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Recyclable magnetic nanoparticles grafted with antimicrobial metallopolymer-antibiotic bioconjugates.

ABSTRACT: Over-prescription and improper use of antibiotics has led to the emergence of bacterial resistance, posing a major threat to public health. There has been significant interest in the development of alternative therapies and agents to combat antibiotic resistance. We report the preparation of recyclable magnetic iron oxide nanoparticles grafted with charged cobaltocenium-containing metallopolymers by surface-initiated reversible addition-fragmentation chain transfer (RAFT) polymerization. ?-Lactam antibiotics were then conjugated with metallopolymers to enhance their vitality against both Gram-positive and Gram-negative bacteria. The enhanced antibacterial activity was a result of synergy of antimicrobial segments that facilitate the inhibition of hydrolysis of antibiotics and local enhancement of antibiotic concentration on a nanoparticle surface. These magnetic nanoparticles can be recycled numerous times without losing the initial antimicrobial potency. Studies suggested negligible toxicity of metallopolymer-grafted nanoparticles to red blood cells and minimal tendency to induce resistance in bacteria.

SUBMITTER: Pageni P

PROVIDER: S-EPMC6054821 | biostudies-literature | 2018 Sep

REPOSITORIES: biostudies-literature

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Recyclable magnetic nanoparticles grafted with antimicrobial metallopolymer-antibiotic bioconjugates.

Pageni Parasmani P Yang Peng P Bam Marpe M Zhu Tianyu T Chen Yung Pin YP Decho Alan W AW Nagarkatti Mitzi M Tang Chuanbing C

Biomaterials 20180503

Over-prescription and improper use of antibiotics has led to the emergence of bacterial resistance, posing a major threat to public health. There has been significant interest in the development of alternative therapies and agents to combat antibiotic resistance. We report the preparation of recyclable magnetic iron oxide nanoparticles grafted with charged cobaltocenium-containing metallopolymers by surface-initiated reversible addition-fragmentation chain transfer (RAFT) polymerization. β-Lacta ...[more]

PMID: 29759729

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Project description:Here we report the construction and characterization of a recoverable, thermoresponsive polymer-endoglucanase bioconjugate that matches the activity of unmodified enzymes on insoluble cellulose substrates. Two copolymers exhibiting a thermoresponsive lower critical solution temperature (LCST) were created through the copolymerization of an aminooxy-bearing methacrylamide with N-isopropylacrylamide (NIPAm) or N-isopropylmethacrylamide (NIPMa). The aminooxy group provided a handle through which the LCST was adjusted through small-molecule quenching. This allowed materials with LCSTs ranging from 20.9 to 60.5 °C to be readily obtained after polymerization. The thermostable endoglucanase EGPh from the hypothermophilic Pyrococcus horikoshii was transaminated with pyridoxal-5'-phosphate to produce a ketone-bearing protein, which was then site-selectively modified through oxime linkage with benzylalkoxyamine or 5 kDa-poly(ethylene glycol)-alkoxyamine. These modified proteins showed activity comparable to the controls when assayed on an insoluble cellulosic substrate. Two polymer bioconjugates were then constructed using transaminated EGPh and the aminooxy-bearing copolymers. After 12 h, both bioconjugates produced an equivalent amount of free reducing sugars as the unmodified control using insoluble cellulose as a substrate. The recycling ability of the NIPAm copolymer-EGPh conjugate was determined through three rounds of activity, maintaining over 60% activity after two cycles of reuse and affording significantly more soluble carbohydrates than unmodified enzyme alone. When assayed on acid-pretreated Miscanthus, this bioconjugate increased the amount of reducing sugars by 2.8-fold over three rounds of activity. The synthetic strategy of this bioconjugate allows the LCST of the material to be changed readily from a common stock of copolymer and the method of attachment is applicable to a variety of proteins, enabling the same approach to be amenable to thermophile-derived cellulases or to the separation of multiple species using polymers with different recovery temperatures.

Dataset Information

Recyclable magnetic nanoparticles grafted with antimicrobial metallopolymer-antibiotic bioconjugates.

Publications

Recyclable magnetic nanoparticles grafted with antimicrobial metallopolymer-antibiotic bioconjugates.

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