chemistry Synthesis (chemical) Electron transitions coordination compound electrolyte horseradish peroxidase lactose osmium polyallylamine polyamine article chemistry electrochemical analysis electrode electron transport enzyme specificity genetic procedures metabolism oxidation reduction reaction quartz crystal microbalance small angle scattering static electricity X ray diffraction Biosensing Techniques Coordination Complexes Electrochemical Techniques Electrodes Electrolytes Electron Transport Horseradish Peroxidase Lactose Osmium Oxidation-Reduction Polyamines Quartz Crystal Microbalance Techniques Scattering, Small Angle Static Electricity Substrate Specificity X-Ray Diffraction
spellingShingle	Bio-electrochemical Bioelectrocatalytic currents Biosensing platforms Electrocatalytic properties Electrode surfaces Electron transfer Electron transfer process Electrostatic driving Glycosidic residues Grazing incidence small-angle X-ray scattering Horseradish peroxidase Interfacial architecture Interfacial configurations Ionic self-assembly ITS applications Mesostructured New dimensions Non-covalent interaction Osmium complexes Polyallylamine Redox-active Self assembled films Self assembled structures Self-assembled architectures Specific recognition Substrate inhibition Supramolecular thin film Synergistic combinations Electrodes Ions Organic compounds Self assembly Sodium dodecyl sulfate Sugars Supramolecular chemistry Synthesis (chemical) Electron transitions coordination compound electrolyte horseradish peroxidase lactose osmium polyallylamine polyamine article chemistry electrochemical analysis electrode electron transport enzyme specificity genetic procedures metabolism oxidation reduction reaction quartz crystal microbalance small angle scattering static electricity X ray diffraction Biosensing Techniques Coordination Complexes Electrochemical Techniques Electrodes Electrolytes Electron Transport Horseradish Peroxidase Lactose Osmium Oxidation-Reduction Polyamines Quartz Crystal Microbalance Techniques Scattering, Small Angle Static Electricity Substrate Specificity X-Ray Diffraction Cortez, María Lorena Pallarola, Diego Andrés Battaglini, Fernando Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors
topic_facet	Bio-electrochemical Bioelectrocatalytic currents Biosensing platforms Electrocatalytic properties Electrode surfaces Electron transfer Electron transfer process Electrostatic driving Glycosidic residues Grazing incidence small-angle X-ray scattering Horseradish peroxidase Interfacial architecture Interfacial configurations Ionic self-assembly ITS applications Mesostructured New dimensions Non-covalent interaction Osmium complexes Polyallylamine Redox-active Self assembled films Self assembled structures Self-assembled architectures Specific recognition Substrate inhibition Supramolecular thin film Synergistic combinations Electrodes Ions Organic compounds Self assembly Sodium dodecyl sulfate Sugars Supramolecular chemistry Synthesis (chemical) Electron transitions coordination compound electrolyte horseradish peroxidase lactose osmium polyallylamine polyamine article chemistry electrochemical analysis electrode electron transport enzyme specificity genetic procedures metabolism oxidation reduction reaction quartz crystal microbalance small angle scattering static electricity X ray diffraction Biosensing Techniques Coordination Complexes Electrochemical Techniques Electrodes Electrolytes Electron Transport Horseradish Peroxidase Lactose Osmium Oxidation-Reduction Polyamines Quartz Crystal Microbalance Techniques Scattering, Small Angle Static Electricity Substrate Specificity X-Ray Diffraction
description	This work describes the synergistic combination of ionic self-assembly and recognition-directed assembly with the aim of creating highly functional bioelectrochemical interfaces compatible with the supramolecular design of a wide variety of biosensing platforms. A recently synthesized glycopolyelectrolyte constituted of polyallylamine bearing redox-active osmium complexes and glycosidic residues (lactose) is used to create a self-assembled structure with sodium dodecylsulfate. In turn, this supramolecular thin films bearing redox-active and biorecognizable carbohydrate units enable the facile assembly of functional lectins as well as the subsequent docking and "wiring" of glycoenzymes, like horseradish peroxidase (HRP) (an elusive enzyme to immobilize via noncovalent interactions). The assembly of this system was followed by quartz crystal microbalance and grazing-incidence small-angle X-ray scattering (GISAXS) studies confirming that spin-coated ionically self-assembled films exhibit mesostructured architectures according to the formation of self-organized lamellar structures. In-depth characterization of the electrocatalytic properties of the biosupramacromolecular assemblies confirmed the ability of this kind of interfacial architecture to efficiently mediate electron transfer processes between the glycoenzyme and the electrode surface. For instance, our experimental electrochemical evidence clearly shows that tailor-made interfacial configurations of the ionic self-assemblies can prevent the inhibition of the glycoenzyme (typically observed in HRP) leading to bioelectrocatalytic currents up to 0.1 mA cm-2. The presence of carbohydrate moieties in the ionic domains promotes the biorecognition-driven assembly of lectins adding a new dimension to the capabilities of ionic self-assembly. © 2013 American Chemical Society.
author	Cortez, María Lorena Pallarola, Diego Andrés Battaglini, Fernando
author_facet	Cortez, María Lorena Pallarola, Diego Andrés Battaglini, Fernando
author_sort	Cortez, María Lorena
title	Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors
title_short	Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors
title_full	Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors
title_fullStr	Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors
title_full_unstemmed	Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors
title_sort	electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: its application to control substrate inhibition in horseradish peroxidase-based sensors
publishDate	2013
url	https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00032700_v85_n4_p2414_Cortez http://hdl.handle.net/20.500.12110/paper_00032700_v85_n4_p2414_Cortez
work_keys_str_mv	AT cortezmarialorena electrontransferpropertiesofdualselfassembledarchitecturesbasedonspecificrecognitionandelectrostaticdrivingforcesitsapplicationtocontrolsubstrateinhibitioninhorseradishperoxidasebasedsensors AT pallaroladiegoandres electrontransferpropertiesofdualselfassembledarchitecturesbasedonspecificrecognitionandelectrostaticdrivingforcesitsapplicationtocontrolsubstrateinhibitioninhorseradishperoxidasebasedsensors AT battaglinifernando electrontransferpropertiesofdualselfassembledarchitecturesbasedonspecificrecognitionandelectrostaticdrivingforcesitsapplicationtocontrolsubstrateinhibitioninhorseradishperoxidasebasedsensors
_version_	1768542864247095296

Electron transfer properties of dual self-assembled architectures based on specific recognition and electrostatic driving forces: Its application to control substrate inhibition in horseradish peroxidase-based sensors

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