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COLLOIDS AND SURFACES B-BIOINTERFACES · 2018 · IF 3.997

An injectable enzymatically crosslinked tyramine-modified carboxymethyl chitin hydrogel for biomedical applications

Bo Bi,Hui Liu,Wenting Kang,Renxi Zhuo,Xulin Jiang

The in-situ forming injectable hydrogels have received much attention as scaffolds in the biomedical field, providing a minimally invasive surgical procedure to fill the damaged area. In the present work, carboxymethyl chitin (CMCH) synthesized homogenously was further functionalized with tyramine , resulted in a new injectable enzymatically crosslinked in-situ forming hydrogel under physiological conditions. This new tyramine-modified carboxymethyl chitin (CMCH-Tyr) hydrogel showed much better mechanical properties than those of the thermosensitive in-situ forming physical-crosslinking CMCH hydrogel. The CMCH-Tyr hydrogels remained stable under physiological conditions and could be degraded by lysozyme. The gelation time, strength and biodegradation rate of the CMCH-Tyr hydrogels can be adjusted by varying the concentrations of the horseradish peroxidase and H 2 O 2 in the certain range. In vitro cytotoxicity assays and in vivo in-situ injection study showed non-toxicity, favorable gel formation, and good tissue biocompatibility of the enzyme-catalyzed CMCH-Tyr hydrogel. Thus, the biodegradable and biocompatible CMCH-Tyr hydrogels may hold great potential for three dimensional cell culture and tissue engineering.

研究领域: 生物医学工程 · 组织工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2020 · IF 5.162

Laccase-mediated construction of flexible double-network hydrogels based on silk fibroin and tyramine-modified hyaluronic acid

Lin Wang,Bo Xu,Yelin Nong,Ping Wang,Yuanyuan Yu,Chao Deng,Jiugang Yuan,Qiang Wang

Silk fibroin (SF) is a promising biomaterial with attractive properties, however, the practical applications of pure regenerated SF materials were severely restricted by their poor water retention and low elasticity. In this study, a tyramine-modified hyaluronic acid (mHA) was introduced to SF chains, followed by constructing double-network hydrogels via laccase-mediated crosslinking of SF and mHA. Mechanism of the enzymatic coupling reaction between SF and mHA was investigated using the model compounds. The morphology, mechanical property, and swelling behavior of SF-g-mHA hydrogel were evaluated. The results reveal that combination use of SF and mHA endowed the obtained hydrogels with high structural stability, improved mechanical properties and drug release behavior, which overcame the intrinsically poor formability of the pure fibroin hydrogels. This work provides a novel method to construct a double-network hydrogel with high flexibility and toughness, and expands the application range of the SF-based materials in biomedical fields.

研究领域: 生物材料学 · 生物医药工程
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AUSTRALIAN JOURNAL OF CHEMISTRY · 2023 ·Vol. 76 ·期 2 ·88-99 · IF 1.1

Injectable hydrogels of enzyme-catalyzed cross-linked tyramine-modified gelatin for drug delivery

Yuanhan Tang,Junjie Ding,Xun Zhou,Xintao Ma,Yi Zhao,Qiyu Mu,Zixu Huang,Qian Tao,Fangjie Liu,Ling Wang

Enzymatically catalyzed cross-linking is a hydrogel fabrication method that generally is considered to have lower cytotoxicity than traditional chemical cross-linking methods. In order to optimize the properties of injectable hydrogels and expand their applications, an enzyme-catalyzed cross-linked injectable hydrogel was designed. The tyramine-modified gelatin (G-T) was formed into a stable injectable hydrogel by the combination of horseradish peroxidase (HRP) and hydrogen peroxide (H2O2) catalysis. 1H NMR spectroscopy was used to demonstrate the successful modification of gelatin by tyramine. The surface morphology of the prepared hydrogels was characterized jointly by atomic force microscopy (AFM) and scanning electron microscopy (SEM). Rheological tests demonstrated the tunable mechanical strength, formation kinetics, shear thinning and good self-recovery properties of the hydrogels. In addition, the hydrogels can be formed into various shapes by injection. The hydrogel network structure is complex and interlaced, as such it is suitable to encapsulate drugs for controlled release. The drug release from the prepared hydrogels followed the Peppas–Sahlin model and belonged to Fickian diffusion. This study constructed injectable hydrogels through the enzyme-catalyzed cross-linking of modified gelatin and applied the hydrogels for drug release, which is expected to expand the application in biomedical fields.

研究领域: 生物材料学 · 药物递送系统 · 组织工程
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Biomedical Materials · 2022 ·Vol. 18 ·期 1 ·015006 · IF 4.103

Enzymatically crosslinked hydrogel based on tyramine modified gelatin and sialylated chitosan

Peng Ding,Qianqian Wei,Ning Tian,Xiaoyue Ding,Ling Wang,Bin Wang,Oseweuba Valentine Okoro,Amin Shavandi,Lei Nie

The enzymatically crosslinked hydrogel could replicate the cellular microenvironment for biomedical applications. In the present study, to improve the cytocompatibility of chitosan (CS), sialic acid (SA) was introduced to CS to synthesize sialylated CS (CS-SA), and the tyramine (TA) was grafted to gelatin (G) to obtain TA modified gelatin (G-TA). The successful synthesis of CS-SA and G-TA was confirmed using 1H NMR and UV–Vis absorption spectra. The interpenetrating polymer networks G-TA/CS-SA (GC) hydrogel was then fabricated via blending G-TA and CS-SA solutions and crosslinked using horseradish peroxidase. The storage modulus (G') of the fabricated GC hydrogels with different ratios of G-TA/CS-SA greatly varied during the formation and strain of hydrogels. With the increase of CS-SA concentration from 0% to 2%, the storage modulus of GC hydrogels was also observed to decrease from 1500 Pa to 101 Pa; the water uptake capacity of GC hydrogels increased from 1000% to 4500%. Additionally, the cell counting kit-8 and fluorescent images demonstrated the excellent cytocompatibility of GC hydrogels after culturing with NIH 3T3 cells. The obtained results indicated that the fabricated GC hydrogels might have potential in biomedical fields, such as wound dressing.

研究领域: 生物材料学 · 组织工程学 · 再生医学
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Nano Today · 2021 · IF 20.722

Chinese herb-crosslinked hydrogel bearing rBMSCs-laden polyzwitterion microgels: Self-adaptive manipulation of micromilieu and stemness maintenance for restoring infarcted myocardium

Yang Liu,Xiaoping Zhang,Tengling Wu,Bo Liu,Jianhai Yang,Wenguang Liu

Injectable hydrogels and stem cells have been increasingly applied to treat myocardial infarction (MI). However, the harsh microenvironment adversely affects the survival of implanted stem cells and ultimate therapeutic outcomes. Herein, we design and prepare rat bone marrow mesenchymal stem cells (rBMSCs)-embedded polyzwitterionic microgels ( [email protected] ) via in situ Michael addition reaction between multivinyl carboxybetaine macromonomer and thiol-ended polyethylene glycol mixed with rBMSCs in a microfluidic system. The [email protected] are then loaded into a tyramine-modified hyaluronic acid (HA-Tyr), into which Chinese herb puerarin (PUE) and horseradish peroxidase (HRP)/H 2 O 2 are added to catalyze inter-phenol crosslinks to form an injectable HA-Tyr-PUE hydrogel encapsulating [email protected] ( [email protected] @microgels). This [email protected] @microgels is injected into the infarct region of rats, where HA-Tyr-PUE hydrogel serves to favorably modulate the microenvironment by scavenging active oxygen and releasing oxygen, and rBMSCs remain stemness in highly hydrophilic microgels and exert a paracrine effect to facilitate anti-inflammation and angiogenesis . These concerted actions boost the highly efficient restoration of ventricular function and structure. The ROS-scavenging medicine-crosslinked biodegradable biomacromolecule hydrogel bearing stemness-maintained microgels can be expanded to diverse tissue engineering and regenerative medicine fields.

研究领域: 组织工程 · 再生医学 · 生物材料 · 干细胞治疗 · 心脏病学
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