The phosphorylated noncollagenous proteins (NCPs) play a vital role in manipulating biomineralization, while the mechanism of phosphorylation of NCPs in intrafibrillar mineralization of collagen fibril has not been completely deciphered. Poly(vinylphosphonic acid) (PVPA) and sodium trimetaphosphate (STMP) as templating analogs of NCPs induce hierarchical mineralization in cooperation with indispensable sequestration analogs such as polyacrylic acid (PAA) via polymer-induced liquid-like precursor (PILP) process. Herein, STMP-Ca and PVPA-Ca complexes are proposed to achieve rapid intrafibrillar mineralization through polyelectrolyte-Ca complexes pre-precursor (PCCP) process. This strategy is further verified effectively for remineralization of demineralized dentin matrix both in vitro and in vivo. Although STMP micromolecule fails to stabilize amorphous calcium phosphate (ACP) precursor, STMP-Ca complexes facilely permeate into intrafibrillar interstices and trigger phase transition of ACP to hydroxyapatite within collagen. In contrast, PVPA-stabilized ACP precursors lack liquid-like characteristic and crystallize outside collagen due to rigid conformation of PVPA macromolecule, while PVPA-Ca complexes infiltrate into partial intrafibrillar intervals under electrostatic attraction and osmotic pressure as evidenced by intuitionistic 3D stochastic optical reconstruction microscopy (3D-STORM). The study not only extends the variety and size range of polyelectrolyte for PCCP process but also sheds light on the role of phosphorylation for NCPs in biomineralization.
The rise of antibiotic resistance necessitates the development of non-antibiotic antibacterial dressings with high biocompatibility and reliable wound-repair performance. In this work, chitosan/cellulose ether composite antibacterial membranes (CCE-ACM) were fabricated from chitosan, hydroxyethyl cellulose, and hydroxypropyl cellulose, and further reinforced through sodium trimetaphosphate (STMP) cross-linking. Response-surface optimization enabled the construction of a compact phosphodiester-linked network with improved mechanical strength, controlled swelling behavior, and stable moisture regulation. The membranes exhibited excellent cytocompatibility (> 80% viability) and strong antibacterial activity against Escherichia coli and Staphylococcus aureus , with the optimized CHEPCS formulation showing the most pronounced inhibition. In vivo, CCE-ACM significantly accelerated wound closure, achieving near-complete healing by Day 15 and promoting reduced inflammation, enhanced re-epithelialization, and more mature collagen deposition. These results demonstrate that the optimized CHEPCS membrane integrates effective antibacterial activity, favorable biocompatibility, and enhanced wound-healing performance, representing a promising non-antibiotic dressing for advanced wound care applications.
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