Engineering Research Center of Special Engineering Plastics, Ministry of Education, College of Chemistry, Jilin University, Changchun, 130012, China.
The First Hospital of Jilin University, Changchun, 130021, China.
Adv Mater. 2024 Oct;36(40):e2406227. doi: 10.1002/adma.202406227. Epub 2024 Aug 21.
Addressing osteoporosis-related bone defects, a supramolecular strategy is innovated for modifying carbon fiber reinforced polyether ether ketone (CF/PEEK) composites. By covalently attaching intelligent macromolecules via in situ RAFT polymerization, leveraging the unique pathological microenvironment in patients with iron-overloaded osteoporosis, intelligent supramolecular modified implant surface possesses multiple endogenous modulation capabilities. After implantation, surface brush-like macromolecules initially resist macrophage adhesion, thereby reducing the level of immune inflammation. Over time, the molecular chains undergo conformational changes due to Fe (III) mediated supramolecular self-assembly, transforming into mechanistic signals. These signals are then specifically transmitted to pre-osteoblast cell through the binding capacity of the KRSR short peptide at the molecular terminus, induced their osteogenic differentiation via the YAP/β-catenin signaling axis. Furthermore, osteoblasts secrete alkaline phosphatase (ALP), which significantly hydrolyzes phosphate ester bonds in surface macromolecular side groups, resulting in the release of alendronate (ALN). This process further improves the local osteoporotic microenvironment. This intelligent surface modification tailors bone repair to individual conditions, automatically realize multiple endogenous regulation once implanted, and truly realize spontaneous activation of a series of responses conducive to bone repair in vivo. It is evidenced by improved bone regeneration in iron-overloaded osteoporotic rabbits and supported by in vitro validations.
针对骨质疏松相关的骨缺损问题，我们创新性地提出了一种超分子策略，用于对碳纤维增强聚醚醚酮（CF/PEEK）复合材料进行改性。通过通过原位 RAFT 聚合将智能大分子共价连接到复合材料表面，利用铁过载骨质疏松症患者特有的病理微环境，智能超分子改性植入物表面具有多种内源性调节能力。植入后，表面刷状大分子最初可抵抗巨噬细胞黏附，从而降低免疫炎症水平。随着时间的推移，由于 Fe(III)介导的超分子自组装，分子链发生构象变化，转化为机械信号。这些信号通过分子末端的 KRSR 短肽的结合能力特异性传递到成前体细胞，通过 YAP/β-catenin 信号通路诱导其成骨分化。此外，成骨细胞分泌碱性磷酸酶（ALP），其可显著水解表面大分子侧基中的磷酸酯键，导致阿仑膦酸钠（ALN）的释放。这一过程进一步改善了局部骨质疏松微环境。这种智能表面改性可根据个体情况定制骨修复，植入后自动实现多种内源性调节，真正实现了一系列有利于体内骨修复的自发激活反应。铁过载骨质疏松兔的骨再生改善情况为这一策略提供了证据支持，体外验证也证实了其有效性。
