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Article

Green Surface Engineering of Spun-Bonded Nonwovens Using Polyphenol-Rich Berry Extracts for Bioactive and Functional Applications

by
Karolina Gzyra-Jagieła
1,*,
Bartosz Kopyciński
2,3,
Piotr Czarnecki
1,
Sławomir Kęska
1,
Natalia Słabęcka
4,
Anna Bednarowicz
1,
Nina Tarzyńska
1,
Dorota Zielińska
1,
Longina Madej-Kiełbik
1 and
Patryk Śniarowski
1,5
1
Łukasiewicz Research Network—Łódź Institute of Technology, Marii Skłodowskiej-Curie 19/27 St., 90-570 Łódź, Poland
2
Łukasiewicz Research Network—Institute of Polymer Materials, Marii Skłodowskiej-Curie 55 St., 87-100 Toruń, Poland
3
Doctoral School, Silesian University of Technology, Akademicka 2A St., 44-100 Gliwice, Poland
4
Institute of Materials Science and Engineering, Faculty of Mechanical Engineering, Łódź University of Technology, Żeromskiego 116 St., 90-924 Łódź, Poland
5
Doctoral School, Institute of Materials Science and Engineering, Lodz University of Technology, 1/15 Stefanowskiego St., 90-924 Lodz, Poland
*
Author to whom correspondence should be addressed.
Eng 2026, 7(1), 49; https://doi.org/10.3390/eng7010049
Submission received: 31 October 2025 / Revised: 7 January 2026 / Accepted: 10 January 2026 / Published: 16 January 2026
(This article belongs to the Special Issue Fibres and Textiles: Innovations, Engineering, and Sustainability—in Memory of Professor Izabella Krucińska (1953–2023))
Browse Figures
Review Reports Versions Notes

Abstract

In response to the growing demand for environmentally friendly and sustainable yet functional technical textiles, this research developed a spun-bonded nonwoven from the biodegradable thermoplastic starch-based biopolymer BIOPLAST®, incorporating fruit extracts as natural sources of polyphenolic compounds and surface-active additives. Extracts from Vaccinium myrtillus L. and Sambucus nigra L. were applied onto a nonwoven’s surface via aerographic spraying using a water/ethanol system. The resulting materials were characterized in terms of morphology, physicochemical and mechanical behavior, surface characteristics, and stability under accelerated ageing and hydrolytic conditions. Treatment with the extracts increased the tensile strength by roughly 38% and elongation at break by about 50%, and it changed the surface from hydrophobic (contact angle of 115°) to hydrophilic, with contact angles of 83° for the blueberry-modified nonwoven and 55° for the elderberry-modified nonwoven. The modified nonwovens also showed sustained release of polyphenolic compounds over 72 h, which is beneficial for biomedical, healthcare, and cosmetic applications, where short-term use, controlled release of active compounds, and bioactivity are more important than long-term durability. Overall, the results indicate that BIOPLAST®-based spun-bonded nonwovens can serve as fully bio-based carriers for fruit extracts in MedTech-related technical textiles, offering a straightforward way to introduce additional functionality into biodegradable nonwovens.

1. Introduction

In recent years, there has been growing interest in the development of bioactive materials that exhibit various biological properties, such as antioxidant [1,2,3], antibacterial [4,5,6], and anti-inflammatory activities [7,8,9]. One research direction involves the surface modification of polymeric materials using natural plant extracts rich in phenolic compounds, with well-documented biological potential [10,11,12].
Natural polyphenols, found for example in berry fruits such as blueberries, chokeberries, and cranberries, represent a rich source of compounds with potent antioxidant and antimicrobial properties [13,14,15]. Anthocyanins, flavonoids, and phenolic acids are recognized for their valuable health-promoting properties [16,17,18,19]. Nevertheless, even with their strong biological potential, maintaining a stable association between polyphenols and polymer surfaces remains challenging. The literature offers differing views on the mechanisms involved. While several authors attribute the interactions mainly to hydrogen bonding and hydrophobic forces, others underline the importance of covalent linkages arising from oxidative polymerization [20,21,22,23].
In most studies on the functionalization of polymeric materials with bioactive compounds, additional surface activation steps such as plasma or chemical treatments are employed to enhance coating adhesion [24,25,26]. However, in recent years, spray coating has gained popularity as a simple and efficient technique for depositing functional layers onto polymer surfaces [27,28,29]. This process enables the even application of bioactive solutions or dispersions onto substrates with complex geometries, such as nonwovens, while keeping both material consumption and energy use low [30,31,32,33]. One of its main advantages is that it operates under gentle thermal and chemical conditions, allowing natural plant extracts to be deposited without damaging their active components [34,35,36]. Therefore, spray coating represents an environmentally friendly alternative to conventional surface functionalization methods that require activation steps or the use of aggressive reagents.
The nonwoven industry is one of the most innovative and rapidly developing sectors within the global fiber market. Spun-bonded and melt-blown technologies enable the production of technical textiles with uniform fiber diameters and strong mechanical performance, supporting applications in filtration, hygiene, medical, construction, and packaging. A significant advantage of technical textiles is their capacity for functional enhancement through surface modification or the addition of active additives, which allows tailoring properties such as wettability, antimicrobial activity, biocompatibility, or controlled release of substances to meet advanced performance requirements [37]. Due to their porous structure, large specific surface area, and favorable mechanical properties, they provide an excellent platform for the deposition of bioactive coating [38,39,40]. For this reason, they have attracted increasing attention in biomedical, filtration, and hygiene applications and even camouflage applications [41,42,43,44]. The BIOPLAST® polymer developed by BIOTEC represents an interesting approach as a biodegradable raw material. Owing to its thermoplastic starch-based composition and biodegradability, BIOPLAST® is particularly attractive as a sustainable alternative to conventional polypropylene nonwovens. In addition, its good melt processability and compatibility with water/ethanol-based systems make it a suitable matrix for surface functionalization with natural plant extracts. Research has been conducted on the production of BIOPLAST® films using various processing methods [45,46,47] as well as the fabrication of molded or extruded parts containing organic fillers [48,49,50,51]. The material can be employed both as a single-component polymer and in multicomponent systems that include other biopolymers or organic fillers.
In textile applications, such as fiber, nonwoven, and fabric production, BIOPLAST® has not yet been widely used. Although the manufacturer lists such processing routes as potential applications, there is limited research in this area. In melt processing techniques, the addition of glycerol has been found necessary to facilitate fiber formation, as the polymer alone is complex to spin [52]. BIOPLAST® is relatively new to the biopolymer market compared with PLA, PCL, or PBS. The manufacturer primarily recommended it for foils or extrusion techniques outside the textile sector. The textile industry is beginning to be considered a potential field of application for this material, with the producer simultaneously introducing targeted modifications to support fiber-forming processes. However, developing an effective processing methodology for such a demanding technology as fiber production requires extensive research and optimization efforts. Limited information is currently available on the applicability of this polymer in textile manufacturing, mainly due to challenges associated with its textile processing behavior.
In the context of increasing demands for sustainability and the reduction of environmental impact in the textile industry, the search for “green” methods of polymer surface modification has become particularly important [53,54]. The use of natural plant extracts as sources of bioactive compounds, combined with low-energy coating processes, aligns well with the principles of green chemistry and surface engineering. In this study, the spray coating technique was used to deposit polyphenol-rich extracts onto spun-bonded nonwovens without chemical modification of the substrate. The technique offers an efficient and low-cost route to surface modification. Because the modifying agents are only physically adsorbed on the fiber surface, they can be gradually released from the nonwoven structure, which acts as a reservoir for the active compounds. In addition, the spray coating process is safe for sensitive compounds that may degrade and thereby lose their biological activity.
This work bridges innovative material engineering with the principles of sustainable development, paving the way for new opportunities in the design of advanced, functional, and environmentally friendly textiles. By utilizing the BIOPLAST® polymer, a uniform spun-bonded web could be produced, even though this material is seldom employed in such processing techniques. This achievement demonstrates the potential of biopolymer-based systems to replace conventional synthetic polymers in nonwoven production, thereby contributing to the development of more sustainable, eco-conscious textile solutions. Moreover, the obtained material enabled surface modification with plant extracts known for their pro-health properties, thereby enhancing its functionality and potential applications. Significantly, this modification did not compromise the material’s ecological character but rather strengthened its sustainable and bioactive profile.

2. Materials and Methods

2.1. Spun-Bonded Nonwoven

Nonwoven samples were prepared from the biodegradable polymer BIOPLAST® EL350 (BIOTEC Biologische Naturverpackungen GmbH & Co., Emmerich am Rhein, North Rhine-Westphalia, Germany), using a spun-bonding process carried out directly on the neat biopolymer. BIOPLAST® is a bio-based material composed of a thermoplastic starch blend. This polymer was selected because its high renewable content, biodegradability, and melt spinnability allowed us to explore a bio-based alternative to conventional polypropylene nonwovens while using standard processing equipment. The nonwoven was produced on a pilot-scale line developed at the Łukasiewicz Research Network’s Łódź Institute of Technology in Poland (Figure 1A) [55]. During processing, the extrusion temperature ranged from about 170 °C to 250 °C, and the spinneret head was maintained at 250 ± 5 °C throughout the run. Air at 22 °C and 1550 Pa was supplied to the cooling chamber, and the calender rolls were set to operate at 50 ± 2 °C. The spinneret used in the spun bonding line comprised 467 holes with a diameter of 0.4 mm each. Before spinning, the polymer pellets were dried for 13 h in a rotary dryer (Fourné Maschinenbau GmbH, Alfter, Germany) at 55 ± 5 °C.

2.2. Preparation of Extracts from Vaccinium myrtillus L. and Sambucus nigra L.

The preparation of the extracts followed the general procedure outlined in the authors’ earlier research [56] (Figure 1B). European blueberry (Vaccinium myrtillus L.) fruits were collected in the Lubliniec forests of Poland. In contrast, European black elderberry (Sambucus nigra L.) was harvested from meadows and agricultural fields in the surrounding area (50°39′54.9″ N, 18°37′58.7″ E) during July and August 2021. All plant materials were hand-harvested, rinsed with running water, air-dried, and stored under cool conditions until further processing.
A solvent mixture of equal volumes of deionized water and 96% ethanol (v/v) was chosen. Prior to extraction, the fruits were frozen at −80 °C for three hours (ULUF 65, Arctiko, Salisbury, UK) and then lyophilized for 96 h at 28 °C under reduced pressure (Alpha 2-4 LDplus, CHRIST, Osterode am Harz, Germany). The dried materials were ground in an agate mortar and subsequently dissolved at a concentration of 0.1 g of dry mass per 1 mL of solvent.
The resulting suspensions were subjected to 24 h of maceration, followed by sonication in an ice bath for 40 min (Sonic-6, Polsonic, Warsaw, Poland). The final extracts were centrifuged at 5000 rpm for one hour (MPW 351/R/RH, MPW MED Instruments, Warsaw, Poland), and the obtained supernatants were carefully collected and filtered before use.

2.3. Surface Functionalization

The extracts obtained from Vaccinium myrtillus L. and Sambucus nigra L. were deposited onto spun-bonded BIOPLAST® nonwoven fabrics using an aerographic spray coating technique (Figure 1C). The nonwoven material used in this study had a basis weight of 49.3 ± 3.0 g/m2 and a thickness of 0.28 ± 0.01 mm. The coating process was carried out with a laboratory airbrush (BD-158S, Fengda, Ningbo, China) connected to an automatic compressor. The extracts were applied through a 1.0 mm nozzle at a working pressure of 4 bar. Strips of nonwoven fabric 500 mm wide were utilized for mechanical and physical testing and to ensure uniform extract distribution. During coating, the spraying distance was maintained at 200 ± 20 mm.
Following surface treatment, the functionalized nonwovens were air-dried at ambient temperature (approximately 23 °C) for 24 h. Subsequently, the samples were subjected to mechanical property evaluation and examined to determine the release behavior of the active components from the fibrous structure. The application of this technique enables the production of a nonwoven in which the extracts are physically adsorbed onto the fiber surface rather than covalently bonded. Such a system, based on physical interactions, facilitates the release of active compounds, making the spun-bonded nonwoven an effective controlled-release matrix.

2.4. Methods

The mechanical properties of the spun-bonded nonwovens were tested under controlled laboratory conditions at 20 ± 2 °C and 65 ± 4% relative humidity, in accordance with PN-EN ISO 139:2006 [57]. The thickness of the samples was measured according to PN-EN ISO 9073-2:2002 using a TILMET-64 thickness gauge (Łódź University of Technology, Łódź, Poland) while applying a constant pressure of 0.5 kPa during the measurements [58]. The surface mass was measured according to PN-EN 29073-1:1994 [59]. The tensile strength and elongation at break in the longitudinal direction were tested on conditioned samples in accordance with PN-EN 29073-3:1994 using a universal testing machine (Instron 5544, Norwood, MA, USA) [60].
Spectroscopic analysis was carried out using a Nicolet iS50 FTIR spectrometer (Thermo Scientific, Waltham, MA, USA) equipped with an attenuated total reflection (ATR) accessory. Spectra were recorded in the 4000–400 cm−1 range, with 32 scans averaged for both the background and the sample. The accuracy of the wavenumber for the characteristic absorption bands was within ±1 cm−1.
The molecular properties, including the weighted average molar mass (Mw), dispersity index (DI), and molar mass distribution, were analyzed via gel permeation/size exclusion chromatography (GPC/SEC). The GPC/SEC measurements were performed using an Agilent chromatographic system (Agilent Technologies, Santa Clara, CA, USA) equipped with an Optilab refractive index detector (Wyatt Technology, Goleta, CA, USA). Polymer separation was performed on a PLgel Mixed-C column (300 mm, Agilent Technologies) while using chloroform as the mobile phase. Calibration of the system was performed against a set of polystyrene standards.
The morphology of the nonwoven surface was examined using a Quanta 200 scanning electron microscope (SEM) (FEI, Eindhoven, The Netherlands) operated at 10 kV.
Surface tension measurements were conducted at 20 °C while using a stalagmometer with distilled water as the reference liquid. The density of the berry extracts was determined with a pycnometer at 20 ± 1 °C. Contact angle measurements were performed using a goniometer (STFI, AB Lorentzen-Wettre, Kista, Sweden) equipped with an Optical Smart 5MP PRO camera (Delta Optical, Mińsk Mazowiecki, Poland). Droplet shape analysis was performed using goniometer Model 90 (Rame-Hart, Succasunna, NJ, USA ) equipped with software DROPimage Pro version 3.19.12.0. For each nonwoven variant, the contact angle was determined as the mean ± standard deviation of 10 independent water droplets deposited at different locations on the sample surface, and each measurement was averaged from the left and right angle values.
Thermal behavior was analyzed using differential scanning calorimetry (DSC) on a Diamond instrument (PerkinElmer, Waltham, MA, USA). The polymer was subjected to first- and second-heating scans and a single cooling cycle in the temperature range from −60 to 200 °C at a heating rate of 20 °C/min.
Accelerated ageing tests were carried out to evaluate how the structural and functional properties of the nonwovens changed under conditions simulating long-term storage. The procedure followed ASTM F1980–16 [61], in which simulated storage periods of 2 and 3 years corresponded to 77 and 111 days of accelerated ageing, respectively. The process was performed in a climate chamber (MK53, Binder, Tuttlingen, Germany) maintained at 55 ± 1 °C.
The ageing test describes the transformed form of the Arrhenius equation based on ASTM F1980–16:
A F F = Q 10 T A A − T R T 10
where TAA is the accelerated ageing temperature (°C), (In our study, TAA is 55 ± 1 °C), TRT is the storage temperature for the real time of ageing of the sample (°C), which in our study is 22 °C, and Q10 is the ageing factor based on the change kinetics of the selected property and material parameter at 10 °C temperature changes.
We assumed that the parameter value for the accelerated ageing factor (AAF) is 9.85.
To calculate the actual ageing time, we used the equation below:
A T T = 365 A F F
The accelerated ageing period was 77 days, corresponding to 2 years and 111 days under the applied acceleration factor, which was equivalent to 3 years in real time.
The release kinetics of the active components were investigated using a UV–Vis spectrophotometer (Evolution 220, Thermo Scientific, Waltham, MA, USA). Test flasks containing the samples were incubated in a water bath (Julabo, Seelbach, Germany) at 37 ± 1 °C. Absorbance was recorded at 282 nm for the Vaccinium myrtillus L. extract and at 268 nm for the Sambucus nigra L. extract.
Degradation in the presence of water (hydrolysis) was conducted at 37 ± 1 °C under static conditions for up to 10 weeks using a VD 23 vacuum dryer (Binder, Germany). Deionized water was used as the degradation medium (pH = 6.2; 3.7 µS/cm). Samples before and after degradation were dried to a constant weight in a VD 23 vacuum dryer (Binder, Germany) at 35 ± 1 °C and 100 mbar to minimize thermal degradation and enable assessment of the degradation progress in the tested system. A proportion of 10 ± 0.01 g of material per 100 ± 0.01 g of extraction medium was used, as this amount of water entirely covered the material. After the degradation process, the physical-mechanical parameters, molar mass, and infrared spectroscopy were investigated.

3. Results

3.1. Spun-Bonded Matrix

The nonwoven matrix was evaluated through a series of physical-mechanical tests performed in the machine direction to determine its key mechanical characteristics (Figure 1D). Overall, the material exhibited relatively low mechanical performance compared with the spun-bonded nonwovens produced from other biopolymers, such as PBS or PLA (Table 1) [62,63,64], which is consistent with the properties typically reported for materials produced using melt-blown technology [52]. Nevertheless, the good elongation at break represents a notable advantage of this material. The morphology and surface geometry of individual fibers were analyzed using SEM (Figure 2A,B). Furthermore, a statistical analysis of the fiber diameter distribution was performed to assess the uniformity and reliability of the nonwoven fabrication process.
SEM micrographs revealed a densely packed nonwoven structure composed of defect-free elementary fibers with slightly rough surfaces (Figure 2A,B). The mean fiber diameter was 23 µm (standard deviation of 2 µm), which falls within the typical 15–35 µm range reported for spun-bonded nonwovens [55,65,66,67,68,69]. Statistical analysis of the diameter distribution (Figure 2C,D) confirmed a narrow, approximately normal distribution, indicating high uniformity for the spun-bonded matrix and good reproducibility of the forming process.
Normality tests, including Kolmogorov–Smirnov (K–S), Lilliefors, and Shapiro–Wilk tests, confirmed that the distribution of fiber diameters followed a normal pattern (p > 0.20 for K–S and Lilliefors and p = 0.9986 for Shapiro–Wilk) (Figure 2C). The calculated skewness (−0.134) and kurtosis (0.76) indicated an almost symmetric distribution with a slight left-hand skew and mildly leptokurtic characteristics, suggesting a concentration of values around the mean [70]. The histogram of fiber diameter distribution (Figure 2C) exhibited a bell-shaped curve typical of a normal distribution.
The close alignment between the mean and median, combined with low skewness (−0.134), further confirmed the distribution’s symmetry and the absence of local clusters. The normal probability plot (Figure 2D) showed that the empirical data points were nearly linearly aligned with the theoretical normal distribution line, with no significant deviations or outliers.
Comprehensively, the statistical indicators, including the skewness and kurtosis, indicated an almost symmetrical, slightly flattened distribution compared with the theoretical normal distribution. The results indicate that the spun-bonded nonwoven forming process was steady and well controlled, with no noticeable fluctuations in polymer flow or interference with cooling. Statistical analyses were performed using STATISTICA software version 13.3 (TIBCO Software Inc., Palo Alto, CA, USA).

3.1.1. Simulation of the Accelerated Ageing Process

Accelerated ageing tests to assess the stability of the designed functional properties were conducted according to a procedure developed based on ASTM F1980–16 guidelines. The nonwoven samples were exposed to elevated temperatures in a climate chamber for a time defined by the Arrhenius equation. After ageing, the initial nonwoven parameters were reevaluated to determine the influence of the simulated ageing process on their structural and functional characteristics (Figure 3).
The obtained physical-mechanical parameters showed a noticeable increase with the ageing time (Figure 3A–C). The ageing process commonly leads to a decrease in these parameters, reflecting the natural degradation behavior characteristic of polymer materials [71,72,73,74,75,76,77]. However, in the present case, since the process was conducted at 55 °C, partial stabilization and crystallization of the material occurred, thereby improving the mechanical characteristics. Such an effect during ageing is not common, but depending on the material type, the additives used, or specific experimental conditions, it may appear.
Zain et al. reported that thermal ageing of HDPE composites reinforced with natural fibers increases the tensile strength [78]. Similarly, Mumenya et al. observed enhanced fiber–matrix interfacial bonding in polypropylene fabric-reinforced composites exposed to accelerated ageing conditions over time [79]. Heat treatment of polymeric materials is well known to induce secondary crystallization, which improves fiber quality and enhances physical-mechanical performance [80,81,82,83,84].
The basis weight of the nonwoven increased from 49.8 g/m2 to 54.3 g/m2 after two years of simulated ageing and to 54.6 g/m2 after three years, which also influenced the measured mechanical properties. GPC/SEC analysis was performed to assess molecular changes during accelerated ageing. The results for the weighted average molar mass (Mw) and the molar mass distribution (Figure 3D and Table 2) clearly indicate polymer degradation, a typical outcome of accelerated ageing. Based on these findings, it can be concluded that accelerated ageing resulted in approximately 20% degradation after the equivalent of two years of storage and 22% after three years, despite the observed increase in mechanical strength.
The rise in physical-mechanical parameters may therefore be attributed to structural reorganization at the supramolecular level, as suggested by the DSC results (Figure 3E). FTIR-ATR analysis also confirmed polymer degradation, a decrease in the intensity of the carbonyl stretching band at 1711 cm−1 and the bending vibration band at 1250 cm−1 was observed (Figure 3F) [85].

3.1.2. Hydrolysis of Spun-Bonded

The analysis of nonwoven hydrolysis is of great importance for potential biomedical applications, as it enables evaluation of the material’s chemical stability, durability, and safety under physiological conditions. Nonwoven fabrics used in medical applications, such as wound dressings, tissue scaffolds, and drug delivery systems, are often made from biodegradable polymers. Their degradation in the presence of water (hydrolysis) leads to polymer chain cleavage, a process that plays a critical role in maintaining functionality and biocompatibility.
Therefore, a hydrolysis experiment was conducted for the spun-bonded nonwoven material. The physico-mechanical tests confirmed the progressive degradation of the nonwoven material (Figure 4A–C). A distinct decrease in the measured parameters was observed after three weeks of hydrolysis, indicating this stage as the most critical period of degradation. With additional exposure time, only a slight reduction in mechanical properties was observed. The hydrolysis process is typically accompanied by a decline in strength, which is characteristic of biodegradable polyesters [62,86,87,88,89,90,91,92].
As a result of hydrolytic degradation, the weighted average molar mass (Mw) of the nonwovens decreased by 12% after 3 weeks, 16% after 5 weeks, and 25% after 10 weeks compared with the initial Mw of the reference sample (Table 3). The dispersity index (DI) increased from 2.55 to 4.58 after 3 weeks, indicating the formation of oligomers and lower molecular weight species, which were not observed during accelerated ageing (Table 3).
Hydrolysis involves depolymerization at the chain ends and cleavage of ester bonds within the polymer backbone. The molar mass distribution (MMD) curve (Figure 4D) showed a clear shift toward lower molecular weight fractions after 10 weeks of hydrolysis, indicating notable degradation of the polymer chains. Evidence of structural degradation was also observed in the FTIR-ATR spectra, where the characteristic absorption bands showed reduced intensity (Figure 4E).

3.2. Vaccinium myrtillus L. and Sambucus nigra L. Extracts

Having established the structural integrity of the nonwoven matrix, the next step was to characterize the berry extracts used for its surface functionalization.
Physicochemical analyses were carried out on extracts of Vaccinium myrtillus L. and Sambucus nigra L. to determine their key properties (Table 4). The densities of both fruit extracts were slightly lower than that of water at the same temperature (0.998 g/cm3). In contrast, their surface tension was more than twice that of water (72.58 mN/m), indicating strong cohesive interactions within the liquid phase. Additionally, both extracts exhibited distinctly low pH values, confirming their acidic nature.
The extract derived from Vaccinium myrtillus L. exhibited a complex, heterogeneous composition of bioactive polyphenols. The main groups of compounds detected included hydroxycinnamic acids, flavanols, flavonols, and flavonolignans, with only trace amounts of anthocyanins [56,93,94]. Among the identified constituents, hydroxybenzoic acids and their hydroxycinnamic derivatives were predominant [95,96]. Likewise, the extract obtained from Sambucus nigra L. contained a broad spectrum of biologically active polyphenols well recognised for their antioxidant and health-promoting effects.
Spectroscopic analysis using the FTIR-ATR technique revealed distinct absorption bands characteristic of polyphenolic molecular structures in both extracts (Figure 5A and Table 5) [97,98,99,100,101]. The recorded spectra were broadly comparable, suggesting that the polyphenolic composition of the two samples was similar. Due to the complexity of the extracts, as well as the structural resemblance and overlapping signals of individual phenolic constituents, FTIR-ATR was applied primarily for overall characterization rather than precise compound identification. The leading absorption bands and their corresponding functional group assignments are listed in Table 5.
It should be noted that the Sambucus nigra L. extract, which contained anthocyanins enriched in hydroxyl (-OH) functional groups, exhibited increased intensities for certain absorption bands, reflecting the strong contribution of these moieties to the spectral profile.

3.3. Surface Engineering of Spun-Bonded Nonwovens Using Extracts

The spun-bonded nonwoven fabrics functionalized with fruit extracts were tested for their physico-mechanical properties in the along direction to assess the influence of surface modification. The mass of each sample was recorded before and after aerographic spraying of the extracts, following a 24 h drying period at ambient temperature (approximately 22 °C). For the samples treated with 100% extract solutions, the deposited mass corresponded to 4.6 ± 0.4% for Vaccinium myrtillus L. and 4.4 ± 0.6% for Sambucus nigra L. The application of the plant extracts produced a uniform coloration of the previously white nonwoven matrix, resulting in a visually homogeneous and evenly coated surface (Figure 5B,C).
The wettability of the nonwoven surface was assessed via contact angle measurements (Figure 6). The unmodified nonwoven exhibited an average contact angle of 115.3 ± 7.8°, confirming its hydrophobic nature (Figure 6A). Following surface modification with plant extracts, the contact angles of both samples decreased for the sample treated with V. myrtillus L to 83.1 ± 3.4° (Figure 6B) and to 55.9 ± 2.4° for the one modified with S. nigra L. (Figure 6C). Depending on the intended application, varying degrees of surface wettability may be advantageous, for example, in wound dressings, filtration media, or hygiene-related products. In contrast, medical and cosmetic textiles generally require a certain degree of hydrophilicity, which facilitates the controlled release of active substances and promotes interaction with the skin or wound surface.
The applied fruit extracts, with low surface tension and diverse functional groups, significantly modified the surface properties of the nonwoven materials [102,103,104]. The resulting hydrophilic behavior supports the diffusion and release of bioactive compounds from the fiber matrix, enhancing the functional performance of the modified fabrics [105].
A moderate increase in nonwoven weight was observed following the application of plant extracts, reaching approximately 51.3 g/m2 for both types of modification. This change was attributed to the deposition of the extract layer on the fiber surface. No notable differences in thickness were detected compared with the unmodified reference nonwoven. In contrast, a distinct improvement in the physico-mechanical properties was recorded after surface treatment (Figure 7A–C).
The obtained results are particularly valuable, as the unmodified nonwoven fabric has a delicate structure; thus, improving its mechanical properties is beneficial for its practical applications. Similar improvements in mechanical properties have been reported in other studies on the surface modification of bio-based textile materials. The improvement observed in the modified nonwoven fabric is likely related to the formation of a thin, cohesive coating that improves fiber bonding and thus structural integrity. As a result, stresses are distributed more evenly throughout the material, allowing the fibers to withstand greater tensile loads under comparable deformation conditions [104].
Although the basis weight increased by only about 4–5% after surface treatment (from 49.8 g/m2 for the pristine material to approximately 51.3 g/m2 for both modified variants), the breaking force and tensile strength rose by roughly 38%, and the elongation at break rose by about 50%. This disproportionate response indicates that the quality of the fiber strongly governs the global mechanical behavior of nonwoven web–fiber contacts rather than the bulk mass [106]. In the present system, the polyphenol-rich extracts provide a high density of hydroxyl and aromatic groups capable of forming multiple hydrogen bonds and hydrophobic and π–π interactions with the BIOPLAST® matrix and within the coating itself [20,107]. Together with the FTIR-ATR and wettability results, this suggests the formation of a continuous, strongly interacting interphase at fiber cross-over regions, which limits local fiber slippage and delays damage initiation under load. Consequently, a relatively small amount of deposited material is sufficient to homogenize stress transfer paths in the fibrous network and yield a significant macroscopic reinforcement effect.

3.4. Evaluation of Active Substance Release from the Nonwoven System

To develop a biosystem enabling the release of active substances, UV-VIS spectrophotometric analysis was performed to assess the release dynamics. The system followed a diffusion-controlled model, in which the active compound was homogeneously distributed within the polymer matrix. Measurements were conducted at 282 nm for the nonwovens modified with Vaccinium myrtillus L. and at 268 nm for those modified with Sambucus nigra L., which were selected based on the UV–Vis spectra recorded over 190–750 nm. The calibration curves established at these wavelengths exhibited high coefficients of determination (R2 = 0.990 for V. myrtillus L. (Figure 8A) and R2 = 0.978 for S. nigra L. (Figure 7B).
The extract-treated nonwovens were immersed in distilled water under static conditions and incubated at 37 °C. The high water solubility of both extracts facilitated their release from the nonwoven matrix, an advantageous feature for health-oriented delivery systems. The release was monitored over 72 h, a time frame relevant to short-term therapeutic applications, such as palliative treatments. The release profiles followed a logarithmic function with strong correlation coefficients (R2 = 0.9343 for S. nigra L. and R2 = 0.9397 for V. myrtillus L.), revealing an initial burst release phase followed by a slower, diffusion-governed stage (Figure 8C).
This biphasic behavior is characteristic of matrix-type delivery systems. S. nigra L. demonstrated a higher terminal concentration (~7 µg/mL) and steeper slope (1.0261 vs. 0.6621), indicating a more rapid and pronounced release. The process was predominantly driven by diffusion into the aqueous medium. This effect may be related to the properties of the modified nonwoven. For S. nigra L., the wetting angle was significantly lower, resulting in better interaction of the material with the aqueous medium during the process and faster release. To determine the mechanism and characteristics of the release of active compounds from extract-treated nonwoven matrices, three classical kinetic models were applied—the Higuchi, Korsmeyer–Peppas, and first-order models—which are among the most commonly used approaches for describing drug release behavior. The parameters obtained for each kinetic model are presented in Table 6.
Based on the determination coefficient (R2) values, the goodness of fit of the applied kinetic models to the experimental data was evaluated (Table 6). The first-order model demonstrated the best fit for both extracts, achieving the highest R2 values and confirming a predominantly diffusion-controlled release mechanism.

4. Discussion

The results confirm that the use of natural plant extracts rich in polyphenols, such as Vaccinium myrtillus L. and Sambucus nigra L., is an effective strategy for the surface modification of spun-bonded nonwovens made from the biodegradable polymer BIOPLAST®. The obtained materials exhibited distinct changes in their physicochemical and mechanical properties compared with the unmodified reference nonwoven. The surface treatment significantly increased the hydrophilicity of the nonwovens, as evidenced by the decrease in the water contact angle. Such an enhancement in surface wettability is highly beneficial, as it promotes better interaction with aqueous environments and facilitates the diffusion-controlled release of active compounds. The spray coating technique proved to be a simple, efficient, and environmentally friendly method that does not require prior chemical or plasma activation of the substrate, aligning with the principles of green chemistry and sustainable materials engineering. Mechanical testing revealed notable improvements in the tensile strength (approximately 38%) and elongation at break (approximately 50%) following surface modification. This strengthening effect is consistent with the presence of a polyphenol-rich interphase at fiber crossover points, which increases inter-fiber adhesion, reduces local slippage under load, and promotes a more uniform stress distribution within the web. Improved mechanical behavior, combined with bioactive surface properties, makes these materials promising for multifunctional and bio-integrative textile applications.
GPC/SEC analysis clearly demonstrated a reduction in the weighted average molar mass (Mw) by approximately 20% after three years of simulated storage, confirming progressive chain scission and molecular degradation. Nevertheless, the DSC results revealed secondary crystallization and amorphous phase reorganization, leading to increased structural order and crystallinity within the polymer matrix. The thermally induced supramolecular reconstruction resulted in a denser, more ordered crystalline morphology and stronger physical interactions between polymer chains. This reorganization compensated for the chemical degradation, resulting in a paradoxical improvement in the mechanical properties. Similar effects have been reported for other biodegradable polymers, such as PLA and PCL, in which moderate heat exposure promoted secondary crystallization and increased the fibers’ rigidity despite chain scission. These findings highlight the importance of considering morphological transformations when interpreting ageing results for biodegradable polymers. The observed mechanical reinforcement during thermal exposure should thus be attributed to reorganization at the supramolecular level, rather than actual resistance to degradation.
In contrast, hydrolytic degradation experiments showed a progressive decrease in molar mass (by approximately 25% after 10 weeks) and a concurrent reduction in mechanical strength. This trend is typical of aliphatic biodegradable polymers.
The release profiles of polyphenolic compounds from the modified nonwovens exhibited a two-phase behavior: an initial burst release followed by a slower, diffusion-controlled stage. Kinetic modeling indicated that the first-order model provided the best fit (R2 ≈ 0.89), confirming that the release mechanism was predominantly governed by diffusion through the polymer matrix. Faster release was observed for the Sambucus nigra L. system, which correlated with its higher surface hydrophilicity and stronger interaction with the aqueous medium.

5. Conclusions

Spun-bonded technology is widely applied in the production of fibers from polymers such as PLA, PCL, and PBS, whose processing routes are well established and increasingly adopted in commercial applications. Despite this progress, there remains considerable potential for introducing novel biopolymers, including BIOPLAST®. The results of this study show that coating BIOPLAST® nonwovens with polyphenol-rich plant extracts can significantly enhance their physicochemical, mechanical, and bioactive properties. The modified nonwovens exhibited increased hydrophilicity and enhanced mechanical performance, consistent with the formation of a cohesive polyphenolic layer that strengthened fiber–fiber interactions. The spray coating method used in this work is simple, readily scalable, and compatible with environmentally friendly processing. At the same time, ageing and hydrolytic degradation tests indicated a predictable biodegradability profile consistent with short-term biomedical applications. Taken together, these findings indicate that combining a biodegradable polymer substrate with natural plant-derived bioactives offers a sustainable route to functional nonwoven materials for biomedical and cosmetic uses and provides a basis for further optimization toward specific MedTech-related products.

Author Contributions

Conceptualization, K.G.-J. and L.M.-K.; methodology, B.K., P.C., and S.K.; formal analysis, P.Ś. and S.K.; investigation, N.S., K.G.-J., P.Ś., and D.Z.; writing—original draft preparation, N.T. and A.B.; writing—review and editing, B.K., P.C., and K.G.-J.; visualization, N.T. and A.B.; supervision, L.M.-K. All authors have read and agreed to the published version of the manuscript.

Funding

The work was funded by the subvention for Łukasiewicz Research Network—Łódź Institute of Technology in 2025.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

The original contributions presented in this study are included in the article. Further inquiries can be directed to the corresponding author.

Acknowledgments

We extend our sincere thanks to Alicja Duda from the Łukasiewicz Research Network’s Institute of Non-Ferrous Metals for her assistance in preparing the plant extracts and Sylwia Jagodzińska from the Łukasiewicz Research Network’s Łódź Institute of Technology. This article was completed while the tenth author was the Doctoral Candidate in the Interdisciplinary Doctoral School at the Lodz University of Technology in Poland.

Conflicts of Interest

The authors declare no conflicts of interest.

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Eng 07 00049 g001
Figure 1. The process of manufacturing modified nonwovens with fruit extract. (A) Spun-bonded process. (B) Preparation of extracts. (C) Surface functionalization of nonwoven fabrics using aerographic spray coating. (D) Characterization methods.
Figure 1. The process of manufacturing modified nonwovens with fruit extract. (A) Spun-bonded process. (B) Preparation of extracts. (C) Surface functionalization of nonwoven fabrics using aerographic spray coating. (D) Characterization methods.
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Figure 2. The morphology and surface geometry of individual fibers. (A) SEM image mag. of ×200 and (B) SEM image mag. of ×10,000. (C) Histogram of the fibers diameter distribution. (D) Normal probability plot of diameter.
Figure 2. The morphology and surface geometry of individual fibers. (A) SEM image mag. of ×200 and (B) SEM image mag. of ×10,000. (C) Histogram of the fibers diameter distribution. (D) Normal probability plot of diameter.
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Figure 3. Structural and functional characteristics of nonwoven. (A) Breaking force along for nonwoven during the accelerated ageing. (B) Elongation along for nonwoven during the accelerated ageing. (C) Tensile strength along for nonwoven during the accelerated ageing. (D) Molar mass distribution. (E) DSC plots (first heating). (F) FTIR-ATR spectra.
Figure 3. Structural and functional characteristics of nonwoven. (A) Breaking force along for nonwoven during the accelerated ageing. (B) Elongation along for nonwoven during the accelerated ageing. (C) Tensile strength along for nonwoven during the accelerated ageing. (D) Molar mass distribution. (E) DSC plots (first heating). (F) FTIR-ATR spectra.
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Figure 4. Structural and functional characteristics of nonwoven after hydrolysis: (A) breaking force along, (B) elongation along, (C) tensile strength along, (D) molar mass distribution, and (E) FTIR-ATR spectra.
Figure 4. Structural and functional characteristics of nonwoven after hydrolysis: (A) breaking force along, (B) elongation along, (C) tensile strength along, (D) molar mass distribution, and (E) FTIR-ATR spectra.
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Figure 5. Structural and functional characteristics of nonwoven with extracts. (A) FTIR-ATR spectra of fruit extracts: V. myrtillus L. and S. nigra L. (B) Picture of spun-bonded nonwoven with V. myrtillus L. (C) Picture of spun-bonded nonwoven with S. nigra L.
Figure 5. Structural and functional characteristics of nonwoven with extracts. (A) FTIR-ATR spectra of fruit extracts: V. myrtillus L. and S. nigra L. (B) Picture of spun-bonded nonwoven with V. myrtillus L. (C) Picture of spun-bonded nonwoven with S. nigra L.
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Figure 6. Pictures of distilled water droplets deposited on the surface of materials (3 repetitions): (A) spun-bonded; (B) spun-bonded + V. myrtillus L.; and (C) spun-bonded + S. nigra L.
Figure 6. Pictures of distilled water droplets deposited on the surface of materials (3 repetitions): (A) spun-bonded; (B) spun-bonded + V. myrtillus L.; and (C) spun-bonded + S. nigra L.
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Figure 7. Mechanical properties of nonwovens with extracts: (A) breaking force along, (B) elongation along, and (C) tensile strength along.
Figure 7. Mechanical properties of nonwovens with extracts: (A) breaking force along, (B) elongation along, and (C) tensile strength along.
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Figure 8. Valuation of active substance release from the nonwoven system. (A) Calibration curves for extracts of V. myrtillus L. (B) Calibration curves for extracts of S. nigra L. (C) Release of plant extracts from the spun-bonded nonwoven.
Figure 8. Valuation of active substance release from the nonwoven system. (A) Calibration curves for extracts of V. myrtillus L. (B) Calibration curves for extracts of S. nigra L. (C) Release of plant extracts from the spun-bonded nonwoven.
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Table 1. Physical-mechanical parameters.
Table 1. Physical-mechanical parameters.
ParameterSpun-Bonded Nonwoven
Thickness (mm)0.27 ± 0.01
Surface density (g/m2)49.8 ± 0.9
Breaking force, along (N)3.04 ± 0.19
Elongation, along (%)28.4 ± 1.8
Tensile strength, along (MPa)0.23 ± 0.02
Table 2. GPC/SEC results after accelerated ageing.
Table 2. GPC/SEC results after accelerated ageing.
ParameterInitial2 Years3 Years
Mw (g/mol)105,40084,10082,500
RSD (%)1.31.02.2
Index D (Mw/Mn)2.52.62.4
RSD (%)1.50.52.0
Table 3. GPC/SEC results after hydrolysis.
Table 3. GPC/SEC results after hydrolysis.
ParameterInitial3 Weeks5 Weeks10 Weeks
Mw (g/mol)105,40092,70088,10079,500
RSD (%)1.33.12.72.9
Index D (Mw/Mn)2.554.584.934.70
RSD (%)1.52.82.83.1
Table 4. Parameters of fruit extract at 20 °C.
Table 4. Parameters of fruit extract at 20 °C.
ParameterV. myrtillus L.S. nigra L.
Density (g/cm3)0.9930.960
Surface tension (mN/m)30.4629.04
pH3.74.7
Table 5. FTIR-ATR characteristics for fruit extract bands.
Table 5. FTIR-ATR characteristics for fruit extract bands.
Band (cm−1)Chemical Group
3307–3280-OH symmetric stretching 
2930-CH asymmetric stretching
2885-CH symmetric stretching
1717C=O in the aglycone-pyranoside combination
1612C=C scissoring on pyran and phenolic group
1519C-H scissoring
1406C=C stretching in the aromatic ring
1300–1223-CO-/C–O–C symmetric stretching
1150-CH2
1028Glycosidic bonding and -CO group in polysaccharides 
900–675Out-of-plane bending vibration of hydrogen atoms in ring
600–400Deformation vibration of the phenol ring
Table 6. Kinetic models of release.
Table 6. Kinetic models of release.
ModelModel EquationR2
V. myrtillus L.S. nigra L.
Higuchi Q = KHt1/20.73630.7607
First orderdC/dt = −Kt0.88940.8843
Korsmeyer–PeppasMt/Mα = Ktn0.86640.7982
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Gzyra-Jagieła, K.; Kopyciński, B.; Czarnecki, P.; Kęska, S.; Słabęcka, N.; Bednarowicz, A.; Tarzyńska, N.; Zielińska, D.; Madej-Kiełbik, L.; Śniarowski, P. Green Surface Engineering of Spun-Bonded Nonwovens Using Polyphenol-Rich Berry Extracts for Bioactive and Functional Applications. Eng 2026, 7, 49. https://doi.org/10.3390/eng7010049

AMA Style

Gzyra-Jagieła K, Kopyciński B, Czarnecki P, Kęska S, Słabęcka N, Bednarowicz A, Tarzyńska N, Zielińska D, Madej-Kiełbik L, Śniarowski P. Green Surface Engineering of Spun-Bonded Nonwovens Using Polyphenol-Rich Berry Extracts for Bioactive and Functional Applications. Eng. 2026; 7(1):49. https://doi.org/10.3390/eng7010049

Chicago/Turabian Style

Gzyra-Jagieła, Karolina, Bartosz Kopyciński, Piotr Czarnecki, Sławomir Kęska, Natalia Słabęcka, Anna Bednarowicz, Nina Tarzyńska, Dorota Zielińska, Longina Madej-Kiełbik, and Patryk Śniarowski. 2026. "Green Surface Engineering of Spun-Bonded Nonwovens Using Polyphenol-Rich Berry Extracts for Bioactive and Functional Applications" Eng 7, no. 1: 49. https://doi.org/10.3390/eng7010049

APA Style

Gzyra-Jagieła, K., Kopyciński, B., Czarnecki, P., Kęska, S., Słabęcka, N., Bednarowicz, A., Tarzyńska, N., Zielińska, D., Madej-Kiełbik, L., & Śniarowski, P. (2026). Green Surface Engineering of Spun-Bonded Nonwovens Using Polyphenol-Rich Berry Extracts for Bioactive and Functional Applications. Eng, 7(1), 49. https://doi.org/10.3390/eng7010049

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