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Open AccessArticle

Surface Functionalization by Stimuli-Sensitive Microgels for Effective Enzyme Uptake and Rational Design of Biosensor Setups

1
Department of Chemistry, M.V. Lomonosov Moscow State University, Leninskie Gory 1/3, 119991 Moscow, Russia
2
Leibniz-Institut für Polymerforschung Dresden e.V., Hohe Str. 6, 01069 Dresden, Germany
3
Institute of Physical Chemistry II, RWTH Aachen University, Landoltweg 2, 52056 Aachen, Germany
4
N.M. Emanuel Institute of Biochemical Physics, Russian Academy of Sciences, Kosygina Str. 4, 119334 Moscow, Russia
5
Physical Chemistry of Polymeric Materials, Technical University of Dresden, Hohe Str. 6, 01069 Dresden, Germany
*
Author to whom correspondence should be addressed.
Polymers 2018, 10(7), 791; https://doi.org/10.3390/polym10070791
Received: 24 May 2018 / Revised: 29 June 2018 / Accepted: 12 July 2018 / Published: 19 July 2018
(This article belongs to the Special Issue Microgels and Hydrogels at Interfaces)
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Abstract

We highlight microgel/enzyme thin films that were deposited onto solid interfaces via two sequential steps, the adsorption of temperature- and pH-sensitive microgels, followed by their complexation with the enzyme choline oxidase, ChO. Two kinds of functional (ionic) microgels were compared in this work in regard to their adsorptive behavior and interaction with ChO, that is, poly(N-isopropylacrylamide-co-N-(3-aminopropyl)methacrylamide), P(NIPAM-co-APMA), bearing primary amino groups, and poly(N-isopropylacrylamide-co-N-[3-(dimethylamino) propyl]methacrylamide), P(NIPAM-co-DMAPMA), bearing tertiary amino groups. The stimuli-sensitive properties of the microgels in the solution were characterized by potentiometric titration, dynamic light scattering (DLS), and laser microelectrophoresis. The peculiarities of the adsorptive behavior of both the microgels and the specific character of their interaction with ChO were revealed by a combination of surface characterization techniques. The surface charge was characterized by electrokinetic analysis (EKA) for the initial graphite surface and the same one after the subsequent deposition of the microgels and the enzyme under different adsorption regimes. The masses of wet microgel and microgel/enzyme films were determined by quartz crystal microbalance with dissipation monitoring (QCM-D) upon the subsequent deposition of the components under the same adsorption conditions, on a surface of gold-coated quartz crystals. Finally, the enzymatic responses of the microgel/enzyme films deposited on graphite electrodes to choline were tested amperometrically. The presence of functional primary amino groups in the P(NIPAM-co-APMA) microgel enables a covalent enzyme-to-microgel coupling via glutar aldehyde cross-linking, thereby resulting in a considerable improvement of the biosensor operational stability. View Full-Text
Keywords: microgel; stimuli-sensitivity; surface modification; adsorption; streaming potential; quartz crystal microbalance with dissipation monitoring; biosensor; choline oxidase; poly(N-isopropylacrylamide-co-N-(3-aminopropyl)methacrylamide); poly(N-isopropylacrylamide-co-N-[3-(dimethylamino)propyl]methacrylamide) microgel; stimuli-sensitivity; surface modification; adsorption; streaming potential; quartz crystal microbalance with dissipation monitoring; biosensor; choline oxidase; poly(N-isopropylacrylamide-co-N-(3-aminopropyl)methacrylamide); poly(N-isopropylacrylamide-co-N-[3-(dimethylamino)propyl]methacrylamide)
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).

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MDPI and ACS Style

Sigolaeva, L.V.; Pergushov, D.V.; Oelmann, M.; Schwarz, S.; Brugnoni, M.; Kurochkin, I.N.; Plamper, F.A.; Fery, A.; Richtering, W. Surface Functionalization by Stimuli-Sensitive Microgels for Effective Enzyme Uptake and Rational Design of Biosensor Setups. Polymers 2018, 10, 791.

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