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Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization

Polymer-grafted nanomaterials based on carbon allotropes and their derivatives (graphene oxide (GO), etc.) are typically prepared by successive reaction stages that depend upon the initial functionalities in the nanostructure and the polymerization type needed for grafting. However, due to the multi...

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Autores principales: Noriega-Navarro, Roxana, Castro-Medina, Jésica, Escárcega-Bobadilla, Martha V., Zelada-Guillén, Gustavo A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7221901/
https://www.ncbi.nlm.nih.gov/pubmed/32230739
http://dx.doi.org/10.3390/nano10040614
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author Noriega-Navarro, Roxana
Castro-Medina, Jésica
Escárcega-Bobadilla, Martha V.
Zelada-Guillén, Gustavo A.
author_facet Noriega-Navarro, Roxana
Castro-Medina, Jésica
Escárcega-Bobadilla, Martha V.
Zelada-Guillén, Gustavo A.
author_sort Noriega-Navarro, Roxana
collection PubMed
description Polymer-grafted nanomaterials based on carbon allotropes and their derivatives (graphene oxide (GO), etc.) are typically prepared by successive reaction stages that depend upon the initial functionalities in the nanostructure and the polymerization type needed for grafting. However, due to the multiple variables involved in the functionalization steps, it is commonly difficult to predict the properties in the final product and to correlate the material history with its final performance. In this work, we explored the steps needed to graft the carboxylic acid moieties in GO (COOH@GO) with a pH-sensitive polymer, poly[2-(diethylamino)ethyl methacrylate] (poly[DEAEMA]), varying the reactant ratios at each stage prior to polymerization. We studied the combinatorial relationship between these variables and the behavior of the novel grafted material GO-g-poly[DEAEMA], in terms of swelling ratio vs. pH (%Q) in solid specimens and potentiometric response vs. Log[H(+)] in a solid-state sensor format. We first introduced N-hydroxysuccinimide (NHS)-ester moieties at the –COOH groups (GO-g-NHS) by a classical activation with N-ethyl-N′-(3-dimethylaminopropyl)carbodiimide (EDC). Then, we substituted the NHS-ester groups by polymerizable amide-linked acrylic moieties using 2-aminoethyl methacrylate (AEMA) at different ratios to finally introduce the polymer chains via radical polymerization in an excess of DEAEMA monomer. We found correlated trends in swelling pH range, interval of maximum and minimum swelling values, response in potentiometry and potentiometric linear range vs. Log[H(+)] and could establish their relationship with the combinatorial stoichiometries in synthetic stages.
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spelling pubmed-72219012020-05-22 Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization Noriega-Navarro, Roxana Castro-Medina, Jésica Escárcega-Bobadilla, Martha V. Zelada-Guillén, Gustavo A. Nanomaterials (Basel) Article Polymer-grafted nanomaterials based on carbon allotropes and their derivatives (graphene oxide (GO), etc.) are typically prepared by successive reaction stages that depend upon the initial functionalities in the nanostructure and the polymerization type needed for grafting. However, due to the multiple variables involved in the functionalization steps, it is commonly difficult to predict the properties in the final product and to correlate the material history with its final performance. In this work, we explored the steps needed to graft the carboxylic acid moieties in GO (COOH@GO) with a pH-sensitive polymer, poly[2-(diethylamino)ethyl methacrylate] (poly[DEAEMA]), varying the reactant ratios at each stage prior to polymerization. We studied the combinatorial relationship between these variables and the behavior of the novel grafted material GO-g-poly[DEAEMA], in terms of swelling ratio vs. pH (%Q) in solid specimens and potentiometric response vs. Log[H(+)] in a solid-state sensor format. We first introduced N-hydroxysuccinimide (NHS)-ester moieties at the –COOH groups (GO-g-NHS) by a classical activation with N-ethyl-N′-(3-dimethylaminopropyl)carbodiimide (EDC). Then, we substituted the NHS-ester groups by polymerizable amide-linked acrylic moieties using 2-aminoethyl methacrylate (AEMA) at different ratios to finally introduce the polymer chains via radical polymerization in an excess of DEAEMA monomer. We found correlated trends in swelling pH range, interval of maximum and minimum swelling values, response in potentiometry and potentiometric linear range vs. Log[H(+)] and could establish their relationship with the combinatorial stoichiometries in synthetic stages. MDPI 2020-03-27 /pmc/articles/PMC7221901/ /pubmed/32230739 http://dx.doi.org/10.3390/nano10040614 Text en © 2020 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Noriega-Navarro, Roxana
Castro-Medina, Jésica
Escárcega-Bobadilla, Martha V.
Zelada-Guillén, Gustavo A.
Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization
title Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization
title_full Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization
title_fullStr Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization
title_full_unstemmed Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization
title_short Control of pH-Responsiveness in Graphene Oxide Grafted with Poly-DEAEMA via Tailored Functionalization
title_sort control of ph-responsiveness in graphene oxide grafted with poly-deaema via tailored functionalization
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7221901/
https://www.ncbi.nlm.nih.gov/pubmed/32230739
http://dx.doi.org/10.3390/nano10040614
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