Although hydrogels have been widely studied because of their satisfactory biocompatibility and plasticity, their application is limited in bone tissue engineering (BTE) owing to their inadequate mechanical properties and absence of osteogenic activity. To address this issue, we developed an updated alendronate (ALN)-Ca²⁺/Mg²⁺-doped supramolecular (CMS) hydrogel based on our previously developed mechanically resilient “host-guest macromer” (HGM) hydrogel to improve the hydrogel's mechanical properties and osteogenic activity. The CMS hydrogel was prepared by introducing a new physical crosslinking comprising the strong chelation of the comonomer acrylate alendronate (Ac-ALN) and Ca²⁺/Mg²⁺ in the HGM hydrogel. Compared with the previously developed HGM hydrogel, the upgraded CMS hydrogel presented better mechanical properties because of the additional physical crosslinking, while possessing injectable and self-healing properties like the HGM hydrogel. Moreover, the addition of Ac-ALN and Ca²⁺/Mg²⁺ also effectively promoted the in vitro proliferation, migration, and osteogenic differentiation of bone marrow-derived stem cells. The healing effect of a rat cranial defect further proved that the in vivo bone regeneration ability of CMS hydrogel was better than that of HGM hydrogel. The updated CMS hydrogel shows significant potential for BTE application.

尽管水凝胶因其令人满意的生物相容性和可塑性而被广泛研究，但由于其机械性能不足且缺乏成骨活性，其在骨组织工程（BTE）中的应用受到限制。为了解决这个问题，我们基于我们之前开发的机械弹性“主客体大分子单体”（HGM）水凝胶，开发了一种更新的阿仑膦酸钠（ALN）-Ca ²⁺ /Mg ²⁺掺杂超分子（CMS）水凝胶，以提高水凝胶的机械性能特性和成骨活性。 CMS水凝胶是通过在HGM水凝胶中引入一种新的物理交联来制备的，该物理交联包括共聚单体丙烯酸酯阿仑膦酸盐(Ac-ALN)和Ca ²⁺ /Mg ²⁺的强螯合。与之前开发的HGM水凝胶相比，升级后的CMS水凝胶由于额外的物理交联而呈现出更好的机械性能，同时具有像HGM水凝胶一样的可注射和自修复性能。此外，Ac-ALN和Ca ²⁺ /Mg ²⁺的添加也有效促进骨髓干细胞的体外增殖、迁移和成骨分化。大鼠颅骨缺损的愈合效果进一步证明CMS水凝胶的体内骨再生能力优于HGM水凝胶。更新后的 CMS 水凝胶显示出 BTE 应用的巨大潜力。