Digital Light Processing (DLP) offers the potential for personalized bone implants. Within this method, the interfacial bonding capacity of inorganic/organic materials and the solid-phase content of the slurry emerge as primary factors influencing scaffolds mechanical properties. In this research, KH571 was applied to establish an interfacial “molecular bridge”, adopting in situ coupling technology to forge stable covalent bonds between calcium silicate (CSi) and KH571. Chemical grafting, surface photografting, and photopolymerization techniques were then utilized to construct a photo-crosslinked network by CSi-KH571-TMPTA/HDDA slurry, thereby transforming the weak physical connections at the interface into strong chemical bonds. Consequently, the curing capacity and mechanical properties of the scaffolds were enhanced. Further control grain size, crystal phase transition, and shrinkage of CSi-KH571 scaffolds, post-treatment sintering processes were employed, resulting in scaffolds with a high content of β-CSi. Moreover, the optimal process parameters were selected concerning grafting rate, chemical composition, microscopic morphology, crystalline transformation, dimensional accuracy, mechanical properties, biodegradability and biocompatibility of CSi-KH571. The elastic modulus and compressive properties of CSi25-55 scaffolds exhibited a notable improvement of 29.71 % and 59.30 %, respectively, compared to CSi-50 scaffolds. By regulating the phase composition of CSi, CSi25-55 scaffolds were designed to possess a controllable degradation. In vitro cell culture experiments validated its excellent biocompatibility and promoted the proliferation and differentiation of bone marrow mesenchymal stem cells (BMSCs) as well as the deposition of bone matrix. Herein, a novel and sustainable approach has been promoted for enhancing the interfacial bonding capacity of inorganic/organic materials and the solid-phase content of printing slurry, which lays the foundation for the printing of high-resolution degradable bioceramic scaffolds.
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