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Title: Synthesis of polymer nanogels by electro-Fenton process: investigation of the effect of main operation parameters
Author: Lanzalaco, Sonia
Sirés Sadornil, Ignacio
Sabatino, Maria Antonietta
Dispenza, Clelia
Scialdone, Onofrio
Galia, Alessandro
Keywords: Oxidació electroquímica
Electrolytic oxidation
Issue Date: 19-Jun-2017
Publisher: Elsevier Ltd
Abstract: Recently, electro-Fenton (EF) process has been shown as a promising, facile, effective, low cost and environmentally-friendly alternative for synthesizing polymer nanogels suitable as biocompatible nanocarriers for emerging biomedical applications. Here, the electrochemically-assisted modification of poly(vinylpyrrolidone) (PVP) by EF process was studied to assess the role of key operation parameters for a precise modulation of polymer crosslinking and its functionalization with -COOH and succinimide groups. The dimensions of the nanogels, in terms of hydrodynamic radius (Rh) and weight-average molecular weight (Mw), can be tuned up by controlling the electrolysis time, current density (j) and PVP and Fe2+ concentrations, as demonstrated via dynamic and static light scattering and gel permeation chromatography analysis. Using PVP at 0.25 wt.%, Fe2+ at 0.5-1.0 mmol dm-3 and low j, short treatment times induced intramolecular crosslinking with chain scission, allowing size reduction of PVP particles from 24 to 9-10 nm. Longer reaction times and higher PVP and Fe2+ contents favored intermolecular crosslinking ending in Mw values higher than the initial 3.95×105 g mol-1. An excessive ¿OH dose from a too high circulated charge (Q), i.e., too prolonged electrolysis time even at low j or too high j even for short time, promoted intramolecular crosslinking (Rh ~ 10-12 nm) along with a very significant chain scission probably owing to the loss of mobility of the three-dimensional nanogel network. In conclusion, EF allowed transforming the architecture of linear, inert PVP chains into a functionalized nanogel with -COOH and succinimide groups that have great potential for further conjugation.
Note: Versió postprint del document publicat a:
It is part of: Electrochimica Acta, 2017, vol. 246, p. 812-822
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ISSN: 0013-4686
Appears in Collections:Articles publicats en revistes (Ciència dels Materials i Química Física)

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