Abstract
Keywords
Introduction
With the rapid increase of the population, the demand for dressings, facial mask substrate, packaging and related products made from petroleum-based materials has increased dramatically. However, petroleum product waste is increasingly accumulating in the environment due to its long life (non-biodegradable), low recycling rates and inadequate waste management.1,2 It has been reported that microplastics in the ocean can move through the food chain and accumulate, which has gradually become a significant hazard to the environment and human health.3–5 Therefore, a replacement with biodegradable, biocompatible, affordable, and environmentally friendly materials is urgently needed. Cellulose-based materials have been widely considered as alternatives to petroleum-based products. Due to the green degradability and biocompatibility of natural fibers, it has been the subject of much research.
Kapok fiber, derived from the fruit of the kapok tree, is a renewable agricultural by-product. As a typical cellulose plant fiber, it is mainly composed of cellulose, hemicellulose, lignin, and a small amount of waxy coating.6,7 Kapok fiber is well known for its light weight (bulk density: 0.30 g/cm3) and its unique large lumen structure gives it the highest hollow rate (>84%) among natural fibers.8–10 These physicochemical properties contribute to its excellent moisture absorption (moisture regain rate: 10.75%) and warmth retention (thermal conductivity: 0.045 W·m−1k−1).11,12 Additionally, kapok fiber exhibits interesting anti-bacterial, anti-mite, biodegradability, and biocompatibility properties. Although challenges such as short length, brittleness, and low cohesive force limit its direct application in spinning, kapok fibers can be blended and spun with other fibers. 13 Meanwhile, kapok fiber as a filler wadding can be well applied to thermal insulation, sound absorption and buoyancy life-saving materials.14,15 Due to the hydrophobic properties of waxes, many scholars have focused their research on kapok fibers for oil-water separation, dye adsorption and wastewater treatment.16–19
Silk fiber is a natural protein fiber that was discovered by chance in China more than 5,000 years ago. It consists mainly of sericin and fibroin, followed by waxy matter, carbohydrates, and inorganic matter. 20 Due to the unique elegant beauty, softness, and wearing comfort of silk products, silk fiber has long been used in the production of high-grade textiles. Moreover, silk is widely used in medicine, cosmetics, biological tissue engineering, and smart wearable materials because of its excellent biocompatibility, biodegradability, mechanical strength, and non-toxicity. However, some silk cannot meet the processing needs and become industrial waste, including damaged cocoons, reeling waste, and waste silk fibers from the spinning process. Since waste silk has similar properties to normal silk, its recycling and utilization is considered to be highly valuable. 21 It is often remade into yarn or fabric in the textile industry, and the modified waste silk can be used to prepare functional textiles.22–24 Waste silk with exactly the same chemical composition is also expected to replace silk as a raw material for the extraction of regenerated silk fibroin protein.25,26 Due to the cost of processing, environmental pollution, and safety considerations, there is still a large waste of waste silk resources. As a result, turning waste silk into goods with a high value-added will reduce the waste of biological resources to a large extent.
In recent years, kapok fiber has garnered more attention from scholars in the textile field. Because of its inherent length and chemical composition limitation, kapok fiber is typically blended with other fibers and processed into nonwoven fabrics using needling techniques. The samples prepared by this method tend to be hydrophobic samples with a certain weight (>80
Materials and methods
Materials
The experiment's kapok fiber came from Pate County in Java Tengah, Indonesia. Its diameter and length were 18.15 ± 4.82 µm and 25.00 ± 2.1 mm (Table S1), respectively. The waste silk was the off-cut from the silk spinning process and provided by a textile factory in China. It belonged to domestic silk with a diameter of 7.09 ± 2.19 µm and a length greater than 10 mm. Sodium hydroxide (NaOH) (purity ≥96.0%) was provided by Sinopharm Chemical Reagent Co., Ltd. Deionized water and vegetable oil were purchased in the local market.
Preparation of kapok/waste silk nonwovens (KSN)
Basic parameters of KSN.
Characterizations
The morphology of samples was observed under a DXS-10ACKT scanning electron microscope (SEM mode: 10.0 kV, WD: 5.0 mm, magnification: 50/100/1000/3000). The chemical compositions were tested by Fourier transform infrared spectrometer (Spectrum Two, America) in the range of 4000∼400 cm−1. Porosity refers to the percentage of pore volume to the total volume of nonwovens. Each sample was measured 5 times. The calculation formula is:
Physical and mechanical test
The air permeability of samples was tested by an automatic air permeability tester (YG461E, China), according to the standard method of GB/T 5453-1997. The bending stiffness and bending hysteresis moment were measured based on GB/T18318.5-2009. The samples were cut into the shape of 100 mm × 50 mm and tested on a Pure Bending Tester (KES-FB-2, Japan). Tensile test was carried out on a multifunctional electronic fabric strength machine (YG026MB-250, China), according to GB/T 3923.1-2013. The samples were cut to the shape with a dimension of 70 mm × 50 mm, and tensile test was conducted at the drawing speed of 100 mm/min with a clamping distance of 40 mm. Each sample was measured 5 times in the air permeability test and 3 times in the bending and tensile tests. All the above tests were conducted in an environment with temperature and humidity of 25 ± 2°C and 60 ± 5%, respectively.
Wettability test
Properties of liquids for experiment.
Soil burial test
ASTM-D5988-12 standard method was adopted in the soil burial test. First, the soils used in the experiment were collected in different environments (woods, bushes, and lakeside), with a sample depth over 200 mm. To control soil particle size below 2 mm, the mixed soil was screened by an experimental standard sieve (10 mesh) to remove stones, plant roots, and other non-soil material. Then, samples were cut into a shape with dimensions of 50 mm × 50 mm, buried in beakers with mixed soil (1 kg) at 30∼50 mm, and placed in a constant temperature and humidity environment (25 ± 2°C and 60 ± 5%). 75 mL of deionized water was added every 5 days. The samples were removed from the soil every 15 days, washed with deionized water to clean the soil adhering to the surface, and dried at 80°C for 6 h. Each sample was measured 3 times. The calculation formula is:
Statistical analysis
Statistical analysis was conducted on the KSN performance data using one-way analysis of variance (ANOVA). The independent variable was the mixing ratio, and a significance level of
Results and discussion
Characterization
The morphology of KSN was illustrated in Figure 1. SEM images in the surface direction (Figure 1(a)–(e)) revealed that numerous fibers compressed into a flat surface and intertwined together to form nonwoven. It can be seen that the KSN-1 had more pores (Figure 1(a)), and the number of pores decreased as the proportion of kapok fiber increased (Figure 1(b)–(e)). The reasonable explanation was that the fiber diameter of the kapok was larger than waste silk, and a single kapok fiber can cover a larger area (Figure 1(c)). In addition, the fibrillation of waste silk was more obvious compared with kapok fiber. SEM images of the cross-sectional direction were shown in Figure 1(f)–(j). It was shown that the thickness of KSN-1 was 0.287 mm, and the thickness of the samples decreased as the proportion of kapok fiber increased (0.242 mm, 0.214 mm, 0.157 mm, and 0.094 mm for KSN-2, KSN-3, KSN-4, and KSN-5, respectively). The fiber cross-section of waste silk in KSN was almost round (Figure 1(k)), while the kapok was flattened (Figure 1(l)). As a result, the nonwoven's thickness has decreased because the flattened kapok fibers have taken on the role of the nonwoven's support structure by securely tying the neighboring fibers together. To our knowledge, the previously reported nonwoven fabrics of the same type containing kapok fiber or silk generally have a certain mass (>80 SEM images of KSN at 100 and 1000× magnifications. (a), (b), (c), (d), (e) Surface direction of KSN, (f), (g), (h), (i), (j), (k), (l) Cross-sectional direction of KSN.
The air permeability of KSN was shown in Figure 2(a). Among the samples, KSN-1 exhibited maximum permeability of 113.62 mm/s. With the increase in the proportion of kapok fiber, the permeability of KSN-2, KSN-3, KSN-4, and KSN-5 decreased to 101.40 mm/s, 37.86 mm/s, 18.32 mm/s, and 8.42 mm/s, respectively. The ANOVA test results showed that there was a significant difference ( Characterization of air permeability and softness (a) Air permeability and porosity, (b) Bending stiffness and bending hysteresis moment.
The softness of KSN was characterized by testing its bending stiffness and bending hysteresis moment. The bending stiffness reveals the nonwoven's capacity to withstand bending deformation, which is related to the thickness and porosity of the nonwovens.43,44 And the bending hysteresis moment reflects the amount of material viscosity. As shown in Figure 2(b), the bending stiffness increased from 0.078 to 0.387 gf·cm2/cm as the proportion of kapok fiber increased (
Mechanical property
According to the stress-strain curves shown in Figure 3(a), the samples were typically linearly deformed before tensile failure. With the proportion of kapok fibers increased, the fracture stress increased from 0.58 MPa to 10.85 MPa ( Fracture mechanism of KSN (a) Stress-strain curves, (b) Fracture stress and fracture strain, (c) SEM images of fracture morphology (magnification: 50 & 3000), (d) schematic diagram of fiber entanglement, (e) FTIR spectrum of fibers before and after alkali modification.
Effective entanglement between fibers can increase the slippage resistance during stretching, which enhanced the strength of the nonwovens.45,50 As shown in Figure 3(d), three types of entanglement can be formed between waste silk and kapok fibers, including silk & silk (S-S), silk & kapok (S-K), and kapok & kapok (K-K). And the contact area of the three entanglements (S-S, S-K, and K-K) increased sequentially. Among them, S-S entanglement not only contained entanglement of waste silk, but also some fibril entanglements, which may provide weak strength. In addition, the rough surface after alkali treatment could increase the contact friction between fibers, which is beneficial to the stability of KSN structure and improve the failure strength. 51
Infrared transmittance peak of untreated kapok fiber and waste silk (cm−1).
In addition to the entanglement between fibers, the breaking strength of nonwovens is also determined by the bonding between the fibers.56–58 Previous studies have demonstrated that alkaline substances can effectively remove surface waxes from plant fibers, thereby exposing cellulose with abundant hydroxyl groups. 59 Under the Campbell effect during hot pressing, cellulose fibers can come close to each other and form hydrogen bonds, thus enhancing the bonding between the fibers. This phenomenon has also been extensively documented in the literature.60,61 In this study, the incorporation of a higher proportion of kapok fiber introduced a greater number of hydroxyl groups, thereby facilitating the formation of hydrogen bonding networks. There was no doubt that this does contribute to the improvement of the fracture strength of nonwovens. Both the flattened shape of kapok and the hot-pressing process contributed equally to favorable interlocking and bonding between the fibers. Additionally, FTIR analysis confirmed the presence of residual lignin in the alkali-treated kapok fibers, which may serve as a natural binder and contribute to the overall strength enhancement of KSN. 62
Wettability
To characterize the wettability of KSN, the static contact angle and dynamic spreading process were measured. As shown in Figure 4(a)–(b) and Table 4, the water contact angle (WCA) and oil contact angle (OCA) of KSN were below 40° and 50°, respectively, and fluctuated within 10°. The difference between the left and right contact angle was less than 8° (Table S3-S4). This indicated that KSN has hydrophilic and lipophilic properties. The ANOVA test results showed significant differences between the water contact angle values ( Characterization of KSN wettability (a) Water contact angle, (b) Oil contact angle, (c) Liquid spreading time, (d) Dynamic water contact angle, (e) Dynamic oil contact angle, (f) Photos of liquid spreading on KSN. Contact angle data of KSN.
As shown in Figure 4(c), the water spreading time of the samples decreased and then increased with the increase of the proportion of kapok fiber, and the water spreading times of KSN-1, KSN-2, KSN-3, KSN-4, and KSN-5 were 69.82 s, 18.00 s, 12.73 s, 7.09 s, and 9.73 s, respectively (
Biodegradability
The biodegradability of KSN was tested by a 30-day soil burial experiment. As shown in Figure 5(a), the degradation rates of KSN-1, KSN-2, and KSN-5 after 15 days of soil burial were 1.44%, 7.77%, and 13.08%, respectively. Figure 5(b) showed that some mycelium appeared on the surface of the samples at this time, and a few tears were observed on KSN-5. When buried for 30 days, the degradation rates of KSN-1, KSN-2, and KSN-5 reached 4.31%, 12.68%, and 49.41%, respectively (Figure 5(a)). Among them, the KSN-1 and KSN-2 remained intact and a large number of mycelia were found on their surfaces, while the KSN-5 was broken down into small pieces by microbes (Figure 5(b)). This result suggested that the biodegradability of KSN improved as the proportion of kapok fiber increased. It can be attributed to the difference in the degradation mechanism of the two fibers. Related studies had shown that cellulose fibers tend to exhibit a faster degradation rate than protein fibers.65–69 Characterization of the degradability of KSN (a) Degradation rate of KSN, (b) Photos of KSN after being buried in the soil for 0,15,30 days, respectively, (c) Schematic diagram of KSN degradation.
We next explained the degradation process of KSN based on the available literature. There were a lot of bacteria, fungi, and other microorganisms in the soil, some of which can secrete cellulase or protein enzymes, such as aspergillus, penicillium, and bacillus. 70 In this study, because waxes were resistant to biodegradation, 66 the removal of waxes from fibers by alkali treatment not only transformed the fiber surface from hydrophobic to hydrophilic but also accelerated fiber disintegration. The degradation mechanism of KSN was shown in Figure 5(c). The cellulose in kapok fiber can be degraded by the synergistic action of cellulases (endoglucanases, exoglucanases, and β- glucosidases). 71 The glycosidic bonds in the amorphous region of cellulose can be hydrolyzed by endoglucanases, resulting in long-chain oligomers. The long-chain oligomers were then hydrolyzed by exoglucanases to produce cellobiose, which was further hydrolyzed by β- glucosidases to glucose. Similarly, the crystalline region of cellulose can be eventually hydrolyzed to glucose by the synergistic action of cellulases. 72 Contrarily, the biodegradation of waste silk was based on the microbial attack on their protein structure, and the presence of water in the soil contributed to the loosening of silk protein chains.20,73 The attack of microorganisms occurred first in the loose amorphous region and then extended to the crystalline region, and the final degradation products were small peptides and amino acids.74,75
Conclusion
In this study, a degradable bio-based nonwoven was prepared from kapok fiber and waste silk, and it was systematically characterized and studied. The results showed that KSN is lightweight, thin, and oil-water amphiphilic. The unit grammage of KSN was 34 g/m2, and the thickness was less than 0.3 mm. As the proportion of kapok fiber increased, the structure of KSN became denser and the bending stiffness increased. The air permeability decreased from 113.62 mm/s to 8.42 mm/s, and the bending stiffness increased from 0.078 gf·cm2/cm to 0.387 gf·cm2/cm. Meanwhile, the fracture strength increased from 0.58 MPa to 10.85 MPa, resulting in significant improvements in mechanical properties. KSN also exhibited oil-water amphiphilicity, with oil/water contact angles all less than 50°. The maximum 30-day degradation rate reached 49.41%. The higher silk content can add high value to the product, making KSN-1 and KSN-2 excellent candidates as potential substitutes for dressing and facial mask substrate. Furthermore, KSN-3, KSN-4, and KSN-5, which exhibited good mechanical properties, hold promise for packaging applications. Meanwhile, the application of biodegradable natural fibers can effectively mitigate the “white pollution problem”, and the recycling of waste silk would avoid the waste of resources.
Ethical statement
Ethical approval
This article does not contain any studies with human participants or animals performed by any of the authors.
Supplemental Material
Supplemental Material - Development and characterization of kapok/waste silk nonwoven as a multifunctional bio-based material for textile applications
Supplemental Material for Development and characterization of kapok/waste silk nonwoven as a multifunctional bio-based material for textile applications by Hongchang Wang, Liyao Cao, Hang Yuan, Yuling Li, Run Wen and guangbiao Xu in Journal of Industrial Textiles.
Footnotes
Declaration of conflicting interests
Funding
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References
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