A biomimetic mineralized dental cement with antibacterial-mineralization synergistic function and a preparation method and application thereof

Abstract

The application discloses a kind of biomimetic mineralization dental cement with antibacterial-mineralization synergistic function and its preparation method and application.The biomimetic mineralization dental cement is constituted by solid phase system and liquid phase system:the solid phase system includes calcium phosphate-based inorganic particles and the antibacterial polysaccharide functional layer in situ constructed on the surface thereof by hydrogen bond and electrostatic interaction;the liquid phase system is ion-regulated solution containing complexing component.Antibacterial polysaccharide is induced to participate in mineral phase growth in solidification process by pre-composite process, and forms biological mineralization composite structure, so as to realize antibacterial and mineralization functions simultaneously.The material is in the form of injectable paste, and the solidification time can be adjusted within 5-240 min, the compressive strength after solidification reaches 5-30 MPa, and it has good X-ray resistance, biocompatibility and broad-spectrum antibacterial performance.The biomimetic mineralization dental cement of the application is suitable for dental root canal filling, tooth remineralization repair and periodontal tissue repair and other fields.

Description

TECHNICAL FIELD

[0001] The present application belongs to the technical field of biomedical materials, and particularly relates to a biomimetic mineralized dental cement with antibacterial-mineralization synergistic function and a preparation method and application thereof. BACKGROUND

[0002] Root canal therapy is the core treatment method for dental pulp disease and periapical disease, and its treatment effect largely depends on effective debridement, sufficient disinfection and dense and durable sealing effect of the root canal system. An ideal root canal sealing material not only needs to have excellent physical sealing performance to isolate re-infection, but also should have good biocompatibility, sustained antibacterial ability and active mineralization induction activity, thereby creating a favorable microenvironment for biological repair and regeneration of periapical tissue.

[0003] At present, the root canal sealers widely used in clinical mainly include two categories of resin-based and bioceramic-based, but both have obvious limitations. For example, the epoxy resin-based sealers represented by AH Plus in the United States may release unreacted monomers and other components in the early stage of curing, which has a potential cytotoxicity risk; more importantly, this kind of material is essentially biologically inert, cannot actively interact with host tissues, and has no ability to promote dentin remineralization or tissue regeneration (Clinical Oral Investigations, 25(3), 891-899). On the other hand, the calcium silicate-based bioceramic material represented by iRootSP in Canada, although its biocompatibility and bioactivity are significantly improved, its curing time is relatively long, and there is a risk of microleakage before complete hydration and curing, which may cause periapical inflammatory reaction (Clinical Oral Investigations (2023) 27:2969-2977). More notably, the existing sealers generally lack effective and persistent antibacterial ability, and cannot inhibit the residual microorganisms in the root canal (especially the biofilm in the deep dentin tubules), which easily leads to postoperative persistent infection, delayed healing and even treatment failure, often requiring retreatment (International Endodontic Journal, 44, 1102-1109, 2011).

[0004] To compensate for the lack of antibacterial performance of existing sealants, researchers have tried various modification strategies, such as incorporating antibiotics (such as metronidazole, ciprofloxacin) or antibacterial metal ions (such as silver ions, copper ions) into the material. These methods can improve the antibacterial effect in the short term, but also bring new problems: the abuse of antibiotics can easily lead to the generation of bacterial drug resistance; metal ions may be toxic to host cells while exerting antibacterial effects, and may interfere with the curing reaction and long-term stability of the material itself, leading to uncontrollable changes in its physical and chemical properties (such as curing time, mechanical strength) (Materials Today Chemistry, 17 (2020) 100299).

[0005] The process of biomineralization in nature provides an excellent model for the design of multifunctional biomaterials. Organisms precisely control the nucleation, growth and assembly of inorganic mineral ions through proteins, polysaccharides and other organic macromolecules, ultimately forming organic-inorganic composite materials with ordered structure, excellent mechanical properties and functional adaptation. Some natural polysaccharides not only have good adhesion and ductility, but also exhibit certain natural antibacterial properties, providing important biomimetic basis for the design of new multifunctional root canal sealing materials (Adv. Funct. Mater. 2019, 29, 1902783). However, existing research has mostly focused on simulating macroscopic structures or improving single properties (such as mechanical strength), and in the specific clinical scenario of root canal sealing, how to systematically coordinate and optimize long-term antibacterial, controllable curing, good injectability and active mineralization through material microstructure design remains a technical problem that has not been fully solved.

[0006] Therefore, there is an urgent need in the art to develop a new type of root canal sealing material that not only achieves the functional synergy of long-term antibacterial and active mineralization, but also achieves a good balance between the curing kinetics and injectability required for clinical operation, thereby fundamentally improving the long-term efficacy of root canal treatment. SUMMARY

[0007] To overcome the shortcomings of the prior art, the present application provides a biomimetic mineralized dental cement with antibacterial-mineralization synergistic function and its preparation method and application. By constructing a ternary synergistic structure of "calcium phosphate-based particles-antibacterial polysaccharide functional layer-ion regulated liquid phase", the antibacterial functional components participate in the nucleation and crystal growth regulation of the mineral phase in situ during the curing process of the material, realizing the coupling construction of antibacterial function and mineralization structure from the microstructure level.

[0008] The present application is realized by the following technical solutions:

[0009] A biomimetic mineralized dental cement with antibacterial-mineralization synergistic function, comprising a solid phase system and a liquid phase system.

[0010] The solid phase system comprises calcium phosphate-based inorganic particles, and an antibacterial polysaccharide functional layer stably combined on the surface of the calcium phosphate-based inorganic particles through hydrogen bonding and electrostatic interaction;

[0011] The liquid phase system is an ion-regulating solution containing a complexing component;

[0012] In the process of mixing the solid phase system with the liquid phase system and material solidification, the antibacterial polysaccharide functional layer participates in inducing nucleation and growth of calcium phosphate mineral phase, forming an organic thin film-platelet-shaped calcium phosphate composite structure of biological mineralization, so that the biomimetic mineralized dental cement has both antibacterial function and mineralization activity.

[0013] Preferably, the antibacterial polysaccharide functional layer is a continuous or semi-continuous nanoscale coating structure with a thickness of 10-200 nm.

[0014] Preferably, the calcium phosphate-based inorganic particles are selected from one or more of amorphous calcium phosphate, octacalcium phosphate, α-tricalcium phosphate, β-tricalcium phosphate, hydroxyapatite, and calcium dihydrogen phosphate.

[0015] Preferably, the ion-regulating solution comprises a complexing agent, and the complexing agent comprises sodium pyrophosphate.

[0016] Preferably, the antibacterial polysaccharide is mucin.

[0017] Preferably, the biomimetic mineralized dental cement is in the form of an injectable paste, and has a solidification time of 5-240 min and a compressive strength of 5-30 MPa after solidification.

[0018] Preferably, the biomimetic mineralized dental cement further comprises an X-ray blocking agent.

[0019] The above-mentioned method for preparing the biomimetic mineralized dental cement with antibacterial-mineralization synergistic function comprises the following steps:

[0020] Step 1) Pre-complexing the calcium phosphate-based inorganic particles with the antibacterial polysaccharide to form an antibacterial polysaccharide functional layer on the surface of the particles, and obtaining a functionalized solid phase system;

[0021] Step 2) Mixing the functionalized solid phase system obtained in step 1) with an ion-regulating solution containing a complexing component to form a uniform injectable paste.

[0022] Preferably, the solid-liquid ratio of the functionalized solid phase system to the ion-regulating solution in step 2) is 1:1.

[0023] The above-mentioned biomimetic mineralized dental cement with antibacterial-mineralization synergistic function is used in dental root canal filling, tooth remineralization repair, or periodontal tissue repair.

[0024] The beneficial effects of the present application are as follows:

[0025] (1) Unlike traditional simple physical mixing of antibacterial agents, the present application forms an "antibacterial polysaccharide functional layer" on the surface of calcium phosphate particles, which participates in and regulates the nucleation and growth of mineral phases in situ during solidification. The functional layer is deeply embedded and stably exists in the final mineralized composite structure, realizing the chemical / physical integration of the antibacterial component and the material matrix, thereby providing stable and persistent contact antibacterial effect, effectively avoiding the problems of premature release, loss or inactivation of antibacterial agents, and avoiding the risks of drug resistance and cytotoxicity caused by the addition of antibiotics or high concentrations of metal ions.

[0026] (2) The present application induces the formation of an organic film- sheet-like calcium phosphate composite microstructure (such as a layered-porous interwoven structure) with characteristics similar to biological mineralization through the interface regulation of the antibacterial polysaccharide functional layer. This multi-level ordered structure from nanometer to micrometer not only simulates the composition and construction method of natural hard tissues, improving the biocompatibility and recognition ability of the material, but also effectively enhances the mechanical interlocking and mechanical stability of the solidified material, enabling it to maintain good injectability while achieving the required compressive strength for clinical requirements.

[0027] (3) The ternary system of "solid phase-interface functional layer-liquid phase regulation" constructed by the present application, especially through the regulation of the type and concentration of complexing agents in the liquid phase, can flexibly and accurately regulate the solidification reaction kinetics without affecting the antibacterial and mineralization functions. The solidification time of the material can be designed within a wide range (5-240 min) according to different clinical operation requirements, significantly improving the clinical operation tolerance and applicability of the material.

[0028] (4) The material of the present application not only has excellent biocompatibility, but also has active mineralization induction ability due to its nature of biomimetic mineralization and continuous release of calcium and phosphate ions. This helps to promote the biological mineralization repair of periapical defect areas and form good physicochemical bonding with dentin, enhancing the sealing effect, providing positive biological stimulation for host tissue regeneration, and realizing the functional leap from "passive sealing" to "active repair".

[0029] (5) The material system of the present application is designed flexibly, suitable for various calcium phosphate raw materials, and can be easily endowed with excellent imaging performance by adding X-ray blocking agents, which is convenient for postoperative evaluation of filling quality. Its good injectability and anti-dispersion ensure smooth delivery and positioning in complex root canal systems. Therefore, the material of the present application is not only suitable for conventional root canal filling, but also can be extended to the fields of tooth tissue remineralization repair and apical barrier preparation, with broad application prospects.

[0030] (6) The preparation method of the application is characterized by "pre-composite" construction of functional solid phase, simple steps, mild conditions, no need for complex and expensive equipment, and wide source of raw materials and high biological safety. The whole process is stable and reliable, easy to realize standardized and large-scale production, and has good industrial transformation potential. BRIEF DESCRIPTION OF DRAWINGS

[0031] Figure 1 X-ray diffraction (XRD) pattern of the biomimetic mineralized dental cement after solidification in Example 1;

[0032] Figure 2 Scanning electron microscope (SEM) image of the biomimetic mineralized dental cement after solidification in Example 1: A is 15 μm scale; B is 5 μm scale;

[0033] Figure 3 Antibacterial performance comparison result graph of materials with different antibacterial polysaccharide contents in Example 2;

[0034] Figure 4 Product microstructure image after replacing calcium phosphate dibasic with octacalcium phosphate (A), alpha-tricalcium phosphate (B) and beta-tricalcium phosphate (C) respectively in Example 3;

[0035] Figure 5 SEM image of agglomeration of calcium phosphate particles after physical mixing in Example 4;

[0036] Figure 6 Antibacterial performance comparison result graph of materials prepared by different methods in Example 4;

[0037] Figure 7 Anticollapse performance evaluation result graph of biomimetic mineralized dental cement in a simulated body fluid environment in Example 6;

[0038] Figure 8 X-ray diffraction (XRD) pattern of the biomimetic mineralized dental cement after solidification in Example 7 with X-ray blocking agent;

[0039] Figure 9 Cell toxicity detection results of each group of materials in Example 8;

[0040] Figure 10 X-ray image of the biomimetic mineralized dental cement for in vitro human tooth filling in Example 9. DETAILED DESCRIPTION

[0041] The application will be further described in detail below in combination with the drawings and specific examples.

[0042] The technical means used in the following examples are conventional means known to those skilled in the art, and the experimental methods not specified are conventional methods in the art.

[0043] The materials, reagents, etc. used in the following examples can be obtained from commercial channels unless otherwise specified.

[0044] Example 1 Preparation and performance characterization of antibacterial biomimetic mineralized dental cement

[0045] 1. Preparation of antibacterial biomimetic mineralized dental cement

[0046] A method for preparing a biomimetic mineralized dental cement with antibacterial-mineralization synergistic function, the specific steps are as follows:

[0047] (1) Take 5 g of calcium phosphate powder with particle size distribution of 10-100 μm and 5 g of amorphous calcium phosphate powder with particle size distribution of 10-200 nm as calcium phosphate-based inorganic particles.

[0048] (2) Take 1 g of mucin from bovine maxillary submandibular gland (as antibacterial polysaccharide) and dissolve it in 10 mL of deionized water to prepare a 1 wt% solution. Slowly add the Ca(H2PO4)2 powder and amorphous calcium phosphate powder to the solution, and stir at 37°C for 30 min to obtain functional solid powder with a mucin functional layer on the surface.

[0049] (3) Prepare the liquid phase system: dissolve 0.3 mol / L sodium pyrophosphate in deionized water as an ion regulating solution.

[0050] (4) Using a sterile spatula, mix the functional solid powder and ion regulating solution at a solid-liquid ratio (mass / volume) of 1:1 (g / mL) on the mixing plate to obtain a uniform and delicate injectable paste.

[0051] 2. Results and characterization

[0052] (1) Handling performance

[0053] The paste has good injectability and can be injected through a 30G (outer diameter 0.3 mm, inner diameter 0.15-0.16 mm) root canal injection needle.

[0054] (2) Curing performance

[0055] In an environment of 37℃ and 100% relative humidity, the initial and final setting times were measured using a Gilmore apparatus. The initial setting time was approximately 20 min, and the final setting time was approximately 45 min. The compressive strength of the cured material was tested using a universal testing machine at a loading rate of 0.5 mm / min, and the measured compressive strength was 28±5 MPa.

[0056] (3) Phase and structure

[0057] like Figure 1 As shown, XRD analysis revealed that the final product was dicalcium phosphate dihydrate, indicating that dicalcium phosphate reacted with amorphous calcium phosphate and solidified. Figure 2 As shown, scanning electron microscopy (SEM) observation revealed that the material has formed a multi-level biomineralized structure with interlaced lamellar calcium phosphate crystals and pores, and organic film-like substances are visible covering the surface of the lamellars.

[0058] (4) Antibacterial properties

[0059] The sample powder (0.2 g / mL) was mixed with Staphylococcus aureus bacterial suspension (1×10⁻⁶). 4 The bacterial suspension (CFU / mL) was co-cultured in a shaker at 37°C for 24 h. Then, 10 μL of the bacterial suspension was dropped onto a solid bacterial culture plate and spread evenly. After incubation at 37°C for 24 h, the plates were photographed and the colony count was performed.

[0060] A control group was also set up, containing 1×10⁻⁶ Staphylococcus aureus bacterial suspension. 4 The bacterial suspension (CFU / mL) was cultured alone in a shaker at 37°C for 24 h. Then, 10 μL of the bacterial suspension was dropped onto a solid bacterial culture plate and spread evenly. After incubation at 37°C for 24 h, the colonies were photographed and counted.

[0061] The results are as follows Figure 3 As shown, the antibacterial rate of the 1 wt% mucin content group was greater than 40% after 24 h.

[0062] Example 2: Effect of antibacterial polysaccharide content on material properties

[0063] 1. Experimental Procedure

[0064] Based on Example 1, the concentration of the mucin solution was changed so that the mucin loading in the final functionalized solid powder was 5 wt% and 10 wt% (relative to the total mass of Ca(H2PO4)2 and amorphous calcium phosphate). Subsequent testing methods were the same as in Example 1.

[0065] 2. Experimental Results and Analysis

[0066] With a mucin loading of 1–10 wt%, the materials can form a stable mineralized structure and maintain injectability.

[0067] like Figure 3 As shown, the antibacterial properties (against Staphylococcus aureus) of the material increase with increasing loading. At a loading of 5 wt%, the antibacterial performance is already very significant (>99%), and it has no negative impact on the material's curing time and compressive strength. At a loading of 10 wt%, it achieves complete antibacterial activity.

[0068] Example 3: Effects of different calcium-phosphorus systems on material properties

[0069] 1. Experimental Procedure

[0070] Based on Example 1, Ca(H2PO4)2 was replaced with the same molar amounts of octacalcium phosphate, α-tricalcium phosphate, and β-tricalcium phosphate, respectively. Subsequent testing methods were the same as in Example 1.

[0071] 2. Experimental Results and Analysis

[0072] The results are as follows Figure 4 As shown, different calcium-phosphorus systems can all form stable organic-inorganic composite structures, demonstrating good system compatibility. The compressive strengths of different calcium-phosphorus systems are shown in Table 1.

[0073] Table 1 Compressive strength of different calcium-phosphorus systems

[0074]

[0075] Example 4: Comparative Experiment (Physical Mixing Method)

[0076] 1. Experimental Procedure (Refer to Example 1)

[0077] (1) Weigh 50 g of Ca(H2PO4)2 powder from the same batch.

[0078] (2) Weigh 0.5 g of mucin dry powder (corresponding to the 1 wt% group in Example 1) and directly grind and mix it with Ca(H2PO4)2 powder in a mortar for 60 min.

[0079] (3) Mix the physically mixed powder with the same ion-regulating solution at a solid-liquid ratio of 1:1 to obtain a paste.

[0080] Subsequent testing methods are the same as in Example 1.

[0081] 2. Experimental Results and Analysis

[0082] (1) Dispersion

[0083] like Figure 5 As shown, SEM images reveal that physically mixed powders exhibit significant agglomeration after mixing in water, while powders pre-composite treated at the interface show uniform dispersion. Figure 2 ).

[0084] (2) Antibacterial properties

[0085] like Figure 6 As shown, under the same loading, the antibacterial performance of the material prepared by the physical mixing method is significantly lower than that of the material pre-composite treated with the interface, which confirms that only interface-bound antibacterial polysaccharides can achieve efficient and stable functionalization.

[0086] Example 5: Control of curing time

[0087] 1. Experimental Procedure

[0088] Based on the functionalized solid powder of Example 1, the concentration of sodium pyrophosphate in the ion-controlled solution was varied to 0 mol / L (control group), 0.1 mol / L, 0.3 mol / L (Example 1), and 0.5 mol / L. The powder was mixed at the same liquid-to-solid ratio, and the initial and final setting times were tested.

[0089] 2. Experimental Results and Analysis

[0090] As the sodium pyrophosphate concentration increased from 0 to 0.5 mol / L, the initial setting time of the material increased from approximately 5 min to 100 min, with a corresponding increase in the final setting time. This demonstrates that by adjusting the complexing agent concentration, the curing kinetics can be effectively controlled over a wide range of 5–240 min, adapting to the needs of different clinical scenarios.

[0091] Example 6 Evaluation of injectability and anti-collapse properties

[0092] 1. Experimental Procedure

[0093] The paste prepared in Example 1 was loaded into a 30G root canal syringe and injected into a transparent mold containing simulated tissue fluid (phosphate buffered saline, PBS) at room temperature at 0, 10, and 20 min after mixing. The morphology of the paste in the liquid was observed.

[0094] 2. Experimental Results and Analysis

[0095] The materials were successfully injected within 20 minutes, such as Figure 7 As shown, after injection into PBS, it can maintain its strip shape for a long time (0~60 min) without immediately dispersing or disintegrating, indicating that it has good clinical operation stability and water resistance.

[0096] Example 7: Imparting X-ray blocking properties

[0097] 1. Experimental Procedure

[0098] In the process of preparing the functionalized solid phase powder in Example 1, the nano hafnium dioxide (HfO2) powder was added in the total solid mass (Ca(H2PO4)2+ mucin) of 0%, 10%, 20%, and 30%, respectively, and pre-composite treatment was carried out together. The subsequent steps were the same as in Example 1.

[0099] The prepared dental cement was filled into a cylindrical mold with a diameter of 10 mm and a height of 1 mm, and after solidification, X-ray photography was performed together with a 3 mm initial height and a 3 mm increment aluminum wedge, and the data was quantified. Each group of samples was repeated 3 times, and the average value was taken.

[0100] 2. Experimental results and analysis

[0101] Table 2 X-ray blocking property

[0102]

[0103] As shown in Figure 8 , XRD analysis showed that HfO2 diffraction peaks appeared in the solidification product, indicating that the dental cement containing HfO2 had been successfully prepared. As shown in Table 2, the finally prepared dental cement had good X-ray blocking property, and the blocking effect of the dental cement with a 30% addition amount was equivalent to that of a 4.9 mm aluminum wedge, which was significantly higher than the international standard (3 mm aluminum wedge), facilitating clinical imaging evaluation.

[0104] Example 8 Biocompatibility evaluation

[0105] 1. Experimental steps

[0106] The other raw materials of the dental cement and the preparation process were the same as in Example 1, and the mucin content was set to 10 wt% which had the best antibacterial effect.

[0107] The mixed dental cement was filled into a cylindrical mold with a diameter of 6 mm and a height of 10 mm. After 24 h, the cement was taken out and immersed in a 0.5% sodium chloride solution for 7 days. After 7 days, the sample was prepared according to the international standard (0.2 g / mL) to configure 5 mL of leaching solution, and the leaching solution was filtered using a sterile filter head before use. Then in a 96-well plate, bone marrow mesenchymal stem cells (BMSCs) were inoculated at a density of 2×10 3 / well, and after the cells were completely adhered, the original culture medium was discarded and replaced with 100 μL of leaching solution for continuous culture for 1, 3, and 5 days. The proliferation activity of the cells was detected at the corresponding culture time nodes using CCK-8 working solution (prepared by mixing CCK-8 reagent and complete culture medium at a ratio of 1:10). Finally, the final value was read using an enzyme marker.

[0108] A control group was also set up, and bone marrow mesenchymal stem cells (BMSCs) were inoculated in a 96-well plate at a density of 2×10 3BMSCs were seeded at a density of / wells, and after the cells were fully adhered, they were cultured for 1, 3, and 5 days. At the corresponding culture time points, the cell proliferation activity was detected using CCK-8 working solution, and the final values ​​were read using an ELISA reader.

[0109] 2. Experimental Results and Analysis

[0110] The results showed that the dental cement of the present invention not only lacked any cytotoxicity, but its extract may also contain bioactive components that can significantly promote the proliferation of BMSCs. For example... Figure 9 As shown, compared with the blank culture medium control group, the extract of the material of the present invention (experimental group) significantly promoted the proliferation of BMSCs on days 1, 3, and 5 of culture. This excellent performance, exceeding the conventional "non-toxic" standard, may be related to the following mechanism:

[0111] (1) Regulation of ion microenvironment: The calcium and phosphate ions continuously released by the material in the simulated body fluid provide essential nutrients for cell metabolism and proliferation, and may activate related cell signaling pathways.

[0112] (2) Release of bioactive components: The surface-functionalized antibacterial polysaccharides are released slowly at the interface, which may provide biological signals similar to the extracellular matrix, which is beneficial to the adhesion and growth of stem cells.

[0113] (3) No toxic interference: The preparation method of the present invention ensures that the antibacterial components are stably integrated into the mineralized structure, avoiding the dissolution of small molecule toxic substances, and creating a pure and supportive microenvironment for cells.

[0114] The experimental results of this embodiment demonstrate that the biomimetic mineralized dental cement provided by the present invention is a bioactive tissue repair material, rather than a passive physical filler. Through the dual action of chemical and biological processes, it is expected to improve the clinical efficacy from "root canal sealing" to "functional regeneration of periodontal tissue".

[0115] Example 9: Demonstration of Extracted Root Canal Filling

[0116] 1. Experimental Procedure

[0117] A single-rooted extracted human tooth was selected, and standard root canal preparation and drying were performed. The paste prepared in Example 1 was injected into the root canal system using a root canal syringe. Subsequently, X-ray images were taken.

[0118] 2. Experimental Results and Analysis

[0119] like Figure 10 As shown, the material can fully fill the main root canal and lateral canals, with clear outlines, no obvious air bubbles or gaps, and fits tightly with the dentin wall, demonstrating excellent root canal sealing ability and clinical applicability.

[0120] The embodiments described above are only some of the embodiments of the present application, not all the embodiments. The detailed description of the embodiments of the present application is not intended to limit the scope of the claimed application, but merely represents selected embodiments of the application. The scope of protection of the present application is defined by the scope of the claims, and all other embodiments obtained by persons of ordinary skill in the art based on the embodiments of the present application without creative labor fall within the scope of protection of the present application.

Claims

1. A biomimetic mineralized dental cement with antibacterial-mineralization synergistic function, characterized in that, Including solid-phase systems and liquid-phase systems; The solid-phase system includes calcium phosphate-based inorganic particles and an antibacterial polysaccharide functional layer stably bound to the surface of the calcium phosphate-based inorganic particles through hydrogen bonding and electrostatic interaction. The liquid phase system is an ion-controlled solution containing complexing components; In this process, the antibacterial polysaccharide functional layer participates in inducing the nucleation and growth of calcium phosphate mineral phases during the mixing of the solid and liquid phases and the curing of the material, forming a biomineralized organic film-sheet calcium phosphate composite structure, thereby giving the biomimetic mineralized dental cement both antibacterial function and mineralization activity.

2. The biomimetic mineralized dental cement with antibacterial-mineralization synergistic function according to claim 1, characterized in that, The antibacterial polysaccharide functional layer is a continuous or semi-continuous nanoscale coating structure with a thickness of 10~200 nm.

3. The biomimetic mineralized dental cement with antibacterial-mineralization synergistic function according to claim 1, characterized in that, The calcium phosphate-based inorganic particles are selected from one or more of amorphous calcium phosphate, octacalcium phosphate, α-tricalcium phosphate, β-tricalcium phosphate, hydroxyapatite, and calcium dihydrogen phosphate.

4. The biomimetic mineralized dental cement with antibacterial-mineralization synergistic function according to claim 1, characterized in that, The ion-regulating solution includes a complexing agent, which includes sodium pyrophosphate.

5. The biomimetic mineralized dental cement with antibacterial-mineralization synergistic function according to claim 1, characterized in that, The antibacterial polysaccharide is a mucin.

6. The biomimetic mineralized dental cement with antibacterial-mineralization synergistic function according to claim 1, characterized in that, The biomimetic mineralized dental cement is in the form of an injectable paste, with an adjustable curing time of 5 to 240 minutes and a compressive strength of 5 to 30 MPa after curing.

7. The biomimetic mineralized dental cement with antibacterial-mineralization synergistic function according to claim 1, characterized in that, The biomimetic mineralized dental cement also includes an X-ray shielding agent.

8. A method for preparing a biomimetic mineralized dental cement with antibacterial-mineralization synergistic function as described in any one of claims 1-7, characterized in that, Includes the following steps: Step 1) Pre-composite calcium phosphate-based inorganic particles with antibacterial polysaccharides to form an antibacterial polysaccharide functional layer on the particle surface, thereby obtaining a functionalized solid phase system. Step 2) Mix the functionalized solid-phase system obtained in Step 1) with an ion-controlled solution containing complexing components to form a homogeneous injectable paste.

9. The preparation method according to claim 8, characterized in that, Step 2) The solid-liquid ratio of the functionalized solid-phase system to the ion-controlled solution is 1:

1.

10. The use of the biomimetic mineralized dental cement with antibacterial-mineralization synergistic function as described in any one of claims 1-7 in the preparation of materials for dental root canal filling, tooth remineralization restoration or periodontal tissue restoration.

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