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Made available in DSpace on 2022-04-29T08:39:18Z (GMT). No. of bitstreams: 0 Previous issue date: 2022-02-01 The dentin matrix is a collagenous scaffold structurally involved in anchoring resin-based materials to the tooth. Time-dependent degradation of this scaffold at the resin–dentin interface remains a core problem in adhesive dentistry, limiting the service life of dental fillings. This study explored the use of emergent materials termed metal–organic frameworks (MOFs)─formed by the self-assembly of metal ions and organic building blocks─to safeguard the collagen integrity in the functional dentin matrix. We demonstrate that collagen fibrils (from demineralized human dentin) can induce the biomimetic growth of MOF crystals as protective coatings to strengthen and stabilize the fibrils. Zeolitic imidazolate framework-8 (ZIF-8), a zinc-based microporous MOF, was used to fabricate the MOF composites via a “one-pot” reaction in water. The ZIF-modified dentin matrix presented superior mechanical strength and resistance to proteolysis, which can positively affect the longevity of collagen as an anchoring substrate. This work identifies a potential biomedical application of biomimetically synthesized MOFs in repairing dental tissues critical to restorative therapies. Department of General Dental Sciences School of Dentistry Marquette University Department of Physics School of Sciences São Paulo State University (UNESP) Department of Inorganic Chemistry Institute of Chemistry Sao Paulo State University (UNESP) Department of Physics School of Sciences São Paulo State University (UNESP) Department of Inorganic Chemistry Institute of Chemistry Sao Paulo State University (UNESP)

Made available in DSpace on 2020-12-12T02:22:14Z (GMT). No. of bitstreams: 0 Previous issue date: 2020-08-10 Plant-derived compounds incite applications virtually on every biomedical field due to the expedient antioxidant, anti-inflammatory and antimicrobial properties in conjunction with a natural character. Here, quercetin (QCT), a flavonoid with therapeutic potentials relevant to the oral environment, was encapsulated within metal-organic frameworks (MOFs) to address the concept of on-demand release of phytochemicals at the biointerface. We verified the applicability of a microporous MOF (ZIF-8) as a controlled-release system for QCT, as well as investigated the incorporation of QCT@ZIF-8 microparticles into a dental adhesive resin for desirable therapeutic capabilities at the tooth-restoration interface. QCT was encapsulated within the frameworks through a water-based, one-step synthetic process. The resulting QCT@ZIF-8 microparticles were characterized with respect to chemical composition, crystal structure, thermal behavior, micromorphology, and release profile under acidic and physiological conditions. A model dental adhesive formulation was enriched with the bioactive microparticles; both the degree of conversion (DC) of methacrylic double bonds and the polymer thermal behavior were accounted for. The results confirm that crystalline QCT@ZIF-8 microparticles with attractive loading capacities, submicron sizes, high thermal stability and responsiveness to environmental pH change were successfully manufactured. The concentration of QCT@ZIF-8 in the resin system was a key factor to maintain an optimal DC plateau and rate of polymerization. Essentially, one-step encapsulation of QCT in biocompatible ZIF-8 matrices can be easily achieved, and QCT@ZIF-8 microparticles proved as smart platforms to carry bioactive compounds with potential use to prevent microbial and enzymatic degradation of hard tissues and extracellular matrix components. Department of Physics School of Sciences São Paulo State University (UNESP) Department of Chemistry School of Sciences São Paulo State University (UNESP) Department of Restorative Dentistry College of Dentistry University of Illinois at Chicago (UIC) Dental Research Division Guarulhos University (UNG) Department of Inorganic Chemistry Institute of Chemistry São Paulo State University (UNESP) Department of Physics School of Sciences São Paulo State University (UNESP) Department of Chemistry School of Sciences São Paulo State University (UNESP) Department of Inorganic Chemistry Institute of Chemistry São Paulo State University (UNESP)

Made available in DSpace on 2021-06-25T10:22:27Z (GMT). No. of bitstreams: 0 Previous issue date: 2021-03-15 The use of polymer additives that stabilize fluidic amorphous calcium phosphate is key to obtaining intrafibrillar mineralization of collagen in vitro. On the other hand, this biomimetic approach inhibits the nucleation of mineral crystals in unconfined extrafibrillar spaces, that is, extrafibrillar mineralization. The extrafibrillar mineral content is a significant feature to replicate from hard connective tissues such as bone and dentin as it contributes to the final microarchitecture and mechanical stiffness of the biomineral composite. Herein, we report a straightforward route to produce densely mineralized collagenous composites via a surface-directed process devoid of the aid of polymer additives. Simulated body fluid (1×) is employed as a biomimetic crystallizing medium, following a preloading procedure on the collagen surface to quickly generate the amorphous precursor species required to initiate matrix mineralization. This approach consistently leads to the formation of extrafibrillar bioactive minerals in bulk collagen scaffolds, which may offer an advantage in the production of osteoconductive collagen-apatite materials for tissue engineering and repair purposes. Department of General Dental Sciences Marquette University School of Dentistry Department of Physics School of Sciences São Paulo State University (UNESP) Department of Restorative Dentistry School of Dentistry of Ribeirão Preto University of São Paulo (USP) Department of Physics School of Sciences São Paulo State University (UNESP)

A growing class of multifunctional porous materials termed metal–organic frameworks (MOFs) has attracted attention for immobilization of biomolecules via self-assembly of inorganic and organic building blocks. Herein, we report the rapid formation of MOF shells surrounding collagen-degrading enzymes by using a biomimetic mineralization approach. Bacterial collagenase, which is functionally related to endogenous proteases in the human body, was used as a nucleating agent to induce the mineralization of zeolitic imidazolate framework-8 (ZIF-8) as a crystalline shell. This zinc-based MOF material was selected due to its remarkable stability under physiological conditions and good biocompatibility. The straightforward, water-based synthesis yielded microporous collagenase-embedded ZIF-8 particles. Once immobilized inside the biomimetically mineralized MOF, the protease presented limited catalytic activity, being ineffective in the proteolysis of a collagen-like peptide. In conclusion, biomimetic mineralization of ZIF-8 using collagenase not only provided immobilization of the enzyme, but also enabled the control of its activity. This synthetic approach provides a potentially useful concept in the prevention of proteolytic activity involved in the degradation of collagen matrices in living organisms.

The objective of this work was to investigate the use of Biogran® functionalized with parathyroid hormone (PTH) 1-34 by sonochemistry for the local delivery of this anabolic agent to the implant site. The effects of Biogran® and topical administration of PTH 1-34 on peri-implant bone regeneration were evaluated from the microscale to ultrastructural levels in healthy (SHAM) and orchiectomized (ORQ). While some animals only received a titanium implant in their tibial metaphyses (CLOT group), in others the peri-implant defect was first filled with Biogran® either without or with PTH 1-34 functionalization (BG and BGPTH groups, respectively) prior to implant installation. Osseointegration was characterized from a biomechanical perspective by measuring the removal torque with the counter-torque technique. Micro-CT was used to evaluate the percentage of bone volume, trabecular thickness, number and separation, and bone-implant contact (BIC). Dynamics of new bone formation were assessed by measuring fluorochrome area, daily mineral apposition rate, and neoformed bone area using confocal laser microscopy. RT-PCR was performed to evaluate ALP and osteocalcin expression. The interface between newly formed bone and Biogran® was examined using scanning electron microscopy (SEM) and scanning transmission electron microscopy (STEM) at the micro-and nanoscale, respectively, while elemental analyses were completed in SEM with energy-dispersive X-ray spectroscopy (EDS). STEM imaging demonstrated the intimate attachment of bone to Biogran® (nanoscale level). Overall, the results suggest that the effectiveness of the topical administration of PTH 1-34 at the implant site seems enhanced in osteoporotic bone, promoting peri-implant bone regeneration to comparable levels in healthy conditions.

The application of resin-based materials is an alternative of treatment for eroded lesions. Nevertheless, there are no studies about the penetration of these materials into eroded lesion, which might affect its adhesion. Therefore, this study evaluated the penetration of four resin-based materials, with and without enamel etching. By using an in vitro protocol, types of treatment were studied at five levels (AdheSE(®) , Tetric N-Bond(®) , Single Bond 2(®) , Helioseal Clear(®) , Icon(®) ) and types of enamel etching in two levels (with and without). Materials were stained with 0.02 mg/mL ethanolic solution of tetramethylrhodamine isothiocyanate. Bovine enamel samples (4 × 4 mm) were immersed in 0.01 M HCl, pH 2.3, for 30 seconds to produce initial eroded lesions. Afterward, the materials were applied on half of sample enamel surface following the manufacturer's instructions. On the other half of sample, the materials were applied without etching the enamel. Materials penetration into the enamel was assessed by Confocal Laser Scanning Microscopy on reflection and fluorescence modes. The penetration depth (PD) was measured using ImageJ software. Data were analyzed by two-way ANOVA and Tukey test (P 0.05). It can be concluded that prior enamel etching increased the materials penetration into eroded enamel and the Icon(®) -infiltrant presented highest penetration.

Rhodamine B (RB) is commonly used to evaluate dental polymers, including dental bonding systems (DBS). For reliability assessments, its effect should not only allow visualization of the dentin-polymer interface but also must not interfere with the bonding of the DBS to dentin as measured by the microtensile bond strength and hardness tests.Flat human dentin surfaces were prepared and randomly distributed (n = 10) into six groups: Adper Scotchbond Multi-Purpose (MP) or Clearfil SE Bond (SE) in concentrations of none/control, 0.02 or 0.1 mg/mL. These combinations were prepared through ethanol dissolution to improve their penetration into the dentin. All specimens were fabricated with Filtek Z250 (n = 10) and prepared for a microtensile bond test (μTBS) (0.5 mm/min) after 7 days and 6 months. The failure modes were determined using a stereomicroscope (×40). For the hardness test, flat human dentin blocks were prepared and treated as previously described (n = 6). The specimens were stored at 37 °C/48 h and were tested (Knoop indenter - 25 gF/10 s). Data were analyzed with two-way ANOVA and Tukey tests for multiple comparisons (α = 0.05). The effect of time was evaluated using the Student t-test.For 7-day μTBS, both the DBS and RB concentrations were significant factors (p 0.01). After 6 months, only the RB concentration was significantly different. Adhesive failures were prevalent for all groups. Regarding hardness, the DBS differed only with the use of 0.10 mg/mL of RB.Ethanol-dissolved rhodamine B in concentrations of 0.02 and 0.10 mg/mL in non-simplified adhesives can affect the physical-mechanical properties of functional monomer-based systems rather more than those of BisGMA systems.

Simplified dentin-bonding systems are clinically employed for most adhesive procedures, and they are prone to hydrolytic degradation. Objective This study aimed to investigate the effect of laser diode irradiation on the degree of conversion (DC), water sorption (WS), and water solubility (WSB) of these bonding systems in an attempt to improve their physico-mechanical resistance. Material and Methods Two bonding agents were tested: a two-step total-etch system [Adper™ Single Bond 2, 3M ESPE (SB)] and a universal system [Adper™ Single Bond Universal, 3M ESPE (SU)]. Square-shaped specimens were prepared and assigned into 4 groups (n=5): SB and SU (control groups – no laser irradiation) and SB-L and SU-L [SB and SU laser (L) – irradiated groups]. DC was assessed using Fourier transform infrared spectroscopy with attenuated total reflectance. Additional uncured resin samples (≈3.0 µL, n=5) of each adhesive were also scanned for final DC calculation. For WS/WSB tests, similar specimens (n=10) were prepared and measured by monitoring the mass changes after dehydration/water storage cycles. For both tests, adhesive fluids were dropped into standardized Teflon molds (6.0×6.0×1.0 mm), irradiated with a 970-nm laser diode, and then polymerized with an LED-curing unit (1 W/cm2). Results Laser irradiation immediately before photopolymerization increased the DC (%) of the tested adhesives: SB-L>SB>SU-L>SU. For WS/WSB (μg/mm3), only the dentin bonding system (DBS) was a significant factor (pSU. Conclusion Irradiation with a laser diode improved the degree of conversion of all tested simplified dentin bonding systems, with no impact on water sorption and solubility.

Made available in DSpace on 2018-11-26T17:20:50Z (GMT). No. of bitstreams: 0 Previous issue date: 2017-02-01 Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) Fluorescent dyes like Rhodamine B (RB) have been used to identify the spatial distribution of adhesive restorative materials in the tooth/restoration interface. Potential effects of the addition of RB to dental adhesives were addressed in the past, but no further information is available on how to determine suitable concentrations of RB in these bonding agents for imaging in the confocal laser scanning microscope. This study provides systematical strategies for adding RB to viscous dental adhesive resins, focusing on the determination of the lowest range of dye concentrations necessary to achieve an acceptable image of the dentin/adhesive interface. It was demonstrated that optimized images of the resin distribution in dentin can be produced with 0.1-0.02 mg/mL of RB in the (tested) adhesives. Our approaches took into account aspects related to the dye concentration, photophysical parameters in different host media, specimen composition and morphology to develop a rational use of the fluorescent agent with the resin-based materials. Information gained from this work can help optimize labeling methods using dispersions of low-molecular-weight dyes in different monomer blend systems. Univ Sao Paulo, Bauru Sch Dent, Dept Operat Dent Endodont & Dent Mat, BR-17012901 Bauru, SP, Brazil Univ Estadual Paulista, Inst Chem, Dept Inorgan Chem, BR-14800060 Araraquara, SP, Brazil Univ Sao Paulo, Bauru Sch Dent, Dept Prosthodont, BR-17012901 Bauru, SP, Brazil Univ Sao Paulo, Sch Dent, Dept Operat Dent, BR-05508000 Sao Paulo, SP, Brazil Univ Estadual Paulista, Inst Chem, Dept Inorgan Chem, BR-14800060 Araraquara, SP, Brazil FAPESP: 2011/14971-2 FAPESP: 2012/13160-3 FAPESP: 2013/13161-2

Objective This study investigated the effect of the fluorescent dye rhodamine B (RB) for interfacial micromorphology analysis of dental composite restorations on water sorption/solubility (WS/WSL) and microtensile bond strength to dentin (µTBS) of a 3-step total etch and a 2-step self-etch adhesive system. Material and Methods The adhesives Adper Scotchbond Multi-Purpose (MP) and Clearfil SE Bond (SE) were mixed with 0.1 mg/mL of RB. For the WS/WSL tests, cured resin disks (5.0 mm in diameter x 0.8 mm thick) were prepared and assigned into four groups (n=10): MP, MP-RB, SE, and SE-RB. For µTBS assessment, extracted human third molars (n=40) had the flat occlusal dentin prepared and assigned into the same experimental groups (n=10). After the bonding and restoration procedures, specimens were sectioned in rectangular beams, stored in water and tested after seven days or after 12 months. The failure mode of fractured specimens was qualitatively evaluated under optical microscope (x40). Data from WS/WSL and µTBS were assessed by one-way and three-way ANOVA, respectively, and Tukey’s test (α=5%). Results RB increased the WSL of MP and SE. On the other hand, WS of both MP and SE was not affected by the addition of RB. No significance in µTBS between MP and MP-RB for seven days or one year was observed, whereas for SE a decrease in the µTBS means occurred in both storage times. Conclusions RB should be incorporated into non-simplified DBSs with caution, as it can interfere with their physical-mechanical properties, leading to a possible misinterpretation of bonded interface.

The application of resin-based materials is an alternative of treatment for eroded lesions. Nevertheless, there are no studies about the penetration of these materials into eroded lesion, which might affect its adhesion. Therefore, this study evaluated the penetration of four resin-based materials, with and without enamel etching. By using an in vitro protocol, types of treatment were studied at five levels (AdheSE(®) , Tetric N-Bond(®) , Single Bond 2(®) , Helioseal Clear(®) , Icon(®) ) and types of enamel etching in two levels (with and without). Materials were stained with 0.02 mg/mL ethanolic solution of tetramethylrhodamine isothiocyanate. Bovine enamel samples (4 × 4 mm) were immersed in 0.01 M HCl, pH 2.3, for 30 seconds to produce initial eroded lesions. Afterward, the materials were applied on half of sample enamel surface following the manufacturer's instructions. On the other half of sample, the materials were applied without etching the enamel. Materials penetration into the enamel was assessed by Confocal Laser Scanning Microscopy on reflection and fluorescence modes. The penetration depth (PD) was measured using ImageJ software. Data were analyzed by two-way ANOVA and Tukey test (P 0.05). Regardless of the material, etched enamel resulted in higher PD than non-etched (P 0.05). Icon(®) showed the highest PD in enamel followed by Helioseal Clear(®) (P 0.05), with significant difference between them (P 0.05) and no difference was found among AdheSE(®) , Tetric N-Bond(®) , and Single Bond 2(®) (P 0.05). It can be concluded that prior enamel etching increased the materials penetration into eroded enamel and the Icon(®) -infiltrant presented highest penetration.