Nanocomposite Hydrogels with Polymer Grafted Silica Nanoparticles, Using Glucose Oxidase

Nanocomposite hydrogels offer remarkable potential for applications in bone tissue engineering. They are synthesized through the chemical or physical crosslinking of polymers and nanomaterials, allowing for the enhancement of their behaviour by modifying the properties and compositions of the nanomaterials involved. However, their mechanical properties require further enhancement to meet the demands of bone tissue engineering. Here, we present an approach to improve the mechanical properties of nanocomposite hydrogels by incorporating polymer grafted silica nanoparticles into a double network inspired hydrogel (gSNP Gels). The gSNP Gels were synthesised via a graft polymerization process using a redox initiator. gSNP Gels were formed by grafting 2-acrylamido-2-methylpropanesulfonic acid (AMPS) as the first network gel followed by a sequential second network acrylamide (AAm) onto amine functionalized silica nanoparticles (ASNPs). We utilized glucose oxidase (GOx) to create an oxygen-free atmosphere during polymerization, resulting in higher polymer conversion compared to argon degassing. The gSNP Gels showed excellent compressive strengths of 13.9 ± 5.5 MPa, a strain of 69.6 ± 6.4%, and a water content of 63.4% ± 1.8. The synthesis technique demonstrates a promising approach to enhance the mechanical properties of hydrogels, which can have significant implications for bone tissue engineering and other soft tissue applications.

[1]  A. Porter,et al.  3D printed superparamagnetic stimuli-responsive starfish-shaped hydrogels. , 2023, Heliyon.

[2]  Julian R. Jones,et al.  Double-Network Hydrogels Reinforced with Covalently Bonded Silica Nanoparticles via 1-Ethyl-3-(3-dimethylaminopropyl)carbodiimide Chemistry , 2022, ACS omega.

[3]  G. Sena,et al.  3D printing nanocomposite hydrogels with lattice vascular networks using stereolithography , 2021, Journal of Materials Research.

[4]  Julian R. Jones,et al.  Cobalt‐containing spherical glass nanoparticles for therapeutic ion release , 2021 .

[5]  Hongyu Liu,et al.  Crucial roles of graphene oxide in preparing alginate/nanofibrillated cellulose double network composites hydrogels. , 2021, Chemosphere.

[6]  Julian R. Jones,et al.  Nanoceria provides antioxidant and osteogenic properties to mesoporous silica nanoparticles for osteoporosis treatment. , 2020, Acta biomaterialia.

[7]  R. Pei,et al.  Nanocomposite hydrogels for tissue engineering applications. , 2020, Nanoscale.

[8]  Julian R. Jones,et al.  Biodegradable zinc-containing mesoporous silica nanoparticles for cancer therapy , 2020, Materials Today Advances.

[9]  M. Maggini,et al.  Fulleropyrrolidine-functionalized ceria nanoparticles as a tethered dual nanosystem with improved antioxidant properties , 2020, Nanoscale advances.

[10]  Julian R. Jones,et al.  Auto-catalytic redox polymerisation using nanoceria and glucose oxidase for double network hydrogels. , 2020, Journal of materials chemistry. B.

[11]  Xiaojing Wang,et al.  Characterizations of absorption, scattering, and transmission of typical nanoparticles and their suspensions , 2020 .

[12]  S. Ramakrishna,et al.  Insight Into the Current Directions in Functionalized Nanocomposite Hydrogels , 2020, Frontiers in Materials.

[13]  F. Boccafoschi,et al.  Overview of natural hydrogels for regenerative medicine applications , 2019, Journal of Materials Science: Materials in Medicine.

[14]  Julian R. Jones,et al.  Open vessel free radical photopolymerization of double network gels for biomaterial applications using glucose oxidase , 2019, Journal of Materials Chemistry B.

[15]  A. Schäfer,et al.  3D bioprinting of triphasic nanocomposite hydrogels and scaffolds for cell adhesion and migration , 2019, Biofabrication.

[16]  P. Ma,et al.  Stimuli-Responsive Conductive Nanocomposite Hydrogels with High Stretchability, Self-Healing, Adhesiveness, and 3D Printability for Human Motion Sensing. , 2019, ACS applied materials & interfaces.

[17]  H. Mirzadeh,et al.  A review on nanocomposite hydrogels and their biomedical applications , 2019, Science and Engineering of Composite Materials.

[18]  Tairong Kuang,et al.  Double network hydrogel for tissue engineering. , 2018, Wiley interdisciplinary reviews. Nanomedicine and nanobiotechnology.

[19]  M. Nair,et al.  Nanocomposite Hydrogels: Advances in Nanofillers Used for Nanomedicine , 2018, Gels.

[20]  Shawn A. Chester,et al.  Printing ferromagnetic domains for untethered fast-transforming soft materials , 2018, Nature.

[21]  T. Rantalainen,et al.  Mechanical basis of bone strength: influence of bone material, bone structure and muscle action , 2017, Journal of musculoskeletal & neuronal interactions.

[22]  Ali Khademhosseini,et al.  Advances in engineering hydrogels , 2017, Science.

[23]  Yonghong Deng,et al.  One‐Pot Fabrication of a Novel Agar‐Polyacrylamide/Graphene Oxide Nanocomposite Double Network Hydrogel with High Mechanical Properties   , 2016 .

[24]  M. Villanueva,et al.  Antimicrobial Activity of Starch Hydrogel Incorporated with Copper Nanoparticles. , 2016, ACS applied materials & interfaces.

[25]  Julian R. Jones,et al.  Controlling particle size in the Stöber process and incorporation of calcium. , 2016, Journal of colloid and interface science.

[26]  Jie Zheng,et al.  Fundamentals of double network hydrogels. , 2015, Journal of materials chemistry. B.

[27]  V. Khutoryanskiy,et al.  Biomedical applications of hydrogels: A review of patents and commercial products , 2015 .

[28]  Hai Wang,et al.  The role of soft colloidal templates in the shape evolution of flower-like MgAl-LDH hierarchical microstructures , 2015 .

[29]  G. Galleri,et al.  Ceria nanoparticles for the treatment of Parkinson-like diseases induced by chronic manganese intoxication , 2015 .

[30]  M. Stevens,et al.  Highly Controlled Open Vessel RAFT Polymerizations by Enzyme Degassing , 2014 .

[31]  M. Stevens,et al.  Polymerization amplified detection for nanoparticle-based biosensing. , 2014, Nano letters.

[32]  Qiuyu Zhang,et al.  Atomic oxygen resistance of polyimide/silicon hybrid thin films with different compositions and architectures , 2014 .

[33]  Jian Ping Gong,et al.  Physical hydrogels composed of polyampholytes demonstrate high toughness and viscoelasticity. , 2013, Nature materials.

[34]  C. Liao,et al.  Hydrogels for biomedical applications. , 2013 .

[35]  Hsu-Tung Lu Synthesis and characterization of amino-functionalized silica nanoparticles , 2013, Colloid Journal.

[36]  R. Amal,et al.  Cellular uptake and activity of heparin functionalised cerium oxide nanoparticles in monocytes. , 2013, Biomaterials.

[37]  Bo Xu,et al.  Nanocomposite hydrogels with high strength cross-linked by titania , 2013 .

[38]  Yasuaki Tokudome,et al.  Combining top-down and bottom-up routes for fabrication of mesoporous titania films containing ceria nanoparticles for free radical scavenging. , 2013, ACS applied materials & interfaces.

[39]  R. Sun,et al.  Studies on the properties and formation mechanism of flexible nanocomposite hydrogels from cellulose nanocrystals and poly(acrylic acid) , 2012 .

[40]  M. Abdollahi,et al.  Modification of silica nanoparticles with hydrophilic sulfonated polymers by using surface-initiated redox polymerization , 2012, Iranian Polymer Journal.

[41]  Jun Fu,et al.  Super-tough double-network hydrogels reinforced by covalently compositing with silica-nanoparticles , 2012 .

[42]  Jason T. George,et al.  Thermoresponsive nanocomposite double network hydrogels. , 2012, Soft matter.

[43]  T. Kurokawa,et al.  Induction of Spontaneous Hyaline Cartilage Regeneration Using a Double-Network Gel , 2011, The American journal of sports medicine.

[44]  T. Quinn,et al.  Reinforcement with cellulose nanocrystals of poly(vinyl alcohol) hydrogels prepared by cyclic freezing and thawing , 2011 .

[45]  Brad J Berron,et al.  Glucose Oxidase-Mediated Polymerization as a Platform for Dual-Mode Signal Amplification and Biodetection , 2011, Biotechnology and bioengineering.

[46]  Molly M Stevens,et al.  Spherical bioactive glass particles and their interaction with human mesenchymal stem cells in vitro. , 2011, Biomaterials.

[47]  Shyni Varghese,et al.  PEG/clay nanocomposite hydrogel: a mechanically robust tissue engineering scaffold , 2010 .

[48]  Jian Ping Gong,et al.  Why are double network hydrogels so tough , 2010 .

[49]  A. Khademhosseini,et al.  Hydrogels in Regenerative Medicine , 2009, Advanced materials.

[50]  Mark W. Tibbitt,et al.  Hydrogels as extracellular matrix mimics for 3D cell culture. , 2009, Biotechnology and bioengineering.

[51]  M. Jafarzadeh,et al.  Synthesis of organo-functionalized nanosilica via a co-condensation modification using γ-aminopropyltriethoxysilane (APTES) , 2009 .

[52]  D. Kohane,et al.  HYDROGELS IN DRUG DELIVERY: PROGRESS AND CHALLENGES , 2008 .

[53]  Khalil-ur-Rahman,et al.  Thermal Characterization of Purified Glucose Oxidase from A Newly Isolated Aspergillus Niger UAF-1 , 2007, Journal of clinical biochemistry and nutrition.

[54]  Eunhye Kim,et al.  Surface modification of silica nanoparticles by UV-induced graft polymerization of methyl methacrylate. , 2005, Journal of colloid and interface science.

[55]  J. Jestin,et al.  Atom transfer radical polymerization from silica nanoparticles using the ‘grafting from’ method and structural study via small-angle neutron scattering , 2005 .

[56]  Gabriel Zoldák,et al.  Irreversible Thermal Denaturation of Glucose Oxidase from Aspergillus niger Is the Transition to the Denatured State with Residual Structure* , 2004, Journal of Biological Chemistry.

[57]  T. Kurokawa,et al.  Double‐Network Hydrogels with Extremely High Mechanical Strength , 2003 .

[58]  K. Gupta,et al.  Graft copolymerization of ethyl acrylate onto cellulose using ceric ammonium nitrate as initiator in aqueous medium. , 2002, Biomacromolecules.

[59]  R E Guldberg,et al.  Mechanical properties of a novel PVA hydrogel in shear and unconfined compression. , 2001, Biomaterials.

[60]  Y. Ikada,et al.  Development of artificial articular cartilage , 2000, Proceedings of the Institution of Mechanical Engineers. Part H, Journal of engineering in medicine.

[61]  N. Manolova,et al.  Polyelectrolyte complex between chitosan and poly(2-acryloylamido-2-methylpropanesulfonic acid) , 1999 .

[62]  T. Patten,et al.  Preparation of Structurally Well-Defined Polymer−Nanoparticle Hybrids with Controlled/Living Radical Polymerizations , 1999 .

[63]  A. Mohammed Double network hydrogels for cartilage repair and their nanocomposite structure , 2017 .

[64]  T. Barder,et al.  Controlled Growth of Monodisperse Silica Spheres in the Micron Size Range , 2017 .

[65]  Ismail Ab Rahman,et al.  Synthesis of silica nanoparticles by sol-gel: size-dependent properties, surface modification, and applications in silica-polymer nanocomposites — a review , 2012 .

[66]  Chengjun Zhou,et al.  Application of rod-shaped cellulose nanocrystals in polyacrylamide hydrogels. , 2011, Journal of colloid and interface science.

[67]  Xiaofeng Wang,et al.  Fabrication of Hybrid Silica Nanoparticles Densely Grafted with Thermoresponsive Poly(N-isopropylacrylamide) Brushes of Controlled Thickness via Surface-Initiated Atom Transfer Radical Polymerization , 2008 .

[68]  W. Stöber,et al.  Controlled growth of monodisperse silica spheres in the micron size range , 1968 .