Uniform antibacterial cylindrical nanoparticles for enhancing the strength of nanocomposite hydrogels

Zehua Li; Amanda K. Pearce; Jianzhong Du; Andrew Dove; Rachel O'Reilly

doi:10.1002/pol.20210853

Uniform antibacterial cylindrical nanoparticles for enhancing the strength of nanocomposite hydrogels

Zehua Li, Amanda K. Pearce, Jianzhong Du, Andrew Dove, Rachel O'Reilly

Chemistry

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Abstract

Crystallization-driven self-assembly (CDSA) was employed for the preparation of monodisperse cationic cylindrical nanoparticles with controllable sizes, which were subsequently explored for their effect on antibacterial activity and the mechanical properties of nanocomposite hydrogels. Poly(ɛ-caprolactone)-block-poly(methyl methacrylate)-block-poly[2-(tert-butylamino) ethyl methacrylate] (PCL-b-PMMA-b-PTA) triblock copolymers were synthesized using combined ring-opening and RAFT polymerizations, and then self-assembled into polycationic cylindrical micelles with controllable lengths by epitaxial growth. The polycationic cylinders exhibited intrinsic cell-type-dependent antibacterial capabilities against gram-positive and gram-negative bacteria under physiological conditions, without quaternization or loading of any additional antibiotics. Furthermore, when the cylinders were combined into anionic alginate hydrogel networks, the mechanical response of the hydrogel composite was tunable and enhanced up to 51%, suggesting that cationic polymer fibers with controlled lengths are promising mimics of the fibrous structures in natural extracellular matrix to support scaffolds. Overall, this polymer fiber/hydrogel nanocomposite shows potential as an injectable antibacterial biomaterial, with possible application in implant materials as bacteriostatic agents or bactericides against various infections.

Original language	English
Journal	Journal of Polymer Science. Part A: Polymer Chemistry
Early online date	21 Feb 2022
DOIs	https://doi.org/10.1002/pol.20210853
Publication status	E-pub ahead of print - 21 Feb 2022

Bibliographical note

Funding Information:
China Scholarship Council; Education and Scientific Research Project of Shanghai, Grant/Award Number: 21520710100; National Outstanding Youth Science Fund Project of National Natural Science Foundation of China, Grant/Award Number: 21925505 Funding information

Funding Information:
The China Scholarship Council and the University of Warwick are acknowledged for a Joint Scholarship to Zehua Li. The 111 project, National Science Fund for Distinguished Young Scholars, NSFC (21925505), and Shanghai international scientific collaboration fund (21520710100) are acknowledged for the collaboration research. The authors are grateful to Dr. Jessica Blair and Helen McNeil for access, expert advice, and training in microbiology experiments.

Publisher Copyright:
© 2022 The Authors. Journal of Polymer Science published by Wiley Periodicals LLC.

Keywords

alginate hydrogels
antibacterial micelles
crystallization-driven self-assembly
nanocomposites

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Materials Chemistry
Polymers and Plastics

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10.1002/pol.20210853Licence: Creative Commons: Attribution (CC BY)

LiZ2022UniformFinal published version, 2.59 MBLicence: Creative Commons: Attribution (CC BY)

Cite this

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title = "Uniform antibacterial cylindrical nanoparticles for enhancing the strength of nanocomposite hydrogels",

abstract = "Crystallization-driven self-assembly (CDSA) was employed for the preparation of monodisperse cationic cylindrical nanoparticles with controllable sizes, which were subsequently explored for their effect on antibacterial activity and the mechanical properties of nanocomposite hydrogels. Poly(ɛ-caprolactone)-block-poly(methyl methacrylate)-block-poly[2-(tert-butylamino) ethyl methacrylate] (PCL-b-PMMA-b-PTA) triblock copolymers were synthesized using combined ring-opening and RAFT polymerizations, and then self-assembled into polycationic cylindrical micelles with controllable lengths by epitaxial growth. The polycationic cylinders exhibited intrinsic cell-type-dependent antibacterial capabilities against gram-positive and gram-negative bacteria under physiological conditions, without quaternization or loading of any additional antibiotics. Furthermore, when the cylinders were combined into anionic alginate hydrogel networks, the mechanical response of the hydrogel composite was tunable and enhanced up to 51%, suggesting that cationic polymer fibers with controlled lengths are promising mimics of the fibrous structures in natural extracellular matrix to support scaffolds. Overall, this polymer fiber/hydrogel nanocomposite shows potential as an injectable antibacterial biomaterial, with possible application in implant materials as bacteriostatic agents or bactericides against various infections.",

keywords = "alginate hydrogels, antibacterial micelles, crystallization-driven self-assembly, nanocomposites",

author = "Zehua Li and Pearce, {Amanda K.} and Jianzhong Du and Andrew Dove and Rachel O'Reilly",

note = "Funding Information: China Scholarship Council; Education and Scientific Research Project of Shanghai, Grant/Award Number: 21520710100; National Outstanding Youth Science Fund Project of National Natural Science Foundation of China, Grant/Award Number: 21925505 Funding information Funding Information: The China Scholarship Council and the University of Warwick are acknowledged for a Joint Scholarship to Zehua Li. The 111 project, National Science Fund for Distinguished Young Scholars, NSFC (21925505), and Shanghai international scientific collaboration fund (21520710100) are acknowledged for the collaboration research. The authors are grateful to Dr. Jessica Blair and Helen McNeil for access, expert advice, and training in microbiology experiments. Publisher Copyright: {\textcopyright} 2022 The Authors. Journal of Polymer Science published by Wiley Periodicals LLC.",

year = "2022",

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journal = "Journal of Polymer Science. Part A: Polymer Chemistry",

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AU - Li, Zehua

AU - Pearce, Amanda K.

AU - Du, Jianzhong

AU - Dove, Andrew

AU - O'Reilly, Rachel

N1 - Funding Information: China Scholarship Council; Education and Scientific Research Project of Shanghai, Grant/Award Number: 21520710100; National Outstanding Youth Science Fund Project of National Natural Science Foundation of China, Grant/Award Number: 21925505 Funding information Funding Information: The China Scholarship Council and the University of Warwick are acknowledged for a Joint Scholarship to Zehua Li. The 111 project, National Science Fund for Distinguished Young Scholars, NSFC (21925505), and Shanghai international scientific collaboration fund (21520710100) are acknowledged for the collaboration research. The authors are grateful to Dr. Jessica Blair and Helen McNeil for access, expert advice, and training in microbiology experiments. Publisher Copyright: © 2022 The Authors. Journal of Polymer Science published by Wiley Periodicals LLC.

PY - 2022/2/21

Y1 - 2022/2/21

N2 - Crystallization-driven self-assembly (CDSA) was employed for the preparation of monodisperse cationic cylindrical nanoparticles with controllable sizes, which were subsequently explored for their effect on antibacterial activity and the mechanical properties of nanocomposite hydrogels. Poly(ɛ-caprolactone)-block-poly(methyl methacrylate)-block-poly[2-(tert-butylamino) ethyl methacrylate] (PCL-b-PMMA-b-PTA) triblock copolymers were synthesized using combined ring-opening and RAFT polymerizations, and then self-assembled into polycationic cylindrical micelles with controllable lengths by epitaxial growth. The polycationic cylinders exhibited intrinsic cell-type-dependent antibacterial capabilities against gram-positive and gram-negative bacteria under physiological conditions, without quaternization or loading of any additional antibiotics. Furthermore, when the cylinders were combined into anionic alginate hydrogel networks, the mechanical response of the hydrogel composite was tunable and enhanced up to 51%, suggesting that cationic polymer fibers with controlled lengths are promising mimics of the fibrous structures in natural extracellular matrix to support scaffolds. Overall, this polymer fiber/hydrogel nanocomposite shows potential as an injectable antibacterial biomaterial, with possible application in implant materials as bacteriostatic agents or bactericides against various infections.

AB - Crystallization-driven self-assembly (CDSA) was employed for the preparation of monodisperse cationic cylindrical nanoparticles with controllable sizes, which were subsequently explored for their effect on antibacterial activity and the mechanical properties of nanocomposite hydrogels. Poly(ɛ-caprolactone)-block-poly(methyl methacrylate)-block-poly[2-(tert-butylamino) ethyl methacrylate] (PCL-b-PMMA-b-PTA) triblock copolymers were synthesized using combined ring-opening and RAFT polymerizations, and then self-assembled into polycationic cylindrical micelles with controllable lengths by epitaxial growth. The polycationic cylinders exhibited intrinsic cell-type-dependent antibacterial capabilities against gram-positive and gram-negative bacteria under physiological conditions, without quaternization or loading of any additional antibiotics. Furthermore, when the cylinders were combined into anionic alginate hydrogel networks, the mechanical response of the hydrogel composite was tunable and enhanced up to 51%, suggesting that cationic polymer fibers with controlled lengths are promising mimics of the fibrous structures in natural extracellular matrix to support scaffolds. Overall, this polymer fiber/hydrogel nanocomposite shows potential as an injectable antibacterial biomaterial, with possible application in implant materials as bacteriostatic agents or bactericides against various infections.

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ER -

Uniform antibacterial cylindrical nanoparticles for enhancing the strength of nanocomposite hydrogels

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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