Preparation and characterization of enzymatically cross-linked gelatin/cellulose nanocrystal composite hydrogels

Gelatin is an attractive hydrogel material because of its excellent biocompatibility and non-cytotoxicity, but poor mechanical properties of gelatin-based hydrogels become a big obstacle that limits their wide-spread application. To solve it, in this work, gelatin/cellulose nanocrystal composite hydrogels (Gel-TG-CNCs) were prepared using microbial transglutaminase (mTG) as the crosslinking catalyst and cellulose nanocrystals (CNCs) as reinforcements. The physicochemical properties of the composite hydrogels were investigated by thermogravimetric analysis (TGA), X-ray diffraction (XRD) and scanning electron microscopy (SEM). The dynamic rheological measurement and uniaxial compression test were performed to study the effects of mTG and CNC contents on the storage modulus and breaking strength of the as-prepared Gel-TG-CNCs. Results showed that the addition of CNCs and mTG could significantly increase the storage modulus and breaking strength of gelatin-based hydrogels, especially when added simultaneously. The breaking strength of Gel-TG-CNCs (2%) at 25 °C can reach 1000 g which is 30 times greater than pure gelatin hydrogels. The biocompatibility of the composite hydrogels was also investigated by the MTT method with Hela cells, and the results demonstrated that the composite hydrogels maintained excellent biocompatibility. With a combination of good biocompatibility and mechanical properties, the as-prepared Gel-TG-CNCs showed potential application value in the biomedical field.

[1]  Xianhai Zeng,et al.  Cellulose nanocrystalline hydrogel based on a choline chloride deep eutectic solvent as wearable strain sensor for human motion. , 2020, Carbohydrate polymers.

[2]  Sabu Thomas,et al.  Fabrication and functionalization of 3D-printed soft and hard scaffolds with growth factors for enhanced bioactivity , 2020, RSC advances.

[3]  Ya Liu,et al.  Research status of self-healing hydrogel for wound management: A review. , 2020, International journal of biological macromolecules.

[4]  A. Boccaccini,et al.  Ionically and Enzymatically Dual Cross-Linked Oxidized Alginate Gelatin Hydrogels with Tunable Stiffness and Degradation Behavior for Tissue Engineering. , 2020, ACS biomaterials science & engineering.

[5]  Y. Tabata,et al.  Gelatin hydrogel membrane containing carbonate hydroxyapatite for nerve regeneration scaffold. , 2020, Journal of biomedical materials research. Part A.

[6]  M. Sobczak,et al.  Hydrogel-Based Active Substance Release Systems for Cosmetology and Dermatology Application: A Review , 2020, Pharmaceutics.

[7]  Anjali Jayakumar,et al.  Hydrogels for Medical and Environmental Applications , 2020 .

[8]  M. G. Karthih,et al.  Fabrication and characterization of chitosan based collagen/ gelatin composite scaffolds from big eye snapper Priacanthus hamrur skin for antimicrobial and anti oxidant applications. , 2020, Materials science & engineering. C, Materials for biological applications.

[9]  Q. Wang,et al.  Enzymatic crosslinking of silk sericin through combined use of TGase and the custom peptide , 2020, The Journal of The Textile Institute.

[10]  W. N. Chen,et al.  Eco-friendly and biodegradable cellulose hydrogels produced from low cost okara: towards non-toxic flexible electronics , 2019, Scientific Reports.

[11]  Ana F. Lourenço,et al.  Enzymatic nanocellulose in papermaking - The key role as filler flocculant and strengthening agent. , 2019, Carbohydrate polymers.

[12]  Hongcan Shi,et al.  Preparation of cellulose nanocrystal/oxidized dextran/gelatin (CNC/OD/GEL) hydrogels and fabrication of a CNC/OD/GEL scaffold by 3D printing , 2019, Journal of Materials Science.

[13]  Xianli Liu,et al.  Nanomaterials and plants: Positive effects, toxicity and the remediation of metal and metalloid pollution in soil. , 2019, The Science of the total environment.

[14]  Feng-qin Feng,et al.  Study on wettability, mechanical property and biocompatibility of electrospun gelatin/zein nanofibers cross-linked by glucose , 2019, Food Hydrocolloids.

[15]  Qinghua Xu,et al.  Fabrication of Cellulose Nanocrystal/Chitosan Hydrogel for Controlled Drug Release , 2019, Nanomaterials.

[16]  Fangqing Yin,et al.  Preparation and properties of cellulose nanocrystals, gelatin, hyaluronic acid composite hydrogel as wound dressing , 2019, Journal of biomaterials science. Polymer edition.

[17]  A. Akbarzadeh,et al.  Fabrication and in Vitro Evaluation of Nanocomposite Hydrogel Scaffolds Based on Gelatin/PCL–PEG–PCL for Cartilage Tissue Engineering , 2019, ACS Omega.

[18]  Haiyang Yang,et al.  A photo-degradable injectable self-healing hydrogel based on star poly(ethylene glycol)-b-polypeptide as a potential pharmaceuticals delivery carrier. , 2018, Soft matter.

[19]  Rafael A. Garcia,et al.  Chemical and Enzymatic Protein Cross-Linking To Improve Flocculant Properties , 2018, ACS Sustainable Chemistry & Engineering.

[20]  H. Ding,et al.  The influence of particles size and its distribution on the degree of stress concentration in particulate reinforced metal matrix composites , 2018, Materials Science and Engineering: A.

[21]  He Liu,et al.  A functional chitosan-based hydrogel as a wound dressing and drug delivery system in the treatment of wound healing , 2018, RSC advances.

[22]  K. Haraguchi,et al.  Nanocomposite hydrogel as a template for synthesis of mono and bimetallic nanoparticles , 2018 .

[23]  N. Bahramifar,et al.  Surface chemical functionalization of cellulose nanocrystals by 3-aminopropyltriethoxysilane. , 2018, International journal of biological macromolecules.

[24]  Wenhang Wang,et al.  Mechanical reinforcement of gelatin hydrogel with nanofiber cellulose as a function of percolation concentration. , 2017, International journal of biological macromolecules.

[25]  Todd Hoare,et al.  Review of Hydrogels and Aerogels Containing Nanocellulose , 2017 .

[26]  M. Amin,et al.  Cellulose nanocrystals extracted from rice husks as a reinforcing material in gelatin hydrogels for use in controlled drug delivery systems , 2016 .

[27]  Fei Liu,et al.  Tailoring physical properties of transglutaminase-modified gelatin films by varying drying temperature , 2016 .

[28]  Z. Shao,et al.  Multi-responsive polyethylene-polyamine/gelatin hydrogel induced by non-covalent interactions , 2016 .

[29]  S. Ismail,et al.  Carbon Nanotubes (CNTs) Nanocomposite Hydrogels Developed for Various Applications: A Critical Review , 2016, Journal of Inorganic and Organometallic Polymers and Materials.

[30]  C. Xue,et al.  Modification of Gelatine with Galla chinensis Extract, a Natural Crosslinker , 2016 .

[31]  Biqiong Chen,et al.  One-pot synthesis and characterization of reduced graphene oxide–gelatin nanocomposite hydrogels , 2016 .

[32]  S. Benjakul,et al.  Characteristics and gel properties of gelatin from skin of seabass (Lates calcarifer) as influenced by extraction conditions. , 2014, Food chemistry.

[33]  M. Shafiee,et al.  Studies on Glutaraldehyde Crosslinked Chitosan Hydrogel Properties for Drug Delivery Systems , 2013 .

[34]  A. Ragauskas,et al.  Improving the mechanical and thermal properties of gelatin hydrogels cross-linked by cellulose nanowhiskers. , 2013, Carbohydrate polymers.

[35]  Xiaoquan Yang,et al.  Characterization of gelatin-based edible films incorporated with olive oil , 2012 .

[36]  A. Khademhosseini,et al.  Carbon nanotube reinforced hybrid microgels as scaffold materials for cell encapsulation. , 2012, ACS nano.

[37]  Øyvind Weiby Gregersen,et al.  Rheological Studies of Microfibrillar Cellulose Water Dispersions , 2011 .

[38]  Min Kyoon Shin,et al.  Nanocomposite Hydrogel with High Toughness for Bioactuators , 2009 .

[39]  H. Bohidar,et al.  Swelling and de-swelling kinetics of gelatin hydrogels in ethanol-water marginal solvent. , 2006, International journal of biological macromolecules.

[40]  A. Bigi,et al.  Relationship between triple-helix content and mechanical properties of gelatin films. , 2004, Biomaterials.

[41]  Seeram Ramakrishna,et al.  Electrospinning and mechanical characterization of gelatin nanofibers , 2004 .

[42]  D. Ejima,et al.  Crystal Structure of Microbial Transglutaminase fromStreptoverticillium mobaraense * , 2002, The Journal of Biological Chemistry.