Biocompatible Natural Polymers and Cutting-Edge Fabrication Techniques in the Development of Next-Generation Oral Thin Films for Enhanced Drug Delivery Systems.

Oral thin films are changing the way drugs are delivered, making drug administration more convenient and patient-friendly. This review delves into the fascinating possibilities of natural polymers in thin film design. We consider the benefits of biocompatible polymers produced from chitosan, gelatin, and pullulan. Their intrinsic biodegradability and safety make them excellent for use with a wide range of patients. Additionally, the research investigates novel strategies for creating these distinctive drug delivery systems. We look beyond standard solvent casting techniques, hot melt extrusion methods, rolling methods, etc. These technologies provide exact control over film qualities, allowing for tailored medication delivery and increased patient compliance. This review seeks to bridge the gap between natural polymers and cutting-edge fabrication processes. By investigating this combination, we pave the road for the development of next-generation oral thin films that are more efficacious, patient-acceptable, and environmentally-friendly.

Genomic analysis and mechanisms exploration of a stress tolerance and high-yield pullulan producing strain.

Pullulan is a kind of natural polymer, which is widely used in medicine and food because of its solubility, plasticity, edible, non-toxicity and good biocompatibility. It is of great significance to improve the yield of pullulan by genetic modification of microorganisms. It was previously reported that Aureobasidium melanogenum TN3-1 isolated from honey-comb could produce high-yield of pullulan, but the molecular mechanisms of its production of pullulan had not been completely solved. In this study, the reported strains of Aureobasidium spp. were further compared and analyzed at genome level. It was found that genome duplication and genome genetic variations might be the crucial factors for the high yield of pullulan and stress resistance. This particular phenotype may be the result of adaptive evolution, which can adapt to its environment through genetic variation and adaptive selection. In addition, the TN3-1 strain has a large genome, and the special regulatory sequences of its specific genes and promoters may ensure a unique characteristics. This study is a supplement of the previous studies, and provides basic data for the research of microbial genome modification in food and healthcare applications.

Fabrication and characterization of electrospun core-shell nanofibers of bilayer zein/pullulan emulsions crosslinked by genipin.

In this study, the electrospun core-shell nanofibers of zein/pullulan stabilized bilayer emulsions before and after genipin crosslinking were fabricated. The experimental results indicated that the addition of pullulan increased the apparent viscosity and elastic modulus of the bilayer emulsions, which was further increased after the chemical crosslinking of genipin. The nanofiber diameter increased from 102.9 nm to 169.9 nm with the increasing ratio of pullulan, but increased significantly to a range of 405.6-708.0 nm after genipin crosslinking. The electrospun nanofiber films of crosslinked emulsions had higher thermal stability and stronger water stability. The FTIR result proved the existence of hydrogen bond interaction between the zein, pullulan, and genipin molecules. In addition, before and after crosslinking, the encapsulation efficiency of electrospun fiber films for camellia oil was >77.68 %, and the maximum encapsulation efficiency could reach 87.94 %, and there was no significant change during the 7-day storage period, showing good stability. These research results can provide a theoretical basis for the encapsulation of hydrophobic active substances in zein-based emulsion electrospun core-shell nanofibers.

Electrospun gelatin/tea polyphenol@pullulan nanofibers for fast-dissolving antibacterial and antioxidant applications.

Bio-based active food packaging materials have a high market demand. We use coaxial electrospinning technology to prepare core-shell structured nanofibers with sustained antibacterial and antioxidant properties. The fiber core layer was composed of gelatin and tea polyphenols, whereas tea polyphenols provide antibacterial and antioxidant properties; the fiber sheath was composed of pullulan polysaccharides with antioxidant properties. By using a scanning electron microscope, it can be seen that the diameter distribution of the prepared nanofibers was uniform and the surface is smooth; using a transmission electron microscope, it can be clearly seen that the nanofibers have a core-shell structure; Fourier Transform Infrared and X-ray diffraction analysis indicate that the nanofibers have an amorphous structure; the 2,2-diphenyl-1-picrylhydrazyl free radical scavenging shows that nanofibers have higher antioxidant properties with the addition of tea polyphenols; antibacterial test showed that nanofibers had obvious inhibitory effect on the growth of Staphylococcus aureus and Escherichia coli; and the nanofiber film dissolution test shows that nanofibers can be used as fast soluble active packaging. Finally, core-sheath-structured nanofibers can serve as active packaging for instant food, possessing both rapid water solubility and excellent antibacterial and antioxidant activity, making water-soluble nanofibers interesting applications in the field of food packaging.

High-capacity adsorption of organic dyes using separable pullulan gel encapsulated with PDA-modified ZIF-8.

In this investigation, a hydrogel adsorbent featuring remarkable efficiency in dye adsorption was successfully synthesized by the integration of natural polysaccharide (pullulan) and nanoparticles (ZIF-8@PDA). The prepared natural polysaccharide nanocomposite hydrogels not only exhibit superior mechanical strength and biocompatibility, but also demonstrate adeptness in the removal of dye pollutants. The dye removal capacities were 615.4 mg/g for malachite green (MG) and 525.8 mg/g for Congo red (CR), respectively. Notably, the adsorption process exhibits minimal susceptibility to variations in water quality and the presence of co-existing ions. The pH-responsive surface charge conversion capability of the adsorbent renders it recyclable, maintaining a dye adsorption performance exceeding 88 % even after 5 cycles of repeated usage. Overall, these environmentally friendly natural polysaccharide nanocomposite hydrogels hold potential for addressing complex wastewater treatment challenges and long-term use.

Preparation and characterization of polyvinyl alcohol/pullulan/ZnO-Nps composite film and its effect on the postharvest quality of Allium mongolicum Regel.

Allium mongolicum Regel is prone to rapid senescence and quality deterioration during postharvest storage. Herein, polyvinyl alcohol/pullulan/ZnO nanoparticles (PVA/PUL/ZnO-Nps) composite films were prepared via solution casting and studied to analyze the effects of ZnO-Nps on the PVA/PUL film matrix. Results revealed that the incorporation of suitable ZnO-Nps effectively reduced the light transmittance, improved water contact angle, water vapor permeability, and mechanical properties of the composite films, as well as enhanced their antimicrobial activity. The composite films were used for the postharvest preservation of A. mongolicum Regel. Results revealed that the PVA/PUL/ZnO-Nps film effectively reduced malondialdehyde accumulation content, superoxide radical generation rate, hydrogen peroxide content, improve the activity of related enzymes, and extend the storage time compared with that of polyethylene films. Therefore, the PVA/PUL/ZnO-Nps film can be used as a novel packaging material for the postharvest preservation of A. mongolicum Regel.

Fortification of pullulan/cassava starch-based edible films incorporated with LC-EO nanoparticles and the application for beef meat preservation.

A multipurpose food packaging film was created using pullulan and cassava starch as bases and sodium caseinate/zein-loaded Litsea cubeba essential oil nanoparticles as fillers. The study showed that the PS, PDI, Zeta potential and encapsulation efficiency of LC-EO in SC/ZNPs1% were 206.34 nm, 0.28 %, -25.73 mV, and 89.69 %, respectively, indicating even distribution and good stability. FTIR and XRD analysis confirmed hydrogen bond formation and structural changes between nanoparticle-forming materials, while SEM analysis revealed uniform distribution and spherical morphology of SC/ZNPs1%.The study found that the psc4% film showed improved mechanical properties, including an increase in elongation at break from 14.76 % to 19.30 %, and enhanced barrier characteristics, despite a slight decrease in tensile strength from 28.53 MPa to 7.77 MPa. The pcs4% film enhanced hydrophobic characteristics from 39.06 % to 20.91 % and showed inhibition against Staphylococcus aureus and E. coli O157:H7 at 28 mm and 23 mm inhibition zones, respectively, with improved antioxidant properties (76.16 %), effectively reducing bacterial populations, color, texture, and pH change and lipid oxidation in fresh beef for up to seven days. The psc4% film is a promising new active antibacterial and antioxidant food-packaging material.

The Role of Fe(III) in Selective Adsorption of Pullulan on Calcite Surfaces: Experimental Investigation and Molecular Dynamics Simulation.

The floatability of fluorite and calcite exhibit similar properties, rendering their flotation separation challenging. Macromolecular polysaccharide reagents containing the polyhydroxyl group have shown broad promising application. The selectivity of polysaccharide is relatively low. In this study, the introduction of Fe3+ was employed to enhance the selective adsorption capacity of Pullulan polysaccharide towards fluorite and calcite minerals, thereby achieving effective flotation separation. Furthermore, the mechanism underlying intramolecular interactions was elucidated. The DFT calculation and XPS analysis revealed that the adsorption of Fe3+ on the calcite surface was more favorable, leading to the formation of a Ca-O-Fe structure. The MD simulation, XPS analysis, and Zeta potential analysis revealed that the Fe-OH groups on the surface of calcite reacted with the -OH groups in Pullulan and formed bonds, resulting in the formation of a Calcite-Fe-Pullulan structure. This facilitated the attachment of a significant number of Pullulan molecules to the calcite surface. The formation of a hydrophilic layer on the outer surface of calcite by Pullulan, in contrast to the absence of such layer on fluorite's surface, results in an increased disparity in surface floatability between these two minerals, thereby enhancing the efficiency of flotation separation.

Stabilization of fermented tomato (Solanum lycopersicum L.) juice by differently charged hydrocolloids.

This study investigated the impact of three different charged hydrocolloids, anionic polysaccharide (soluble soybean polysaccharide, SSPS), neutral polysaccharide (pullulan polysaccharide, PUL), and cationic polysaccharide (chitosan, CS), and their complexation on the stabilization efficiency of fermented tomato juice (FTJ). The effect of hydrocolloids on FTJ under different treatment conditions were comprehensively evaluated by determining the particle size distribution, zeta potential, rheological properties, Fourier transform infrared spectroscopy, surface tension, and LUMiSizer. The combined conditions suggest that PUL exhibits better storage stability than SSPS and CS when used individually. Compared with the use of the stabilizers, the combination of hydrocolloids had a greater impact on the storage stability of the FTJ, and the storage stability of the FTJ increased when 0.15% SSPS + 0.03% PUL + 0.15% CS was added. This study lays the groundwork for the development of stable fruit juice beverages.

Efficient production of pullulan by Aureobasidium pullulans using a multi-objective optimization strategy with orthogonal experimental design coupling artificial neural network and genetic algorithm.

Efficient pullulan production has long been a central research focus. This study used maltodextrin as the carbon source for pullulan production by Aureobasidium pullulans fermentation. A hybrid optimization approach, integrating orthogonal experimental design (OED), backpropagation artificial neural network (BP-ANN), and elite strategy non-dominated sequential genetic algorithm-II (NSGA-II), was developed. Range analysis based on OED revealed that MgSO4·7H2O significantly affects production but less impacts molecular weight, while pH notably influences molecular weight with a lesser effect on production, underscoring the need for multi-objective optimization. The BP-ANN model showed strong predictive capabilities, with goodness-of-fit values of 0.984 and 0.980 for production and molecular weight, respectively. Using this model as the fitness function for the optimization algorithm enhanced efficiency. Taking cost factors into account, the BP-ANN-NSGA-II algorithm identified the optimal fermentation medium conditions, resulting in a 6.89 % increase in production, a 368.97 % increase in molecular weight, and a 42.49 % reduction in cost. The maximum comprehensive optimization efficiency is 63.73 %, and the multi-objective optimization is better than the single objective optimization. This method significantly guides the improvement of pullulan fermentation optimization efficiency.

Facile synthesis of ATTM@ZIF-8 modified pullulan hydrogels for enhanced adsorption of Congo red and malachite green.

Efficient capture of dyes from wastewater is of great importance for environmental remediation. Yet constructing adsorbents with satisfactory adsorption efficiency and low cost remains a major challenge. This work reports a simple and scalable method for the fabrication of functionalized porous pullulan hydrogel adsorbent decorated with ATTM@ZIF-8 for the adsorption of congo red (CR) and malachite green (MG). The embedding of ammonium tetrathiomolybdate (ATTM) into the ZIF-8 nanoclusters offered additional adsorption sites and enlarged the pore size of the resulting ATTM@ZIF-8. The homogeneous dispersion of the nanoparticles in the three-dimensional network of polysaccharide gels prevents their agglomeration and thus improves the affinity for dye molecules. The resulting adsorbent AZP-20 at optimized composite ratios exhibits high activity, selectivity, interference resistance, reusability and cytocompatibility in dye adsorption applications, and possesses high removal rate of dye in real water systems. Batch experiments demonstrated that the adsorption rate of AZP-20 for MG and CR was 1645.28 mg g-1 and 680.33 mg g-1, and would be influenced by pH conditions. Adsorption kinetics followed pseudo-second-order model. Adsorption isotherms followed Langmuir model for MG and Freundlich model for CR. The adsorption of dye molecules primarily relied on electrostatic interaction (MG) and π-π stacking interaction (CR). Conclusively, the prepared AZPs adsorbent illuminated good application prospects in the treatment of complex component dye wastewater.

Polyethylene Glycol/Pullulan-Based Carrier for Silymarin Delivery and Its Potential in Biomedical Applications.

Restoring the structures and functions of tissues along with organs in human bodies is a topic gathering attention nowadays. These issues are widely discussed in the context of regenerative medicine. Excipients/delivery systems play a key role in this topic, guaranteeing a positive impact on the effectiveness of the drugs or therapeutic substances supplied. Advances in materials engineering, particularly in the development of hydrogel biomaterials, have influenced the idea of creating an innovative material that could serve as a carrier for active substances while ensuring biocompatibility and meeting all the stringent requirements imposed on medical materials. This work presents the preparation of a natural polymeric material based on pullulan modified with silymarin, which belongs to the group of flavonoids and derives from a plant called Silybum marianum. Under UV light, matrices with a previously prepared composition were crosslinked. Before proceeding to the next stage of the research, the purity of the composition of the matrices was checked using Fourier-transform infrared (FT-IR) spectroscopy. Incubation tests lasting 19 days were carried out using incubation fluids such as simulated body fluid (SBF), Ringer's solution, and artificial saliva. Changes in pH, electrolytic conductivity, and weight were observed and then used to determine the sorption capacity. During incubation, SBF proved to be the most stable fluid, with a pH level of 7.6-7.8. Sorption tests showed a high sorption capacity of samples incubated in both Ringer's solution and artificial saliva (approximately 350%) and SBF (approximately 300%). After incubation, the surface morphology was analyzed using an optical microscope for samples demonstrating the greatest changes over time. The active substance, silymarin, was released using a water bath, and then the antioxidant capacity was determined using the Folin-Ciocâlteu test. The tests carried out proved that the material produced is active and harmless, which was shown by the incubation analysis. The continuous release of the active ingredient increases the biological value of the biomaterial. The material requires further research, including a more detailed assessment of its balance; however, it demonstrates promising potential for further experiments.

Cytotoxicity of two fluoride-releasing adhesive tapes.

Sodium fluoride-polyvinyl alcohol (NaF-PVA) tape was developed to deliver fluoride to teeth by adding fluoride to polymer tape. Previous studies have demonstrated that tapes are effective and have antimicrobial properties. This study aimed to evaluate the cytotoxicity of two fluoride-releasing adhesive tapes. We investigated two polyvinyl alcohol (PVA) tapes: (i) a fluoride-PVA (F-PVA) tape, and (ii) a pullulan-incorporated F-PVA (PF-PVA) tape. The cytotoxicity test was conducted on human gingival fibroblasts (HGF) and human periodontal ligament (PDL) cells. Using an adhesive tape containing fluoride, we performed the 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT) assay on these cells. Genetic analysis of the cells was performed to conduct a stability test on humans. In the MTT assay, PF-PVA had 66% greater cytotoxicity than control by PDL and 69% by HGF. F-PVA showed less cytotoxicity than PF-PVA by 29% in PDL and 33% in HGF. Gene ontology (GO) analysis and gene set enrichment analysis (GSEA) were performed as gene expression analyses. GO analysis indicated that PF-PVA displayed more expression changes of genes related to cytotoxicity than F-PVA. In addition, GSEA found more inflammatory response associations in PF-PVA than in F-PVA. MTT and genetic testing yielded comparable results.

Improvement in probiotic intestinal survival by electrospun milk fat globule membrane-pullulan nanofibers: Fabrication and structural characterization.

Studies have demonstrated the protective effect of milk fat globule membrane (MFGM) on probiotics in harsh environments. However, currently, there are no reports on the encapsulation of probiotics using MFGM. In this study, MFGM and pullulan (PUL) polysaccharide fibers were prepared by electrostatic spinning and used to encapsulate probiotics, with whey protein isolates (WPI)/PUL as the control. The morphology, physical properties, mechanical properties, survival, and stability of the encapsulated Lacticaseibacillus rhamnosus GG (LGG) were studied. The results showed that the MFGM/PUL solution had significant effects on pH, viscosity, conductivity, and stability. Electrostatic spinning improved the mechanical properties and encapsulation ability of the polymer formed by MFGM/PUL. LGG encapsulated in MFGM/PUL nanofibers survived rate was higher than WPI/PUL nanofibers in mimic intestinal juice, which could be attributed to the phospholipid content contained in MFGM. These results demonstrate that MFGM is a promising material for probiotic encapsulation, providing an important basis for the potential use of MFGM/PUL nanofibers as a robust encapsulation matrix.

Green synthesis, characterization, and multifunctional applications of Ag@CeO2 and Ag@CeO2-pullulan nanocomposites for dye degradation, antioxidant, and antifungal activities.

The synthesis and characterization of novel nanocomposites with unique properties have garnered significant interest. Ag@CeO2 nanocomposite and its pullulan counterparts were prepared using a green approach involving rosemary extract. Characterization techniques, including Fourier Transform Infrared Spectroscopy, UV-visible spectroscopy, zeta potential, Dynamic Light Scattering, High-Resolution Transmission Electron Microscopy, Energy-Dispersive X-ray Spectroscopy, Scanning Electron Microscopy, and X-ray Diffraction, confirmed the formation of Ag@CeO2 nanoparticles (NPs). Pullulan led to increased particle size and improved homogeneity. Employing the Artificial Neural Networks (ANN) model to optimize methylene blue removal by Ag@CeO2 NPs and Ag@CeO2-pullulan NPs demonstrated predictive capabilities up to 97.53 % of MB removal (R2 = 0.9991). The antioxidant test demonstrated that rosemary extract exhibited the highest activity (IC50 = 0.011 mg/mL), then Ag@CeO2 NPs (IC50 = 0.039 mg/mL), and Ag@CeO2-pullulan NPs (IC50 = 0.041 mg/mL). Both Ag@CeO2 NPs and Ag@CeO2-pullulan NPs inhibited Candida albicans growth, with the latter exhibiting enhanced efficacy (MIC = 468.27, MFC = 936.53, and IC50 = 129.60 µg/mL). The study successfully synthesized novel Ag@CeO2-based nanocomposites coupled with pullulan with promising applications in dye removal, and antimicrobial therapy. The incorporation of pullulan improved the properties of the nanocomposites, enhancing their potential for practical use in environmental and biomedical applications.

ARTP mutagenesis of Aureobasidium pullulans RM1603 for high pullulan production and transcriptome analysis of mutants.

Pullulan is a microbial exopolysaccharide produced by Aureobasidium spp. with excellent physical and chemical properties, resulting in great application value. In this study, a novel strain RM1603 of Aureobasidium pullulans with high pullulan production of 51.0 ± 1.0 g·L- 1 isolated from rhizosphere soil was subjected to atmospheric and room temperature plasma (ARTP) mutagenesis, followed by selection of mutants to obtain pullulan high-producing strains. Finally, two mutants Mu0816 and Mu1519 were obtained, with polysaccharide productions of 58.7 ± 0.8 and 60.0 ± 0.8 g∙L- 1 after 72-h fermentation, representing 15.1 and 17.6% increases compared with the original strain, respectively. Transcriptome analysis of the two mutants and the original strain revealed that the high expression of α/ß-hydrolase (ABHD), α-amylase (AMY1), and sugar porter family MFS transporters (SPF-MFS) in the mutants may be related to the synthesis and secretion of pullulan. These results demonstrated the effectiveness of ARTP mutagenesis in A. pullulans, providing a basis for the investigation of genes related to pullulan synthesis and secretion.

Fabrication of Abelmoschus manihot gum/pullulan/magnesium L-ascorbate green composite packaging film and its excellent performance in preserving fresh-cut carrots.

Pullulan-based composite film can be a potential alternative packing material to non-environmentally friendly plastic wrap (PE) to preserve fresh-cut carrots. However, many developed pullulan-based composites either have high water vapor permeability (WVP) and high mechanical strength or vice versa, which limits the practicality of the developed packaging materials for potential commercialization. Herein, Abelmoschus manihot gum (AMG)/pullulan/magnesium L-ascorbate (MLA) was created as a green composite film (APL) to preserve fresh-cut carrots. The optimal amount of MLA was found to be 10 % (APL10), demonstrating a balance of lower WVP and greater mechanical strength and antioxidant performance than many pullulan-based films. This effectively solved many problems faced by other pullulan-based packaging films. After the fresh-cut carrots were packed with the composite film for 4 days, it was found that APL10 was effective in preserving the quality of carrots, in terms of freshness, weight loss rate, Vitamin C (VC), and malondialdehyde (MDA) content after 4 days of storage, much better than non-biodegradable PE. Thus, based on these findings, it is concluded that APL films have huge potential as a green packaging material for food to replace PE in the future.

ß-Cyclodextrin mediated controlled release of phenothiazine from pH-responsive pectin and pullulan-based hydrogel optimized through experimental design.

Drugs with lower permeability and water solubility provide major challenges for producing safe and efficient formulations. The current work aims to prepare ICs of the drug phenothiazine and ß-cyclodextrin via physical, microwave, freeze-drying, and kneading methods. Many analytical methods, such as 1H NMR, ROESY, FT-IR, DSC, SEM, and XRD, were then used to confirm the formation of inclusion complexes. The natural polysaccharide-based hydrogel comprising pectin and pullulan was synthesized in air and optimized through various parameters. In order to maximize the reaction parameters, Response Surface Methodology design was employed for experimental optimization. We use FT-IR, TGA, SEM, EDX, and XRD to investigate hydrogel formation. At 37 °C, an investigation was carried out on the in vitro controlled release of PN at pH 2, 7, and 7.4. The analysis of drug release data revealed that PM and KM exhibited an initial burst release of drugs, with the MW and FD method proving to be the most suitable approach for achieving precise ICs of PN and ß-CD for sustained drug release. The kinetics of drug release were evaluated using various kinetic models, with the Riteger-Peppas and Peppas-Sahlin models demonstrating the best fit for drug release in all instances.

Sinapic acid-pullulan based inflammation responsive nanomicelles for the local treatment of experimental inflammatory arthritis.

Rheumatoid arthritis (RA) is a chronic inflammatory disorder of joints. It is one of the major causes of disability and morbidity worldwide. Administration of conventional drugs through the systemic route restricts the bioavailability of drugs, systemic toxicity, and reduced efficacy. We have introduced Rebamipide (Reb)-loaded Sinapic acid (SA)-Pullulan (PL) nanomicelles (Reb@SA-PL NMs), a nanotechnology based drug delivery system for the treatment of inflammatory arthritis. PL is a polysaccharide obtained from the fungus Aureobasidium pullulans, and SA is a bioactive polyphenol found in various plants. Both are classified by US-FDA Generally Recognised as Safe (GRAS) materials. Reb@SA-PL NMs found to be cytocompatible. Subsequently, intra-articular administration of Reb@SA-PL NMs enhances the anti-arthritic potential compared to free Reb drug in collagen-induced experimental inflammatory arthritis rat model. Reb@SA-PL NMs reduced the expression of RANKL receptor and Nf-κB. Reb@SA-PL NMs reverses the breakdown of type II collagen, MMP-13, and inhibits the pro-inflammatory markers. Reb@SA-PL NMs prevented bone erosion, cartilage degradation, joint oedema, and synovial inflammation. The results of the study demonstrated that Reb@SA-PL NMs, an enzyme-responsive drug delivery system, has excellent potential for alleviating inflammatory arthritis by blocking MMP-13 and RANKL.

Antimicrobial effect of two fluoride-releasing adhesive tapes on Streptococcus mutans biofilm.

Fluoride-releasing adhesive tapes have been developed as a new fluoride delivery agent. However, application as caries prevention agents remains underexplored. This study aimed at evaluating the antimicrobial activity of two fluoride-releasing adhesive tapes against S. mutans biofilm. Two polyvinyl alcohol (PVA) tapes were investigated: (i) a fluoride-PVA (F-PVA) tape, (ii) a pullulan incorporated F-PVA (PF-PVA) tape. S. mutan strains were cultured and treated with the tapes. Antimicrobial effects were evaluated using the agar diffusion test, field-emission scanning electron microscopy (FE-SEM), and confocal laser scanning microscopy (CLSM). F-PVA tapes showed higher inhibition-zone diameters than PF-PVA at 48 h and 72 h. However, there were no significant differences (p > 0.05) between the effects of F-PVA and PF-PVA. The bio-volume of S. mutans and extracellular polymeric substances significantly decreased in the F-PVA tapes than in the PF-PVA tapes (p < 0.05). FE-SEM micrographs revealed less S. mutans colonization in F-PVA. F-PVA exhibited better antimicrobial activity against S. mutans than PF-PVA.