This study explored the development of polyvinylpyrrolidone (PVP)–honey-gel (PHG) through 3D printing, aiming to develop a multifunctional bio-tape with adhesive and degradable properties. Based on the potential of honey to promote wound healing due to its antibacterial and anti-inflammatory properties, a PVP–honey-based 3D printing ink was developed by combining honey and PVP to create PHG through 3D printing technology that can form a film with strong adhesion and flexibility. First, the chemical–physical properties of PHG and its 3D printing performance were characterized. The line width achievable in 3D printing for the PHG line can extend to ∼100 µm. In addition, the adhesive properties of the PHG film were evaluated by using a 180° peeling test on various materials (glass, copper, wood, and pig skin), highlighting its potential for diverse applications. Finally, the application of the PHG film as a bio-tape was demonstrated through a successful animal experiment on a rabbit’s skin wound. Due to its adhesive and degradable properties, the bio-tape exhibited 3D conformability and ease of removal without residue.

Due to its antibacterial, anti-inflammatory, and antioxidant properties, honey has been extensively studied for centuries regarding its role in promoting wound healing.1–3 Research has identified several factors contributing to its outstanding antibacterial effects, including high sugar content, low moisture content, low pH value, and the presence of endogenous hydrogen peroxide in honey.4 The high sugar and other solutes in honey create a potent osmotic gradient, facilitating fluid movement into subcutaneous tissues and promoting the healing process at the wound’s base. Moreover, the elevated sugar content in honey serves as an additional source of glucose for cell proliferation, supporting fibroblasts and endothelial cells, thereby enhancing the biological processes of wound healing.5 These unique properties position honey as a promising natural wound treatment, providing comprehensive support and protection for wounds.

Despite honey’s extensive historical use in wound healing, challenges arise when directly applying it to the wound bed, as it gradually drains over time, causing patient discomfort.6 The predominant clinical approach involves directly applying honey to the wound and covering it with gauze. However, this method proves highly inefficient, requiring multiple applications and dressing changes to maintain honey at the wound site.

Honey-incorporated nanoparticles/nanofibers offer potential for wound healing, with numerous recent studies exploring honey-based nanoparticle wound dressings incorporating materials such as gold, silver, chitosan, and cellulose.7–14 The primary challenge with honey-based nanoparticles lies in the crucial need to identify the molecules in honey responsible for metal reduction and determine suitable honey formulations for nanoparticle production. Hydrogels represent another emerging method for utilizing honey in wound dressing, gaining popularity due to their enhanced wound healing activity.15–20 Noori et al. developed and evaluated a novel wound dressing composed of poly(vinyl alcohol) (PVA)/chitosan/honey/clay.21 A similar study by Rafati et al. demonstrated honey-loaded bionanocomposite hydrogels based on egg white, PVA, and clay.22 Fathollahipour and team explored cross-linked hydrogels based on PVA, incorporating honey and sucrose, for the delivery of erythromycin.23 Stojkovska et al. reported the simultaneous application of alginate hydrogels, incorporating Ag-nanoparticles (NPs) and honey components, for the purpose of addressing multidrug-resistant bacterial strains responsible for nosocomial wound infections.24 These fundamental discoveries are in harmony with research, suggesting that the integration of honey and hydrogels, when implemented under optimal conditions, amplifies the efficacy of honey in the process of wound healing. Despite these promising results, additional research is required to further simplify the fabrication process and enhance its application.

Polyvinylpyrrolidone (PVP) is a synthetic water-soluble polymer material with film-forming, adhesive, hygroscopic, solubilizing, and coagulating properties, which has excellent solubility and physiological compatibility properties. In 3D printing technology, it can serve as a sacrificial layer. However, at low humidities, PVP materials are in a glassy state, making them extremely prone to fracturing, limiting their further applications. At high humidities, PVP materials are in a viscous state and have strong adhesion ability. Honey possesses strong moisturizing properties. Honey fillers can be added to PVP to improve its toughness, further enhancing its usability. Based on this discovery, this study developed a PVP–honey-based 3D printing ink (PH-ink), which is a mixture of PVP and honey. The preparation process is illustrated in Fig. 1(a). After chemical–physical characterization, the PVP–honey-gel (PHG) film was easily 3D printed as shown in Fig. 1(a). Due to its strong adhesive properties in a viscous state, the PHG film can adhere shape-conformingly to tissues without impeding their normal activities, which could serve as a bio-tape, as shown in Figs. 1(a) and 1(b).

FIG. 1.

PHG-based bio-tape. (a) Conceptual illustration of the preparation of PH-ink. (b) 3D printing of the PHG. (c) The application of the PHG-based bio-tape. PVP, polyvinylpyrrolidone; PHG, PVP–honey-gel; PH-ink, PVP–honey-based 3D printing ink.

FIG. 1.

PHG-based bio-tape. (a) Conceptual illustration of the preparation of PH-ink. (b) 3D printing of the PHG. (c) The application of the PHG-based bio-tape. PVP, polyvinylpyrrolidone; PHG, PVP–honey-gel; PH-ink, PVP–honey-based 3D printing ink.

Close modal

Attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopy was utilized to study the changes in the polymer structure of the thin PHG film prepared by 3D printing technology. PVP and honey were mixed with a weight ratio (w/w) of 2:1, 4:1, and 5:1, respectively. The ATR-FTIR spectra were recorded in the range of 4000–400 cm−1 in the transmittance mode, and the results are shown in Fig. 2(a). Table S1 of the supplementary material summarizes the characteristic peaks of pure PVP and its composites.25–30 Overall, the spectra of composites were highly similar between the samples. However, the spectra of the composites were slightly different from those of pure PVP and very different from those of pure honey. In particular, a broad band over 3000–3700 cm−1 was observed for the pure PVP. This band was attributed to the O–H stretching because the mesomeric structure of PVP enables hydrogen bonding to the C=O groups between the pyrrolidone rings in the presence of moisture where the stretching vibration peak of C=O (amine I) was confirmed by the strong band located at ∼1642 cm−1.25 This band was also observed in all the spectra with some differences in the width, intensity, and peak position. For example, the pure PVP showed a narrower width and less intensity compared with the composites and pure honey. In addition, the peaks of pure PVP that were located at 3393 and 3285 cm−1 were shifted to 3372 and 3264 cm−1 after compositing with pure honey, which exhibited a peak at 3272 cm−1. The formation of hydrogen bonds between the OH groups of honey and the C=O groups of PVP was indicated by the somewhat lower frequency shift of the C=O groups in the pyrrolidone ring in the composites compared with the pure PVP. The peaks from 2990 to 2910 cm−1 were attributed to the asymmetric and symmetric stretching vibrations of the C–H bond in CH2.26 Similarly, the peaks of spectra of the composites in this range exhibited a slight shift toward lower frequencies, which indicated specific interactions in the PVP matrix. The peak located at 2873 cm−1 was assigned to the symmetric stretching of CH3 (tertiary C–H stretching). Clear absorption peaks in the PVP and the composites from 1400 to 1480 cm−1 were produced by the wagging vibration of –CH2 in the PVP.26 The stretching of C–N in the PVP was also observed at 1289 cm−1. In addition, the peak located at 570 cm−1 was attributed to the bending of N–C=O in PVP. The corresponding peaks in the spectra of composites shifted to a lower frequency, which proved once again that the interaction of honey and PVP could be produced at the groups of C=O in PVP. As can be observed, the spectrum of pure honey shows five primary individual regions at 3000–3700, 2800–300, 1700–1600, 1540–1175, 1175–940, and 940–500 cm−1, which is fully consistent with the findings of previous studies.27 After the incorporation of honey in the PVP, an additional band in the spectra of all the composites was observed that was particularly pronounced at the range of 1175–940 cm−1, which was ascribed to the C–O and C–C stretching of carbohydrates. Therefore, the groups of C–O, C–C, and OH in honey strongly interacted with the groups of C=O and CH2 in PVP that induced structural rearrangements to the polymer matrix that led to a significant enhancement in its mechanical properties.

FIG. 2.

Chemical–physical characterization of the PHG. (a) ATR-FTIR spectroscopy of the PHG in the range of 4000–400 cm−1. (b) Weight loss curve of PHG from 20 to 600 °C. (c) PHG SEM images of PHG samples after freeze-drying. ATR-FTIR, attenuated total reflectance-Fourier transform infrared; PVP, polyvinylpyrrolidone; PHG, PVP–honey-gel.

FIG. 2.

Chemical–physical characterization of the PHG. (a) ATR-FTIR spectroscopy of the PHG in the range of 4000–400 cm−1. (b) Weight loss curve of PHG from 20 to 600 °C. (c) PHG SEM images of PHG samples after freeze-drying. ATR-FTIR, attenuated total reflectance-Fourier transform infrared; PVP, polyvinylpyrrolidone; PHG, PVP–honey-gel.

Close modal

As shown in Fig. 2(b), compared with the smooth descent curve for pure PVP, the PHG weight loss curve was divided into four descending segments: (1) during the period of 20–150 °C, the adsorbed water of the product escaped, which resulted in a weight loss rate of 15%. This is due to the fact that the deionized water in the sample did not completely evaporate during the preparation process. (2) The weight loss curve was gently flat between 150 and 210 °C, and there was only a small amount of mass loss, which could possibly be owing to the coupling of PVP and honey that locked the crystal water. (3) The percentage of mass loss between 210 and 400 °C was 20%, while the weight loss curve suddenly changed in the front section and started to flatten at ∼350 °C, indicating that the samples began to thermally degrade. Typically, most organic matter begins to oxidize and decompose at 250–300 °C. Combined with the weight loss curve of PVP, it was apparent that honey began to decompose, and the coupling between PVP and honey was destroyed, while the crystal water escaped. (4) The mass between 400 and 600 °C was reduced to ∼10%. The rest of the PVP began to decompose. The decomposition of PHG was basically completed until 500 °C, and the quality gradually tended to be stable. Overall, PHG maintained a good capacity of water absorption and holding, as well as thermal stability below 200 °C.

In general, the self-assembly and subsequent phase separation of polymers could construct micro-/nanostructures during the processing of formation, which provide a simple approach to characterize the mechanical properties of the PHG. As shown in Fig. 2(c), all the freeze-dried PHG were observed by scanning electron microscopy (SEM) to exhibit structures with nanometer-sized pores. Moreover, the pores decreased with the increase in content of honey, which could have originated from the following: (1) the water absorption of the prepared PHG was also enhanced with the increase in the content of honey, while some moisture was absorbed at the end of freeze-drying and before entering the scanning electron microscope, and (2) the water of crystallization was found in the PHG plastic-like hydrogel, which could be the reason why it was able to remain flexible for a long time. Generally speaking, the addition of honey fixed more water in the interior of the PHG in the form of crystal water so that the PHG polymer-gel could exhibit long-term flexibility and adhesion ability.

As mentioned earlier, the addition of honey to pure PVP can enhance its mechanical properties. To quantitatively analyze the printing performance of the PH-ink, we investigated various factors influencing the PHG line resolution, including the nozzle diameter (D), the printing speed (v), the pneumatic nozzle pressure (p), and the distance between the nozzle and substrate (d). After applying pressure, the PH-ink was squeezed out through the nozzle and reached an equilibrium state. The extruded PH-ink contacted the substrate, adhering to it to form PHG as shown in Fig. 1(b). Figures 3(a)3(c) depicted the variation in the width of the printed PHG line with changes in p, where d, v, and D are varied. When v is 7 mm/s and D is 160 μm, the width of the constructed PHG line increased with an increase in d. A decrease in d led to PH-ink accumulation, affecting the flow rate of the PH-ink ink. As d increases, the resistance to extruding the PH-ink decreased. The PH-ink gradually diffused from both sides of the PHG line during the printing process. With other parameters held constant, the flow rate of the extruded PH-ink per unit path length decreased with an increase in v, resulting in a narrowing of the PHG line, as shown in Fig. 3(b). The nozzle diameter D also affected the precision of the printing PHG line. Nozzles with the diameter ranging from 160 to 510 μm were used. Figure 3(c) shows the width of the constructed PHG line with different nozzle diameters. The width of the constructed PHG line decreased with a reduction in D. After optimization, the smallest width of the PHG line is ∼100 μm, with the following printing parameters: D, 160 μm; d, 0.05 mm; p, 0.035 MPa; and v, 7 mm/s). When D is less than 160 μm, even with a high pneumatic nozzle pressure of 0.6 MPa (the pressure limit of the 3D bioprinter: 0.6 MPa), the PH-ink cannot be extruded from the nozzle due to its high viscosity. Based on the above analysis, the printing resolution of the PHG can be further improved by decreasing D, p, and d or by increasing v. To further validate the applicability of the 3D printing PHG, PHG films with various patterns are presented as shown in Fig. 3(d). Figure 3(e) illustrates a printed PHG film with the penguin pattern. Due to its strong adhesion, it easily adhered to the skin and exhibited the 3D conformability. In addition, because of the water solubility of PVP and honey, the PHG film attached on the skin can be easily degraded and cleaned with water. The PHG has good mechanical properties at 40%–60% humidity. Only when the humidity exceeds 70%, the gel becomes viscous.31 After attaching the PHG film to one side of the cheek, it did not affect the film even when the surface of the cheek was covered with sweat. It means that the PHG is stable in water-rich environments.

FIG. 3.

3D printing of the PHG. (a) Investigating the PHG line width in relation to pressure across different distances between the nozzle and substrate, maintaining a printing speed of 7 mm/s and a nozzle diameter of 160 µm. (b) Investigating the PHG line width in relation to pressure across different printing speeds, maintaining a distance of 0.05 mm and a nozzle diameter of 160 μm. (c) Investigating the PHG line width in relation to pressure across different nozzle diameters, maintaining a distance of 0.05 mm and a printing speed of 7 mm/s. (d) PHG-based films with various patterns. (e) 3D conformal capability and degradability of the printed the PHG-based film with the penguin pattern attached on the skin.

FIG. 3.

3D printing of the PHG. (a) Investigating the PHG line width in relation to pressure across different distances between the nozzle and substrate, maintaining a printing speed of 7 mm/s and a nozzle diameter of 160 µm. (b) Investigating the PHG line width in relation to pressure across different printing speeds, maintaining a distance of 0.05 mm and a nozzle diameter of 160 μm. (c) Investigating the PHG line width in relation to pressure across different nozzle diameters, maintaining a distance of 0.05 mm and a printing speed of 7 mm/s. (d) PHG-based films with various patterns. (e) 3D conformal capability and degradability of the printed the PHG-based film with the penguin pattern attached on the skin.

Close modal

The main components of honey are fructose and glucose, accounting for more than 60% of the total components, with a mass ratio of ∼1:1. To prove the role of fructose and glucose in PHG, PVP–glucose composite, PVP–honey composite, and PVP–fructose composite were prepared in our previous work.31 The self-conformal ability and the adhesion performance of PVP glucose composite is not as good as that of PVP–honey composite and PVP–fructose composite. However, since the PVP–fructose composite is in a viscous state, it is difficult to peel the PVP–fructose composite from the skin. Fructose can greatly improve the stretchability of PVP. However, the poor formability of the PVP–fructose composite makes its use as a base material for bio-tape difficult. A 180° peeling test was performed on different materials to quantitatively assess the adhesion ability of PHG as shown in Fig. 4(a). It was apparent that the PHG dry film could adhere to various materials, including glass, copper, wood, and pig skin as shown in Figs. 4(b) and 4(c). As seen from Figs. 4(d) and 4(e), the peel strength was larger for smoother objects and smaller for rougher objects, whereas the peel strength for bio-skin (pig skin) was ∼100 N/m, which was similar to that of medical tape. This led us to prepare a type of bio-tape for ordinary wounds. The bio-tape consisted of bonding polyethylene (PE) film and PHG film, which not only ensured the transparency and viscosity but also ensured the toughness of the tape. To test the performance of the PHG bio-tape in a clinical setting, we designed an animal experiment as shown in Fig. 5. Prior to sealing with the PHG bio-tape, a 20 mm long incision was created on the back of a rabbit with a scalpel and sterilized with medicinal alcohol. In this study, the seamless interface could be explained by a dry cross-linking mechanism.32,33 An instant bond was formed by the PHG bio-tape adsorbed water in alcohol at first, and then, the polymer chains would quickly entangle, as well as cross-link with the tissue surface, to achieve topological adhesion as shown in Fig. 5(b). The topological adhesion could ensure that the blood had difficulty overflowing without affecting the normal activities of humans. In fact, the healing process of the wound on back of the rabbit in 1, 3, and 5 days is shown in Fig. 5(c). A clear and tight interface was formed between the PHG bio-tape and skin, which confirmed its tough and topological interfacial bonding. In particular, an alcohol-washing method was used to remove the bio-tape, which could simply degrade and remove the PHG bio-tape to ensure that there was no residue left. No obvious signs of damage or inflammation were observed when the PHG bio-tape was replaced with a new one every other day, further indicating the excellent biocompatibility of the PHG. In addition, PHG can be designed into a porous film to improve its air permeability in the application of bio-tape.

FIG. 4.

The 180° peel test of the PHG film. (a) Schematic diagram of the 180° peel test of the PHG film. (b) 180° peel test of the PHG film adhered on (b) the glass and (c) the pig skin. (d) The 180° peel (d) force and (e) average force of the PHG film adhered on various materials, including glass, copper, wood, and pig skin.

FIG. 4.

The 180° peel test of the PHG film. (a) Schematic diagram of the 180° peel test of the PHG film. (b) 180° peel test of the PHG film adhered on (b) the glass and (c) the pig skin. (d) The 180° peel (d) force and (e) average force of the PHG film adhered on various materials, including glass, copper, wood, and pig skin.

Close modal
FIG. 5.

Mechanism of the PHG bio-tape. (a) Demonstration of the PHG bio-tape adhering to the rabbit skin. (b) A schematic diagram of the application of PHG bio-tape. (c) The effect of PHG bio-tape adhering on the rabbit skin wound in 5 days.

FIG. 5.

Mechanism of the PHG bio-tape. (a) Demonstration of the PHG bio-tape adhering to the rabbit skin. (b) A schematic diagram of the application of PHG bio-tape. (c) The effect of PHG bio-tape adhering on the rabbit skin wound in 5 days.

Close modal

In summary, the study explored the synergistic properties of honey and PVP in creating a versatile and effective bio-tape for wound care. First, the analysis of the chemical–physical properties revealed intricate interactions between honey and PVP, influencing the polymer structure and enhancing mechanical properties. After chemical–physical characterization, the 3D printing parameters were optimized, enabling the production of PHG lines with a width as small as 100 μm. The adhesive properties of the printed PHG film were systematically evaluated on various materials, emphasizing its potential for widespread applications. Finally, the study introduced a bio-tape comprising PHG and a polyethylene film, exhibiting strong adhesion to the skin. The application of the bio-tape on a rabbit skin substantiated its efficacy in wound healing, with a seamless interface formed through a topological adhesion mechanism. The bio-tape’s ability to adhere to the skin tightly, promoting wound healing without adverse effects, establishes its potential for clinical use.

Materials were sourced from suppliers in China. Natural honey, toluidine blue/polyvinylpyrrolidone (PVP-K90), and PE plastic wrap/3D printed blue masking paper were, respectively, purchased from the Anhui Susong County Liu’s Bee Products Co., Ltd., Hefei Qiansheng Biotechnology Co., Ltd., and Shenzhen Mingtai 3D Technology Co., Ltd.

Honey, PVP, and deionized water were mixed in a weight ratio of 1:2:15. After standing for 48 h in a dust-free environment at room temperature, honey and PVP were fully dissolved to form a uniform colloid, which can be used as the PH-ink.

1. SEM

The morphologies of the lyophilized PHG were observed by scanning electron microscopy (SEM) (SU5000; Hitachi, Tokyo, Japan). Before observation with the SEM, the PHG film was placed in an environment of 20 °C and 60% humidity for more than 24 h, while they were freeze-dried for 18 h in a freeze vacuum drier and coated with a thin layer of gold.

2. Thermal gravimetric analyzer

The moisture content and thermal stability of various PHG films were quantified using a thermal gravimetric analyzer (TGA) (TG209; NETZSCH, Selb, Germany). It was significant to calibrate the balance to quantitatively estimate the mass changes before the experiments, and the flow rate of nitrogen through the sample was kept constant at 40 ml/min. In addition, all the experiments were conducted in the temperature range of 20–600 °C and at a 10 °C min−1 heating rate with a sample size of ∼5 mg.

3. ATR-FTIR

The copolymer structure change of the as-prepared PHG film with the coupling of honey was quantified by ATR-FTIR spectroscopy. All the PHG samples were made into small flakes (10 mm in diameter and 0.3 mm in thickness) before the experiments and placed in ∼60% humidity for more than 24 h. In addition, the ATR-FTIR spectra were recorded in the range of 4000–400 cm−1 in the transmittance mode.

4. Peel strength

The 3D printed blue masking paper were bonded with the back of the PHG film as stiff backings to prevent the PHG samples from stretching along the peeling direction before the 180° peeling test. The adhered surface was prepared by the pre-prepared PHG film and pressing it on the substrate with a 2 kg weight for 10 s. Finally, the interfacial toughness of the PHG films were determined using a Shimadzu AGS-X machine and quantified using standard 180° peeling tests at a constant peeling speed of 300 mm min−1 with a peel distance of 25 mm.

The rabbit experiment was strictly compliant with the standard guidelines approved by the Ningbo University Ethics Committee (Ningbo, China), and the interrelated operations were reviewed and approved by the Committee on Animal Care.

All supplementary material is posted online exactly as provided by the author.

This study was supported by the Natural Science Foundation of Ningbo city, China (Grant No. 2023J010), and Natural Science Foundation of China (Grant No. 52275343). It was also supported by the Fundamental Research Funds for the Provincial Universities of Zhejiang (Grant No. SJLY2024007).

The authors have no conflicts to disclose.

S.H. and Y.L. contributed equally to this work.

Shilong Hu: Conceptualization (equal); Data curation (equal); Formal analysis (equal); Visualization (equal); Writing – original draft (equal). Yan Liu: Conceptualization (equal); Data curation (equal); Supervision (equal); Validation (equal); Visualization (equal). Zhengzhou Yin: Supervision (equal); Validation (equal); Visualization (equal). Husheng Chen: Conceptualization (equal); Data curation (equal); Formal analysis (equal); Methodology (equal). Yuan Jin: Supervision (equal); Validation (equal); Visualization (equal). Minghua Zhang: Supervision (equal); Validation (equal); Visualization (equal). Licheng Hua: Supervision (equal); Validation (equal); Visualization (equal). Jianke Du: Supervision (equal); Validation (equal); Visualization (equal); Writing – review & editing (supporting). Guangyong Li: Conceptualization (equal); Funding acquisition (lead); Writing – original draft (equal); Writing – review & editing (lead).

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

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