Facile Preparation of Polymer-Grafted Halloysite Nanotubes via a Redox System: a Novel Approach to Construct Antibacteri
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Article www.springer.com/13233 pISSN 1598-5032 eISSN 2092-7673
Facile Preparation of Polymer-Grafted Halloysite Nanotubes via a Redox System: a Novel Approach to Construct Antibacterial Hydrogel Yanfang Ma1 Zhihang Zhao2 Boyan Tang2 Yonggang Wu2 Hailei Zhang*,2
1 2
Shijiazhuang Institute of Railway Technology, Shijiazhuang, P. R. China College of Chemistry and Environmental Science, Hebei University, Baoding, P. R. China
Received February 15, 2020 / Revised May 18, 2020 / Accepted June 1, 2020
Abstract: We demonstrate the use of a supernormal valence transition-metal (Ce(IV) and Cu(III))-mediated redox system for the surface grafting on the halloysite nanotubes (HNTs). Following this way, commonly-used vinyl monomers were grafted on HNTs in one step under mild condition. The grafting was evidenced using FTIR, X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). The micromorphology was carefully characterized by transmission electron microscope (TEM). The results indicate that the surface grafting reaction was successfully processed in all cases, in which the Ce(IV) shows a much higher initiation activity than that of Cu(III). Then a uniform hydrogel was constructed by mixing poly(triethyl(4-vinylbenzyl)phosphonium chloride-grafted HNTs (HNTs-P(Et-P)) with sodium polyacrylate-grafted HNTs (HNTs-P(AA-Na)), which show desirable antibacterial activity. Keywords: halloysite nanotubes, clay, surface grafting, hydrogel, antibacterial.
1. Introduction In past decades, clay material has drawn an increasing attention in the field of polymer composites.1-3 Among them, halloysite nanotube (HNT) occupies a special place owing to the favorable tubular structure, which exhibit good aerodynamic and hydrodynamic properties and better processability than that of sphere, rod and plate materials.4-6 Like other nanoscale tubular materials, e.g., carbon nanotubes, halloysite nanotubes (HNTs) share a similar geometry, but exhibit many excellent advantages such as biocompatibility, environmental friendliness, as well as lowcost and widely spreadable properties.7-9 Generally, the internal surface of HNTs consists of a gibbsite octahedral array (Al-OH) groups, whereas the siloxane groups (Si-O-Si) mainly overspread on the external surface.10 Owing to the curving structure and hydrolysis effect, a small amount of -OH groups also exist on external surface of HNTs.11 The -OH groups allows various chemical modification methods upon HNTs.12,13 Especially, the surface modification would generate functionalized or active groups onto HNTs, provide HNTs with advanced architectures and thereby open up broader applications including catalysis,14-16 anticorrosion,17 adsorbent,18-21 drug delivery,3,22-26 enzyme immobilization,27,28 flameresistant material,29 pigment,30 rubber filler,31,32 and so on.33,34 For example, Takahara and coworkers developed a surface initiating atom transfer radical polymerization (SI-ATRP) method to give polymethyl methacrylate-filled HNTs through a pre-modification of HNTs with dopamine derivativ
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