Developing double-crosslinking 3D printed hydrogels for bone tissue engineering

IF 4.5 3区 工程技术 Q1 CHEMISTRY, APPLIED
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Abstract

Bone defects are one of the main causes of disability worldwide. Due to the disadvantages associated with autografts, the latest advances have been focused on tissue regeneration approaches that use injectable hydrogels or 3D printed hydrogel-based structures that could refill appropriately the bone gap area without the need for external fixatives, leading to bone formation in the long term. Injectable hydrogels could be applied in extrusion-based 3D printing as inks; in this sense, double-crosslinking hydrogels appear as ideal candidates. In this work, injectable and printable double crosslinkable hydrogels based on oxidized xanthan gum (XGox) and methacrylate polyaspartylhydrazide (PAHy-MA) were produced. The formation of dynamic hydrazone bonds, occurring between aldehyde groups on the polysaccharide backbone and hydrazine moieties of PAHy-MA, induced an instant gelation, conferring, also, injectability and self-healing properties to the hydrogels. The presence of methacrylic moieties on the synthetic polymer allowed further crosslinking upon UV irradiation that stabilized the hydrogel shape and mitigated its susceptibility to hydrolytic degradation. Obtained hydrogels showed pseudoplastic behaviour and good recovery of viscoelastic properties over time. The physicochemical and rheological characterization highlighted increased stability and higher viscoelastic moduli after photo-crosslinking. The hydrogels also showed good printability, cytocompatibility and the early formation of a bone-like matrix when osteosarcoma-derived cells (MG-63) were cultured in the scaffolds for 21 days, with an increased collagen I deposition, mineralization and the expression of characteristic osteogenic markers.

Abstract Image

开发用于骨组织工程的双交联三维打印水凝胶
骨缺损是导致全球残疾的主要原因之一。由于自体移植的缺点,最新进展集中在使用可注射水凝胶或基于三维打印的水凝胶结构的组织再生方法上,这种方法可以在不需要外部固定剂的情况下适当填充骨缺损区域,从而实现长期的骨形成。可注射水凝胶可作为油墨应用于挤压式三维打印;从这个意义上讲,双交联水凝胶似乎是理想的候选材料。在这项工作中,制备了基于氧化黄原胶(XGox)和甲基丙烯酸酯聚天冬氨酰肼(PAHy-MA)的可注射和可打印双交联水凝胶。多糖骨架上的醛基团与 PAHy-MA 的肼基团之间形成的动态腙键诱导了瞬间凝胶化,同时赋予了水凝胶可注射性和自愈性。合成聚合物上甲基丙烯酸分子的存在使其在紫外线照射下进一步交联,从而稳定了水凝胶的形状,并降低了其水解降解的敏感性。获得的水凝胶表现出假塑性,随着时间的推移粘弹性能恢复良好。物理化学和流变学特征突出表明,光交联后的水凝胶稳定性增强,粘弹性模量提高。当骨肉瘤衍生细胞(MG-63)在支架中培养 21 天后,水凝胶还显示出良好的可印刷性、细胞相容性和类骨基质的早期形成,胶原 I 沉积、矿化和特征成骨标志物的表达均有所增加。
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来源期刊
Reactive & Functional Polymers
Reactive & Functional Polymers 工程技术-高分子科学
CiteScore
8.90
自引率
5.90%
发文量
259
审稿时长
27 days
期刊介绍: Reactive & Functional Polymers provides a forum to disseminate original ideas, concepts and developments in the science and technology of polymers with functional groups, which impart specific chemical reactivity or physical, chemical, structural, biological, and pharmacological functionality. The scope covers organic polymers, acting for instance as reagents, catalysts, templates, ion-exchangers, selective sorbents, chelating or antimicrobial agents, drug carriers, sensors, membranes, and hydrogels. This also includes reactive cross-linkable prepolymers and high-performance thermosetting polymers, natural or degradable polymers, conducting polymers, and porous polymers. Original research articles must contain thorough molecular and material characterization data on synthesis of the above polymers in combination with their applications. Applications include but are not limited to catalysis, water or effluent treatment, separations and recovery, electronics and information storage, energy conversion, encapsulation, or adhesion.
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