Auto-catalytic redox polymerisation using nanoceria and glucose oxidase for double network hydrogels
File(s)
Accepted version
Author(s)
Mohammed, Ali A
Pinna, Alessandra
Li, Siwei
Sang, Tian
Jones, Julian R
Type
Journal Article
Abstract
A novel auto-catalytic reaction, a combination of naturally occurring enzyme glucose oxidase (GOx) and amine-functionalised cerium oxide nanoparticles (nanoceria), was employed for open vessel free radical polymerisation of double network hydrogels (DNHGs). The nanoceria also incorporated into the gels to enhance mechanical strength. GOx reduces atmospheric O2 to H2O2, causing a cyclic change of cerium ion states, resulting in propagating free radicals in the carbon group in the amino functionalised nanoceria surface. We synthesised novel nanocomposite DNHGs by grafting polymers onto amine-functionalised nanoceria (ANC), with poly(2-acrylamido-2-methylpropanesulfonic acid), PAMPS, and polyacrylamide (PAAm) in the first and second networks respectively. The graft polymerisation was initiated using the alternating cerium states on the ANC. GOx held two major roles within the reaction: to provide an oxygen free system, without any other form of degassing, and to provide cyclical cerium ion states between Ce4+ and Ce3+, creating new free radicals for polymerisation. Polymer conversion using ANC as the sole initiator in the presence of GOx resulted in 83% conversion for PAMPS and 64% PAAm. Polymers degassed only with argon resulted in less than 55% conversion for both PAAm and PAMPS, proving that the addition of GOx enhanced the reaction. The new gels (1.76 MPa) showed an order of magnitude improvement in mechanical properties compared to DNHG made without ANC/GOx (0.10 MPa).
Date Issued
2020-04-14
Date Acceptance
2020-03-06
Citation
Journal of Materials Chemistry B, 2020, 8 (14), pp.2834-2844
ISSN
2050-750X
Publisher
Royal Society of Chemistry
Start Page
2834
End Page
2844
Journal / Book Title
Journal of Materials Chemistry B
Volume
8
Issue
14
Copyright Statement
© The Royal Society of Chemistry 2020.
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000525489500007&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Technology
Materials Science, Biomaterials
Materials Science
HIGH MECHANICAL STRENGTH
SILICA NANOPARTICLES
CERIA NANOPARTICLES
RADICAL INITIATORS
CARTILAGE
GELS
CYTOTOXICITY
ANTIOXIDANT
INDUCTION
TOUGHNESS
Publication Status
Published
Date Publish Online
2020-03-06