Article_FabricationOfGreenCompositeFib (2)

Journal of Material Cycles and Waste Management https://doi.org/10.1007/s10163-021-01269-6 ORIGINAL ARTICLE Fabrication of green composite fibers from ground tea leaves and poly(lactic acid) as eco‑friendly textiles with antibacterial property Kankavee Sukthavorn1 · Benjarut Ketruam1 · Nollapan Nootsuwan1 · Suchada Jongrungruangchok2 · Chatchai Veranitisagul3 · Apirat Laobuthee1  Received: 4 January 2021 / Accepted: 28 June 2021 © Springer Japan KK, part of Springer Nature 2021 Abstract This work aims to prepare bio-based polymer composite fiber using poly(lactic acid) (PLA) and ground tea leaves (GTL) as a matrix and bio-based filler, respectively, via the melt-spinning process. The masterbatch obtained from PLA and GTL, with a mass ratio of 90:10, was varied as 0–20 phr, for mixing with PLA to prepare the green composite fibers. The fibers were then characterized using a SEM, UTM and DSC technique. The composite fibers showed a slightly rough surface in their cross-section. Tensile strength and elongation at break of the composite fibers were found to be the highest for the fiber prepared by adding 5 phr masterbatch. This is consistent with the good dispersion of GTL particles in the PLA matrix. The thermal properties of the composite fibers did not significantly change with an increasing amount of GTL. The dye removal properties of the composite fibers showed that the removal efficiency of methylene blue dye was more than reactive blue-19 dye after 24 h under room temperature conditions. By the knitting fabric manufacturing process, the obtained green composite fibers with the best mechanical properties were used as an eco-friendly textile to make fabrics with the antimicrobial property. Keywords  Green composite fiber · Ground tea leaves (GTL) · Poly(lactic acid) (PLA) · Eco-friendly textiles · Antimicrobial property Introduction fibrous form via electrospinning [2, 3] or melt-spinning [4, 5]. In recent years, poly(lactic acid) (PLA) has been confirmed as one of the most environmentally friendly polymers due Nowadays, PLA has been studied and employed in sev- to its renewability, biodegradability, biocompatibility, and eral applications, such as packaging, biomedical, electronic, good thermomechanical properties [1]. PLA can, therefore, transportation, and agriculture, etc. Because of its biode- be processed using many techniques, such as compression, gradable and biocompatibility properties, PLA became the injection, and extrusion molding, and can be made into a most promising material for commercially replacing non- degradable materials. The biodegradable property of PLA * Apirat Laobuthee can be shown via the simple hydrolysis of ester bonds in [email protected] suitable conditions consisting of a combination of mois- Chatchai Veranitisagul ture, oxygen, and naturally occurring microorganisms [6]. [email protected] Although PLA shows various advantages, its drawback is in its mechanical properties of high brittleness and low impact 1 Department of Materials Engineering, Faculty strength. Therefore, to improve the durability property of of Engineering, Kasetsart University, Ladyao, PLA, it has been blended with other bio-based polymers or Chatuchak 10900, Bangkok, Thailand plasticizers, such as polybutylene succinate (PBS) [7, 8], poly(ε-caprolactone) (PCL) [9, 10], poly(3-hydroxybutyrate) 2 College of Pharmaceutical Chemistry, Faculty of Pharmacy, (PHB) [11, 12], poly(3-hydroxybutyrate-co-3-hydroxyvaler- Rangsit University, Pathumthani 12000, Thailand ate) (PHBV) [13, 14], poly(butylene adipate-co-terephtha- late) (PBAT) [15], and poly(ethylene glycol) (PEG). [16, 3 Department of Materials and Metallurgical Engineering, 17]. Faculty of Engineering, Rajamangala University of Technology, Thanyaburi, Pathumthani 12110, Thailand 1 3Vol.:(0123456789)

Journal of Material Cycles and Waste Management In the case of the green composite materials, several antimicrobial properties was also investigated. Moreover, the natural fibers, such as bamboo fiber [18], banana fiber [19], obtained green composite fibers have been further used to chestnut shell [20], spent coffee grounds [21], and spent tea prepare the prototype fabrics via the knitting process. leaves [21, 22], etc. were used as fillers, or reinforcements, for PLA composites. Tea was one of the most widely con- Experimental sumed beverages in the world until it became a commercial product in the form of instant tea, where a large amount Materials of spent tea leaf waste remained. In many previous works, the spent tea leaves waste was used to study and apply in Poly(lactic acid) (PLA, grade 3052D) was purchased from several applications, such as adsorbent dye and toxic metal Nature Works LLC, USA, while poly(ethylene glycol) (PEG, [23, 24], composite materials for construction [25, 26], etc. analytical grade) was purchased from Ajax Finechem Pty. Consequently, the resourceful utilization of this waste has Ltd., Australia. Waste tea leaves were collected from a bever- been important in reducing the environmental impact and age shop in Bangkok, Thailand. value-addition of this waste [22, 26]. Preparation and characterization of the ground tea Uddin et al. (2012) modified the black tea leaf extract leaves (GTL) with Ag nanoparticle to use for poly(vinyl alcohol) (PVA) composite film to enhance its dielectric properties [27]. Mat- The ground tea leaves (GTL) were prepared, as follows: tos et al. applied waste tea leaves and wood particles as natu- Waste tea leaves were washed in water and dried at 100 °C ral fillers for polypropylene composites. The results show for 24 h to eliminate moisture. The cleaned tea leaves were that the mixture of both fillers is a good alternative renew- then ground and sieved to obtain the GTL with a particle able material in the production of the polymeric composite size < 45 μm. After that, GTL was stored in a sealed plastic [28]. Duan et al. presented the use of spent tea leaf powder bag. as a filler to develop cellulose green composite films [29]. The surface morphology of GTL was studied by scanning Although there was little literature focusing on the anti- electron microscopy (Philips, XL30) with an acceleration microbial properties of PLA materials for packaging, the voltage of 10 kV. relationship between antimicrobial agents and PLA degrada- tion was not clear and less studied. Furthermore, the report The chemical composition of the GTL was characterized of Tawakkal et al. reports that the PLA was a suitable car- by X-ray fluorescence spectroscopy (Horiba XGT-2000 W) rier of antimicrobial agents and did not show the impact on with the X-ray tube operated at 50 kV and 1 mA. the biodegradation process [30]. This has corresponded to Erdohan et al. who found that the antimicrobial poly(lactic Fourier-Transform Infrared (FTIR) spectrum was acid)-based films using the olive leaf extract (OLE) as an obtained from the GTL sample, prepared by the KBr pellet antimicrobial agent, did not show any effect to decrease or technique, and recorded in the range 4000–500 ­cm−1 using inhibit the degradability rate of composite materials [31]. a Perkin-Elmer 2000-FTIR to identify the functional groups This might be due to the mechanism of the PLA biodegra- of the GTL. dation. PLA chains were split apart by heat and moisture in the compost, resulting in small molecular weight and even- The phase and structure of the GTL were carried out by tually lactic acid. After that, lactic acid was degraded by an X-ray diffractometer (X’PertPRO MPD diffractometer) microorganisms in the compost [32]. It can be seen that the operating at 40 kV and 30 mA. The scanning rate was 0.02°/ lactic acid and small molecular weight PLA were degraded min in the 2theta diffraction angle from 10 to 90°. by microorganisms, not including the PLA chain. Moreover, the present study demonstrated that adding antimicrobial Preparation of the green composite fibers agents into the PLA products, leading to an extended food and fabrics shelf life [33]. Poly(lactic acid) (PLA) pellets and the ground tea leaves However, no one reported the use of the ground tea leaves (GTL) were dried in an oven at 60 °C for 24 h before pro- (GTL) waste from consumption to make green composite cessing to prevent any potential hydrolytic degradation of fibers with biodegradable polymers, such as PLA, PBS, etc. the PLA and to reduce moisture during the melt process- In this present work, ground tea leaves (GTL) waste from ing. The masterbatch pellets of PLA/GTL, with 10 wt% of consumption was, therefore, used as a filler for poly(lactic GTL, were prepared by melt blending technique using a acid) (PLA) matrix to make the green composite fibers. To twin-screw extruder at 150–180 °C. The masterbatch, PEG, overcome the drawback of PLA, the PEG was selected and and PLA pellets were then mixed and spun to obtain the used as a plasticizer to improve the brittleness property of green composite fibers with a 24-hole spinneret and diameter PLA. The effect of GTL loading on mechanical, thermal, and size of 0.32 mm, spinning temperature 190–220 °C, screw 13

Journal of Material Cycles and Waste Management speed 8 rpm, and spinning speed 500 m/min. The weight into 25 mL of the dye solution. Then, the green composite ratio of PLA and PEG was kept constant at 90/10 while the fiber and dye solutions were stirred at room temperature masterbatch contents were varied at 5, 10, 15, and 20 phr, for 24 and 48 h. The dye solution was then collected and respectively. The nomenclature of the green composite fib- investigated using UV–visible absorption spectroscopy at ers is given in Table 1. The green composite fibers were also a wavelength of maximum absorbance 663 and 592 nm of used to make the green composite fabrics using a circular MB and RB dye, respectively. The dye removal percentage knitting machine. was calculated, as follows: [34] Characterization of the green composite fibers Dye removal percentage (%) = 1 − Ct∕C0 × 100 and fabrics where The melt flow index (MFI) of the composite compounds was Ct: The initial concentration of dye, and analyzed by an MFI tester (CEAST; TELEX 220,147) with C0: The concentration of dye after time t a temperature of 190 °C and a weight of 2.16 kg. Then, the The antimicrobial property of the green composite fabrics extruded composite material was weighed and calculated to was measured according to the ASTM E2149-01 standard report as an MFI value (g/10 min). testing method. The bacteria used in this study were Gram- positive bacteria, like Staphylococcus aureus (S. aureus) and The phase identification and structure of the fibers were Bacillus subtilis (B. subtilis), including fungus as Candida investigated by an X-ray diffraction spectrometer (XRD) albicans (C. albicans). The efficiency of the antimicrobial operating at 40 kV and 30 mA. The scanning rate was 0.02°/ property was calculated from the percent reduction of bac- min in the 2theta diffraction angle from 10 to 90°. teria, as follows: A tensile test was performed to analyze the tenacity and R = (B − A) × 100∕B elongation at break of the green composite fibers using Instron 5944. According to the ASTM D3822 standard test- where ing method, a 25 mm gauge length, 30 mm/min elongation R: A percentage reduction of bacteria, rate, and 10 N of a load cell were used. A: The number of bacteria recovered after dynamic con- tact of the sample at time 24 h, and The cross-sectional surface morphology of the fibers was B: The number of bacteria before the addition of the sam- characterized using a scanning electron microscope (SEM) ple at time 0 h operating at an accelerating voltage of 5 kV. The surface of the fibers was coated with a thin layer of gold to avoid image Results and discussion distortion due to charging. Characterization of the ground tea leaves (GTL) Differential scanning calorimeter (DSC) was used to analyze the glass transition temperature ­(Tg), crystalliza- The physical appearance and SEM image of GTL are shown tion temperature (­Tc), and melting temperature (­Tm) of the in Fig. 1a and b, respectively. The GTL particles are small green composite fibers with a Mettler Toledo DSC1 over a in size and dark green in color. temperature ranging of 0–200 °C, and with a heating rate of 10 °C/min under a nitrogen atmosphere. The SEM image showed that GTL, with irregular shape and rough surface, has particle sizes < 30  µm [35]. The The dye adsorption property of green composite fiber was results from XRF measurement (Table 2), revealed that GTL studied using cationic dye (methylene blue, MB) and anionic particles consist of five main elements, namely potassium, dye (reactive blue 19, RB). The solution of MB and RB dyes calcium, manganese, iron, and zinc, but especially calcium, was prepared from 1 mg of each dye in 1000 mL deion- with a content of up to 54.71 wt% [36]. ized water. 0.3 g of green composite fiber was dispersed FTIR spectrum of the GTL particles (see Fig. 1c) showed Table 1  Compositions of PLA, PEG and masterbatch of GTL in the that the peak at 3364 c­ m−1 was assigned to O–H stretch- green composite fibers ing, while the peaks at 2923 and 2855 c­ m−1 were assigned to C–H stretching of alkane. The peak at 1637 c­ m−1 was Code PLA as a PEG as a Plas- Masterbatch assigned to C = O stretching of the carbonyl group, and the Matrix (wt%) ticizer (wt%) of GTL (phr) peaks at 1452 c­ m−1 were assigned to C = C stretching of the aromatic group. Moreover, the peak at 1238 c­ m−1 was PLA/PEG 90 10 0 assigned to C-O stretching vibration of acetyl or aryl groups PLA/PEG + GTL-5 90 10 5 in the lignin [37–39]. PLA/PEG + GTL-10 90 10 10 PLA/PEG + GTL-15 90 10 15 PLA/PEG + GTL-20 90 10 20 13

Journal of Material Cycles and Waste Management the GTL color, and shiny, resulting from the alignment of the fibers in the machine’s direction from the spinning and draw- ing processes. The obtained fibers were further processed via the circular knitting process to obtain a light green-colored fabric (see Fig. 2b). In our related work, these obtained fib- ers were blended with natural fibers, e.g. cotton or rayon, for making green-colored fabrics in the form of scarves and purses, via a weaving machine (see Fig. 2c). MFI measurement The molten composite compounds were analyzed to study the effect of GTL filler on the melting flow rate of the PLA matrix. MFI value indicated the relationship between the melt viscosity and the molecular weight during melt pro- cessing [41, 42]. Figure 3a showed the MFI values of the composites compound. It was found that the GTL filler leads to a slight increase in the melt flow index of the PLA matrix. This might be due to the chain scission mechanism dur- ing melt processing or dispersion of GTL filler, resulting in lower viscosity or melt strength and lower molecular weight which corresponding to the research of Aouat et al. [41] found that the MFI values of PLA fibers increased by adding the cellulosic filler. XRD measurement Fig. 1  a Physical appearance b SEM image c FTIR spectrum and d XRD patterns of the PLA/PEG fiber and the green compos- XRD pattern of the ground tea leaves (GTL) ite fibers are shown in Fig. 3b. The PLA/PEG fiber showed a broad peak at around 16.01°, consistent with previous Table 2  Element compositions of the ground tea leaves (GTL) evidence presented by Chieng et al. [43]. For the green composite fibers, it was found that the two broad peaks at Element Percentage of around 16.01° and 21.79° corresponded to the highest peak weight (wt%) of PLA/PEG and GTL, respectively. As the GTL content increased, the intensity of diffraction peaks also increased. Potassium (K) 4.38 These results confirmed that the crystallization in PLA/PEG Calcium (Ca) 54.71 increased with an increase in the GTL content. Moreover, it Manganese (Mn) 17.48 was observed that the diffraction peak at 29.03° is consistent Iron (Fe) 22.76 with the previous research by Atiqah et al. [44]. Zinc (Zn) 0.69 Tensile measurement The XRD pattern of the GTL is shown in Fig. 1d. The broad Tensile measurements were carried out to evaluate the tenac- peak observed in the diffraction pattern of the GLT at around ity and elongation at break of all green composite fibers 21.79° agrees with the previous evidence presented by Qiao obtained from various masterbatch ratios. The stress–strain et al. [38] and showed it was the amorphous region [39, 40]. curve of all green composite fibers was shown in Fig. 4a. The results (Fig. 4b) show that the tenacity of the PLA/ Characterization of the green composite fibers PEG + GTL-5 composite fiber was higher than that of the and fabrics PLA/PEG fiber. Because the GTL has short fibers, they may act as a reinforcement in the polymer matrix [29]. How- The physical appearance of the green composite fibers ever, the increment of masterbatch above 5 phr decreased (Fig. 2a) was found to be light green in color resulting from the tenacity due to the inevitable aggregation of the filler at 13

Journal of Material Cycles and Waste Management Fig. 2  Physical appearances of the PLA/PEG + GTL-5 a fiber, b fabric, and c scarves Fig. 3  a MFI values and b XRD patterns of the PLA/PEG fiber, and the green composite fibers high content, and the reduction of efficiency to load a high Fig. 4  a Stress–strain curve b Tenacity and c Elongation at break of content of filler to the matrix [43]. the PLA/PEG fiber and the green composite fibers Figure 4c shows that the elongation at break of PLA/ PEG + GTL-5 composite fibers was higher than that of the PLA/PEG fibers. Moreover, the greater the increase of the masterbatch content, the greater the decrease of the elonga- tion at break obtained. Because GTL is quite rigid and irreg- ular in shape, it might inhibit the movement of the polymer chains [43]. The elongation at break of all composite fibers 13

Journal of Material Cycles and Waste Management was, therefore, higher than that of the PLA/PEG fibers, and Glass transition temperature (Tg) of the PLA/PEG fiber GTL might act as a plasticizer, consistent with previous evi- was found to be 61.54 °C, while the increment of the mas- dence presented by Cahcko et al. (2010) [45] and Duan et al. terbatch contents showed the decrement of glass transition [29]. Similarly, the increment of the mechanical properties temperature tendency of green composite fibers, from 55.29 agreed with the results from the previous study by Zucca- to 52.81 °C. This might be due to the GTL inserted in the rello et al. who reported that the addition of only 2 wt% bio- molecular chains of PLA, increasing the free space and free char in epoxy resin leading to the significant improvement of volume between molecules of PLA. The polymer chains can mechanical properties [46]. Moreover, Das et al. found that move easier leading to a lower glass transition temperature adding the biochar over 15 wt% in polypropylene matrix led [49, 50]. to less plastic deformation and more resistant deformation. This caused a decrease in the percentage elongation due to The crystallization temperature (Tc) of the PLA/PEG fiber the reduction of ductility [47]. was 92.50 °C. The greater the increase of masterbatch con- tents, the lower the tendency of crystallization temperature Morphology Figure 5 shows SEM images of the cross-sectional surfaces of the PLA/PEG fiber and the green composite fibers filled with various masterbatch content. The PLA/PEG fiber has a smooth surface due to the homogeneous mixing between PLA and PEG [48]. The green composite fibers have slightly rough surfaces and good adhesion between GTL and matrix which might be due to the small size of the GTL, resulting in good dispersion and distribution in the PLA matrix. Thermal properties Figure 6 shows the DSC thermograms of the PLA/PEG fiber Fig. 6  DSC thermograms of the PLA/PEG fiber and the green com- and the green composite fibers, whereas the calorimetric posite fibers parameters are summarized in Table 3. Fig. 5  SEM images of cross-section surfaces of a the PLA/PEG fiber and the green composite fibers, with different masterbatch contents at b 5, c 10, 15, and d 20 phr 13

Journal of Material Cycles and Waste Management Table 3  Thermal parameters Samples Temperature ( °C) ∆Hc (J/g) ∆Hm (J/g) Xc (%) from DSC for the PLA/PEG fiber and the green composite PLA/PEG Tg Tc Tm 17.75 26.62 9.47 fibers PLA/PEG + GTL-5 10.06 29.74 21.02 PLA/PEG + GTL-10 61.54 92.50 155.00 13.01 32.95 21.30 PLA/PEG + GTL-15 52.92 75.00 156.50 8.18 23.36 16.21 PLA/PEG + GTL-20 52.81 79.83 156.50 13.91 36.91 24.57 55.29 88.17 157.17 53.25 79.17 156.33 from 88.17 to 75.00 °C, because the ground tea leaves act as a nucleating agent promoting crystallization of PLA [51]. Crystallinity (Xc) of the PLA/PEG fiber was found to be 9.47%. Increasing the masterbatch contents showed the increment of crystallinity from 16.21 to 24.57%. It can be confirmed that the nucleation was generated by incorporat- ing the organic fillers as GTL to the PLA matrix. This is in agreement with the previous work reported by Ouchiar et al. [52] and Barczwski et al. [20]. The melting temperature (Tm) of the PLA/PEG fiber was 155.00 °C, while the masterbatch content increased with a slight rise in the melting temperature to around 157.17 °C. This agreed with the results presented by R. Pantani et al. [53] and B. W. Chieng et al. [43]. Dye removal The dye removal of the PLA/PEG + GTL-5 was studied Fig. 7  Dye removal property of PLA/PEG + GTL-5 fiber on a Meth- using methylene blue (MB) and reactive blue 19 (RB) dyes, ylene blue and b Reactive blue dye, under room temperature as shown in Fig. 7a and b, respectively. It was observed that the MB removal efficiency of PLA/PEG + GTL-5 composite Here, PLA/PEG + GTL-5 composite fabric was used as a fiber is 81 and 100% after 24 and 48 h, respectively. How- model study as this composite fabric, prepared from PLA/ ever, the RB dye removal efficiency of PLA/PEG + GTL-5 PEG + GTL-5 composite fiber, showed the best mechanical composite fiber is 36 and 100% after 24 and 48 h, respec- property. Results showed that the PLA/PEG + GTL-5 compos- tively, perhaps because GTL can adsorb dye color or cleav- ite fabric can inhibit S. aureus, B. subtilis, and C. albicans at age of chromophore bonds in the dye molecule. These results up to 65.57%, 94.44%, and 7.69%, respectively. Moreover, the agree with previous evidence presented by Nasuha et al. [54] bacteria population significantly decreased all along the incu- who reported that the rejected tea can be used as an effective bation time. This revealed that the GTL particles, dispersed adsorbent for methylene blue removal. Reza et al. [55] also within the PLA matrix, acted as an antimicrobial agent, espe- reported that tea waste showed excellent adsorption for the cially for inhibiting the growth of Gram-positive bacteria. The removal of reactive blue from aqueous solutions. However, obtained results agree with the antimicrobial property of tea the composite fiber can absorb cationic dye (MB) rather than found in previous studies [56, 57]. Moreover, Erdohan et al. anionic dye (RB) after 24 h, perhaps due to the structures prepared the antimicrobial poly(lactic acid)-based films using of tea and PLA, consisting of polar groups as hydroxyl and the olive leaf extract (OLE) as an antimicrobial agent. It was carbonyl groups, including the ether linkage, which can found that the OLE did not show any effect to decrease or interact with methylene blue as a cationic dye. Moreover, inhibit the degradability rate of composite materials. However, these groups did not show significant absorption after 48 h. Antimicrobial property of the green composite fabric The antimicrobial property of the green composite fabrics has been studied using S. aureus, B. subtilis, and C. albi- cans as model microbials, as shown in Table 4 and Fig. 8a–c. 13

Journal of Material Cycles and Waste Management Table 4  Number of colonies and percentage inhibition against of the green composite fabric Microbial Initial concentration (cfu/ml) Number of colonies (cfu/ml) percentage reduction Staphylococcus aureus (S. aureus) 142.33 × ­108 ± 6.66 × 1­ 08 49.00 × ­108 ± 5.57 × 1­ 08 (%) Bacillus subtilis (B. subtilis) 18.00 × ­107 ± 1.00 × ­107 1.00 × 1­ 07 ± 1.00 × ­107 13.00 × 1­ 07 ± 2.00 × 1­ 07 12.00 × 1­ 07 ± 1.00 × ­107 65.57% Candida albicans 94.44% (C. albicans) 7.69% Conclusion Ground tea leaves from waste consumption and poly(ethylene glycol) were successfully used as a filler and a plasticizer, respectively, in poly(lactic acid) to pre- pare green composite fibers. The green composite fib- ers showed a light green to dark green color, according to the increment of the ground tea leaf contents. The PLA/ PEG + GTL-5 showed the best mechanical property as the highest values of tenacity (16.47 cN/tex) and elongation at break (103.50%). The cross-sectional surface of the green composite fiber showed a rough surface, and the size of the fibers was found to be 15–20 μm. The green composite fibers showed the decrement of glass transition and crystallization temperature (52.29–53.25 °C), and the slight increment of melting temperature (156.33–157.17 °C) and crystallinity (16.21–24.57%) compared to that of the PLA/PEG fiber. Besides, the green composite fiber with dye removal and anti-bacterial properties, especially Gram-positive bacteria, can be used to make anti-bacterial green composite fabrics for waste-water treatment. Acknowledgements  The authors would like to thank the following for their financial support: The National Research Council of Thailand (NRCT), and The Institute of Research and Development, Rajaman- gala University of Technology Thanyaburi (RMUTT), Thailand. The authors would also like to express their thanks to the following for its support of the processing machines: The Department of Textile Engi- neering, Faculty of Engineering, Rajamangala University of Technol- ogy Thanyaburi (RMUTT), Thailand. Fig. 8  Physical appearances of the petri dishes with a S. aureus b References B. subtilis and c C. albicans for (right) control and (left) the PLA/ PEG + GTL-5 fabric 1. Raquez JM, Habibi Y, Murariu M, Dubois P (2013) Polylactide (PLA)-based nanocomposites. Prog Polym Sci 38:1504–1542. by increasing the amount of olive leaf extract (OLE) in the https://​doi.​org/​10.​1016/j.​progp​olyms​ci.​2013.​05.​014 PLA matrix, the degradability rate of composite materials was increased. [31]. 2. Ye F, Dong S, Tian Z, Yao S, Zhou Z, Wang S (2013) Fabrica- tion of the PLA/Sr2MgSi2O7:Eu2+, ­Dy3+ long-persistent lumines- cence composite fibers by electrospinning. Opt Mater 36:463–466. https://​doi.​org/​10.​1016/j.​optmat.​2013.​10.​019 3. Ye F, Dong S, Tian Z, Yao S, Zhou Z, Wang S (2015) Fabrication and characterization of long-persistent luminescence/ polymer ­(Ca2MgSi2O7:Eu2+, ­Dy3+/PLA) composite fibers by electrospin- ning. Opt Mater 45:64–68. https://d​ oi.o​ rg/1​ 0.1​ 016/j.o​ ptmat.2​ 015.​ 03.​011 13

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