Fe掺杂Ti-MOFs用于牙周炎抗菌声动力治疗

doi:10.15541/jim20250165

摘要/Abstract

摘要： 牙周炎是临床极富挑战的问题,由口腔致病菌过度生长失衡引起,可导致牙周组织的不可逆损伤。与清创术相比,抗菌声动力疗法（aSDT）具有优异的生物相容性和组织穿透能力,是一种有前景的替代方案。本工作制备了铁掺杂的钛基金属有机框架（Fe/Ti-MOFs）,研究了铁掺杂与声催化效率间的量效关系。Fe的引入能够调节MOFs的能带结构和结晶度,且未改变其晶格结构。结果表明,Fe/Ti-MOFs在超声波作用下表现出增强的羟基自由基（•OH）的产生能力,从而催化杀灭细菌病原体。其中,Fe/Ti摩尔比为0.025:1的样品表现出较佳的声催化性能,且受带隙工程、铁掺杂浓度和结晶度的共同调节。此外,牙龈成纤维细胞增殖和活死染色结果表明,Fe/Ti-MOFs具有优异的生物相容性。超声响应的Fe/Ti-MOFs材料为牙周炎的aSDT治疗提供了新的见解和策略,有望避免抗生素的不良反应。

关键词: 抗菌, 声动力治疗, 牙周炎, 金属有机框架, NH₂-MIL-125

Abstract: Periodontitis is a clinical challenging caused by bacterial overgrowth, resulting in irreversible damage to periodontal tissue. Antibacterial sonodynamic therapy (aSDT) has emerged as a promising alternative to conventional debridement due to its excellent biocompatibility and tissue penetration capability. Here, Fe doped Ti based metal-organic frameworks (Fe/Ti-MOFs) were prepared to explore the relationship between Fe doping and sonoresponsive efficiency. The incorporation of Fe enabled precise modulation of the band structure and crystallinity while maintaining the lattice architecture. Results showed that Fe/Ti-MOFs exhibited enhanced hydroxyl radical (•OH) generation under ultrasonic irradiation, effectively facilitating the eradication of bacterial pathogens. Notably, the sample with a Fe/Ti molar ratio of 0.025:1 exhibited exceptional performance. The sonocatalytic activity was collectively influenced by bandgap engineering, Fe doping concentration, and crystallinity. Moreover, Fe/Ti-MOFs exhibited no cytotoxicity toward gingival fibroblasts and maintained excellent biocompatibility, without adverse effects on tissue repair. The ultrasound responsive Fe/Ti-MOFs material developed in this study offers potential for mitigating the adverse effects of antibiotics and providing novel insights and strategies for the application of aSDT in periodontitis treatment.

Key words: antibacterials, sonodynamic therapy, periodontitis, metal organic framework, NH₂-MIL-125

中图分类号:

R781

王浩宇, 柯学, 关世伟, 钱仕, 刘宣勇. Fe掺杂Ti-MOFs用于牙周炎抗菌声动力治疗[J]. 无机材料学报, DOI: 10.15541/jim20250165.

WANG Haoyu, KE Xue, GUAN Shiwei, QIAN Shi, LIU Xuanyong. Fe Doped Ti-MOFs for Enhanced Antibacterial Sonodynamic Therapy of Periodontitis[J]. Journal of Inorganic Materials, DOI: 10.15541/jim20250165.

参考文献

[1] TAN X, LIU S, HU X,et al. Near-infrared-enhanced dual enzyme-mimicking Ag-TiO_2-x@alginate microspheres with antibactericidal and oxygeneration abilities to treat periodontitis. ACS Applied Materials and Interfaces, 2023, 15(1): 391-406.
[2] MIYAUCHI S, KAWADA-MATSUO M, FURUSHO H,et al. Atrial translocation of porphyromonas gingivalis exacerbates atrial fibrosis and atrial fibrillation. Circulation, 2025, DOI: 10.1161/CIRCULATIONAHA.124.071310.
[3] LIU H, NAN Z, ZHAO C,et al. Emerging synergistic strategies for enhanced antibacterial sonodynamic therapy: Advances and prospects. Ultrasonics Sonochemistry, 2025, 116: 107288.
[4] ZHANG K, WANG T, HUANG X,et al. Ultrasound-mediated nanomaterials for the treatment of inflammatory diseases. Ultrasonics Sonochemistry, 2025, 114: 107270.
[5] LI K, XU W, CHEN Y,et al. Piezoelectric nanostructured surface for ultrasound-driven immunoregulation to rescue titanium implant infection. Advanced Functional Materials, 2023, 33(28): 2214522.
[6] CHEN H, LIU L, MA A,et al. Noninvasively immunogenic sonodynamic therapy with manganese protoporphyrin liposomes against triple-negative breast cancer. Biomaterials, 2021, 269: 120639.
[7] PAN X, WU N, TIAN S,et al. Inhalable MOF-derived nanoparticles for sonodynamic therapy of bacterial pneumonia. Advanced Functional Materials, 2022, 32(25): 2112145.
[8] QIN W, YANG Q, ZHU C,et al. A Distinctive insight into inorganic Ssonosensitizers: design principles and applicationdomains. Small, 2024, 20(25): 2311228.
[9] LI D, YANG Y, LI D,et al. Organic sonosensitizers for sonodynamic therapy: from small molecules and nanoparticles toward clinical development. Small, 2021, 17(42): 2101976.
[10] YANG F, DONG J, LI Z,et al. Metal-organic frameworks (MOF)-assisted sonodynamic therapy in anticancer applications. ACS Nano, 2023, 17(5): 4102
[11] DAN-HARDI M, SERRE C, FROT T,et al. A new photoactive crystalline highly porous titanium(IV) dicarboxylate. Journal of the American Chemical Society, 2009, 131(31): 10857
[12] VERMOORTELE F, MAES M, MOGHADAM P Z, ,et al. p-Xylene-selective metal-organic frameworks: a case of topology-directed selectivity. Journal of the American Chemical Society. p-Xylene-selective metal-organic frameworks: a case of topology-directed selectivity. Journal of the American Chemical Society, 2011, 133(46): 18526-
[13] NGUYEN H L.Perspectives on titanium-based metal-organic frameworks.Journal of Physics: Energy, 2021, 3(2): 021003.
[14] CHEN J, CHENG F, LUO D,et al. Recent advances in Ti-based MOFs in biomedical applications. Dalton Transactions, 2022, 51(39): 14817.
[15] LIANG S, XIAO X, BAI L,et al. Conferring Ti-based MOFs with defects for enhanced sonodynamic cancer therapy. Advanced Materials, 2021, 33(18): 2100333.
[16] WANG Q, TIAN Y, YAO M,et al. Bimetallic organic frameworks of high piezovoltage for sono‐piezo dynamic therapy. Advanced Materials, 2023, 35(41): 2301784.
[17] LI Y, REN Z, HE Z,et al. Crystallinity-defect matching relationship of g-C3N4: experimental and theoretical perspectives. Green Energy and Environment, 2024, 9(4): 623.
[18] JIN Y, LIU F, LI Y,et al. Efficient adsorption of azo anionic dye Congo Red by micro-nano metal-organic framework MIL-68(Fe) and MIL-68(Fe)/chitosan composite sponge: Preparation, characterization and adsorption performance. International Journal of Biological Macromolecules, 2023, 252: 126198.
[19] WANG Y, FENG W, LI J,et al. A novel route for the facile synthesis of NH2-MIL-53(Fe) and its highly efficient and selective adsorption of congo red. Inorganica Chimica Acta, 2023, 547: 121332.
[20] OLCZAK T, SIMPSON W, LIU X,et al. Iron and heme utilization in Porphyromonas gingivalis. FEMS Microbiology Reviews, 2005, 29(1): 119.
[21] WÓJTOWICZ H, GUEVARA T, TALLANT C,et al. Unique structure and stability of HmuY, a novel heme-binding protein of porphyromonas gingivalis. PLOS Pathogens, 2009, 5(5): e1000419.
[22] WANG X, ZHONG X, BAI L,et al. Ultrafine titanium monoxide (TiO_1+x) nanorods for enhanced sonodynamic therapy. Journal of the American Chemical Society, 2020, 142(14): 6527
[23] ZHANG D Y, LIU H, YOUNIS M R,et al. In-situ TiO_2-x decoration of titanium carbide MXene for photo/sono-responsive antitumor theranostics. Journal of Nanobiotechnology, 2022, 20(1): 53.
[24] GUAN S, XU W, TAN J,et al. Metainterface heterostructure enhances sonodynamic therapy for disrupting secondary biofilms. ACS Nano, 2024, 18(23): 15114.