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Fulltext Thixotropic Supramolecular Pectin-Poly(Ethylene Glycol) Methacrylate (PEGMA) Hydrogels

Chan SY, Choo WS, Young DJ, Loh XJ

Polymers (Basel), 2016 Nov 18;8(11).
PMID: 30974681 DOI: 10.3390/polym8110404

Pectin is an anionic, water-soluble polymer predominantly consisting of covalently 1,4-linked α-d-galacturonic acid units. This naturally occurring, renewable and biodegradable polymer is underutilized in polymer science due to its insolubility in organic solvents, which renders conventional polymerization methods impractical. To circumvent this problem, cerium-initiated radical polymerization was utilized to graft methoxy-poly(ethylene glycol) methacrylate (mPEGMA) onto pectin in water. The copolymers were characterized by ¹H nuclear magnetic resonance (NMR), Fourier transform infrared (FTIR) spectroscopy and thermogravimetric analysis (TGA), and used in the formation of supramolecular hydrogels through the addition of α-cyclodextrin (α-CD) to induce crosslinking. These hydrogels possessed thixotropic properties; shear-thinning to liquid upon agitation but settling into gels at rest. In contrast to most of the other hydrogels produced through the use of poly(ethylene glycol) (PEG)-grafted polymers, the pectin-PEGMA/α-CD hydrogels were unaffected by temperature changes.
Pectin as a rheology modifier: Origin, structure, commercial production and rheology

Chan SY, Choo WS, Young DJ, Loh XJ

Carbohydr Polym, 2017 Apr 01;161:118-139.
PMID: 28189220 DOI: 10.1016/j.carbpol.2016.12.033

Pectins are a diverse family of biopolymers with an anionic polysaccharide backbone of α-1,4-linked d-galacturonic acids in common. They have been widely used as emulsifiers, gelling agents, glazing agents, stabilizers, and/or thickeners in food, pharmaceutical, personal care and polymer products. Commercial pectin is classified as high methoxy pectin (HMP) with a degree of methylation (DM) >50% and low methoxy pectin (LMP) with a DM <50%. Amidated low methoxy pectins (ALMP) can be obtained through aminolysis of HMP. Gelation of HMP occurs by cross-linking through hydrogen bonds and hydrophobic forces between the methyl groups, assisted by a high co-solute concentration and low pH. In contrast, gelation of LMP occurs by the formation of ionic linkages via calcium bridges between two carboxyl groups from two different chains in close proximity, known as the 'egg-box' model. Pectin gels exhibit Newtonian behaviour at low shear rates and shear-thinning behaviour when the shear rate is increased. An overview of pectin from its origin to its physicochemical properties is presented in this review.
Recent Advances in Shape Memory Soft Materials for Biomedical Applications

Chan BQ, Low ZW, Heng SJ, Chan SY, Owh C, Loh XJ

ACS Appl Mater Interfaces, 2016 04 27;8(16):10070-87.
PMID: 27018814 DOI: 10.1021/acsami.6b01295

Shape memory polymers (SMPs) are smart and adaptive materials able to recover their shape through an external stimulus. This functionality, combined with the good biocompatibility of polymers, has garnered much interest for biomedical applications. In this review, we discuss the design considerations critical to the successful integration of SMPs for use in vivo. We also highlight recent work on three classes of SMPs: shape memory polymers and blends, shape memory polymer composites, and shape memory hydrogels. These developments open the possibility of incorporating SMPs into device design, which can lead to vast technological improvements in the biomedical field.
Nanoparticle-Hydrogel Composites: Concept, Design, and Applications of These Promising, Multi-Functional Materials

Thoniyot P, Tan MJ, Karim AA, Young DJ, Loh XJ

Adv Sci (Weinh), 2015 02;2(1-2):1400010.
PMID: 27980900

New technologies rely on the development of new materials, and these may simply be the innovative combination of known components. The structural combination of a polymer hydrogel network with a nanoparticle (metals, non-metals, metal oxides, and polymeric moieties) holds the promise of providing superior functionality to the composite material with applications in diverse fields, including catalysis, electronics, bio-sensing, drug delivery, nano-medicine, and environmental remediation. This mixing may result in a synergistic property enhancement of each component: for example, the mechanical strength of the hydrogel and concomitantly decrease aggregation of the nanoparticles. These mutual benefits and the associated potential applications have seen a surge of interest in the past decade from multi-disciplinary research groups. Recent advances in nanoparticle-hydrogel composites are herein reviewed with a focus on their synthesis, design, potential applications, and the inherent challenges accompanying these exciting materials.
Unprecedented Acid-Promoted Polymerization and Gelation of Acrylamide: A Serendipitous Discovery

Chan SY, Goh SS, Dou Q, Chan BQY, Choo WS, Young DJ, et al.

Chem Asian J, 2018 Jun 20.
PMID: 29924504 DOI: 10.1002/asia.201800552

Dilute acid polymerizes degassed, aqueous acrylamide with concomitant gelation, without the need for added free radical initiator or cross-linking agent. This reaction is accelerated by sonication or UV irradiation, but inhibited by adventitious oxygen or the addition of a free radical inhibitor, suggesting an acid-accelerated free radical process. The resulting hydrogels are thixotropic in nature and partially disrupted by the addition of chaotropic agents, indicating the importance of hydrogen bonding to the 3D network. This discovery was made while trying to prepare pectin-polyacrylamide hydrogels. We observed that pectin initiated the gelation of acrylamide, but only if the aqueous pectin samples had a pH lower than ca. 5.
Fulltext Electrospun Pectin-Polyhydroxybutyrate Nanofibers for Retinal Tissue Engineering

Chan SY, Chan BQY, Liu Z, Parikh BH, Zhang K, Lin Q, et al.

ACS Omega, 2017 Dec 31;2(12):8959-8968.
PMID: 30023596 DOI: 10.1021/acsomega.7b01604

Natural polysaccharide pectin has for the first time been grafted with polyhydroxybutyrate (PHB) via ring-opening polymerization of β-butyrolactone. This copolymer, pectin-polyhydroxybutyrate (pec-PHB), was blended with PHB in various proportions and electrospun to produce nanofibers that exhibited uniform and bead-free nanostructures, suggesting the miscibility of PHB and pec-PHB. These nanofiber blends exhibited reduced fiber diameters from 499 to 336-426 nm and water contact angles from 123.8 to 88.2° on incorporation of pec-PHB. They also displayed 39-335% enhancement of elongation at break relative to pristine PHB nanofibers. pec-PHB nanofibers were found to be noncytotoxic and biocompatible. Human retinal pigmented epithelium (ARPE-19) cells were seeded onto pristine PHB and pec-PHB nanofibers as scaffold and showed good proliferation. Higher proportions of pec-PHB (pec-PHB10 and pec-PHB20) yielded higher densities of cells with similar characteristics to normal RPE cells. We propose, therefore, that nanofibers of pec-PHB have significant potential as retinal tissue engineering scaffold materials.
Fulltext Antimicrobial quaternary ammonium organosilane cross-linked nanofibrous collagen scaffolds for tissue engineering

Dhand C, Balakrishnan Y, Ong ST, Dwivedi N, Venugopal JR, Harini S, et al.

Int J Nanomedicine, 2018;13:4473-4492.
PMID: 30122921 DOI: 10.2147/IJN.S159770

Introduction: In search for cross-linkers with multifunctional characteristics, the present work investigated the utility of quaternary ammonium organosilane (QOS) as a potential cross-linker for electrospun collagen nanofibers. We hypothesized that the quaternary ammonium ions improve the electrospinnability by reducing the surface tension and confer antimicrobial properties, while the formation of siloxane after alkaline hydrolysis could cross-link collagen and stimulate cell proliferation.
Materials and methods: QOS collagen nanofibers were electrospun by incorporating various concentrations of QOS (0.1%-10% w/w) and were cross-linked in situ after exposure to ammonium carbonate. The QOS cross-linked scaffolds were characterized and their biological properties were evaluated in terms of their biocompatibility, cellular adhesion and metabolic activity for primary human dermal fibroblasts and human fetal osteoblasts.
Results and discussion: The study revealed that 1) QOS cross-linking increased the flexibility of otherwise rigid collagen nanofibers and improved the thermal stability; 2) QOS cross-linked mats displayed potent antibacterial activity and 3) the biocompatibility of the composite mats depended on the amount of QOS present in dope solution - at low QOS concentrations (0.1% w/w), the mats promoted mammalian cell proliferation and growth, whereas at higher QOS concentrations, cytotoxic effect was observed.
Conclusion: This study demonstrates that QOS cross-linked mats possess anti-infective properties and confer niches for cellular growth and proliferation, thus offering a useful approach, which is important for hard and soft tissue engineering and regenerative medicine.