JIT-23-0218 Proof Hi

Journal of Industrial Textiles
The biodegradation of natural fibre-reinforced composites

after cold plasma treatments
Journal: Journal of Industrial Textiles
Manuscript ID JIT-23-0218
Manuscript Type: Original Manuscript

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Smart textiles, composites < Materials, Technical textiles, Industrial
Keywords:
textiles, Specialty textiles, materials < Materials
This study investigates the application of plasma treatment as a means

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to enhance biodegradation and modify the structural characteristics of

fibrous composites. The methodological component of the study includes
the selection of the research object; production of composites; low-
temperature plasma treatment, and treatment of biodegradability and
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mechanical strength of samples. The strengthening of fibers with

cellulose leads to a significant improvement in mechanical strength. Such
an indicator as mechanical strength increased from 18 to 21 MPa, or by
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16.7%. Treatment of natural fibers with low-temperature plasma led to

an increase in mechanical strength from 18 to 25 MPa, or by 33.3%.
Treatment of reinforced fibers with low-temperature plasma led to an
even greater increase in mechanical strength, namely from 18 to 29 MPa
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or by 50%. The electron microscopy of samples revealed some

Abstract:
differences in cell wall microfibrils between plasma-treated and non-
treated samples. The non-treated fibres were found to have chips and
voids. Meantime, the plasma-treated fibres show structural changes in
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certain regions which resemble wood charring. Through a comprehensive

analysis, this research underscores the substantial impact of plasma
treatment on the degradation kinetics and morphological features of
cellulose-based composites. The results reveal distinct alterations in the
composition and behaviour of plasma-treated fibres, signifying a shift
towards enhanced biodegradability. The natural fibres examined in this
study contained 28-30% lignin, whereas the composites exhibited a
lower lignin content of 21-23%. These findings corroborate the inference
that plasma treatment induces significant changes in fibre structure,
accelerating the biodegradation process by 7 days.
http://mc.manuscriptcentral.com/JIT
Page 1 of 57 Journal of Industrial Textiles
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3 The biodegradation of natural fibre-reinforced composites after cold plasma treatments
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8 Abstract
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10 This study investigates the application of plasma treatment as a means to enhance
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biodegradation and modify the structural characteristics of fibrous composites. The
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15 methodological component of the study includes the selection of the research object; production
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17 of composites; low-temperature plasma treatment, and treatment of biodegradability and
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19 mechanical strength of samples. The strengthening of fibers with cellulose leads to a significant
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22 improvement in mechanical strength. Such an indicator as mechanical strength increased from

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24 18 to 21 MPa, or by 16.7%. Treatment of natural fibers with low-temperature plasma led to an
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26 increase in mechanical strength from 18 to 25 MPa, or by 33.3%. Treatment of reinforced fibers
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with low-temperature plasma led to an even greater increase in mechanical strength, namely
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31 from 18 to 29 MPa or by 50%. The electron microscopy of samples revealed some differences
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33 in cell wall microfibrils between plasma-treated and non-treated samples. The non-treated
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fibres were found to have chips and voids. Meantime, the plasma-treated fibres show structural
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38 changes in certain regions which resemble wood charring. Through a comprehensive analysis,
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40 this research underscores the substantial impact of plasma treatment on the degradation kinetics
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42 and morphological features of cellulose-based composites. The results reveal distinct alterations
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45 in the composition and behaviour of plasma-treated fibres, signifying a shift towards enhanced
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47 biodegradability. The natural fibres examined in this study contained 28-30% lignin, whereas
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49 the composites exhibited a lower lignin content of 21-23%. These findings corroborate the
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inference that plasma treatment induces significant changes in fibre structure, accelerating the
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54 biodegradation process by 7 days.
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56 Keywords: biodegradability, composites, degradation, discharge, fibres, plasma.
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Journal of Industrial Textiles Page 2 of 57
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3 Introduction
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The lightweight materials industry is a strategically important sector of the economy in many
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8 countries. Due to the growing population, the demand for clothing, footwear, and other textile
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10 products increases each year. At the same time, lightweight materials industry products must
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meet strict requirements related to hygiene, durability, and performance properties such as
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15 adhesion, water resistance, and so forth. Compliance and product quality largely depend on the
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17 methods and technologies used to manufacture and process natural and synthetic materials.1,2
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19 The textile industry makes use of both natural and synthetic materials. Man-made fibres are
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22 used to create new non-woven and artificial materials or impart specific properties to those
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24 materials. Synthetic fibres are superior to some products and inferior to others; hence, the choice
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26 of synthetics may be justified. However, polymeric materials do not decompose easily, and
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represent a serious threat to the environment in countries with intense production. According
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31 to recent reports, nearly 30% of polymer waste is subjected to incineration, some 30% is
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33 recycled, and the remaining 30% is left undisposed.3-5
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Scholars are actively engaged in the advancement of novel synthetic polymers designed for
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38 degradation by bacteria and other microorganisms within the natural ecological milieu.6,7 These
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40 polymers can be useful in many industries, including packaging, the textile industry, medical
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42 equipment, the automotive industry, and so forth.8 Recent studies have also investigated the use
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45 of plasma for processing synthetic polymers to increase their biodegradation. Plasma treatment
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47 can change the surface structure of the polymer, thereby providing a more efficient
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49 decomposition of the synthetic material by biological processes.9-11
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The study of biodegradation of synthetic polymers exhibits certain gaps. Unexplored areas
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54 encompass the pathways of biodegradation for various polymer types, factors influencing
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56 biodegradation, resultant products, and novel biodegradation methods.12 Some researchers posit
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that successful biodegradation of the synthetic component within a natural-synthetic blend
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3 occurs when the natural polymer is chemically attached (grafted) to the synthetic polymer.
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Bacterial activity initiates the degradation of the natural polymer chain, which subsequently
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8 extends into the synthetic segment.13-15
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10 The work16 uses epoxy as a matrix material, and polymer composites with reinforcement from
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untreated and alkali-treated Zanthoxylum acanthopodium bark fibres (5–25 wt.%). Hand lay-
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15 up was used in the development of the epoxy composites. The mechanical characteristics and
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17 water absorption rates of the produced epoxy composites were evaluated following ASTM
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19 standards. Epoxy composites containing 20 wt.% of alkali-treated Zanthoxylum
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22 acanthopodium bark fibres had excellent mechanical qualities, including an ultimate tensile
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24 strength of 47.3 MPa, according to the test findings. However, there was a positive correlation
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26 between fibre loading and water absorption. The fibre bonding and void properties of the
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investigated composites were viewed with a scanning electron microscope.
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31 In the work,17 Vachellia farnesiana fibres were selected and extracted by the manual retting
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33 process. The obtained Vachellia farnesiana fibres were chemically treated with hydrochloric
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acid (HCl) and sodium hydroxide (NaOH) solutions. The chemically treated and
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38 untreated Vachellia farnesiana fibres were characterized for physical, chemical, tensile,
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40 morphological, and thermal properties. Test results showed that the cellulose content was
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42 47.8 ± 0.697 wt % for NaOH-treated Vachellia farnesiana fibres with reduced moisture and
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45 amorphous contents. HCl-treated Vachellia farnesiana fibre showed more cellulose content
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47 removal, which resulted in the degradation of its properties due to the acidic nature of HCl.
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49 Plasma treatment is recognized as a dry and clean process. The utilization of low-pressure cold
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plasma for the pre-treatment of natural fibres is becoming increasingly prevalent as a novel
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54 method for surface modification.18 This approach offers advantages compared to traditional
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56 chemical treatment, as it does not require water or chemicals, rendering it environmentally
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friendly and cost-effective. Plasma modification substantially reduces the number of chemical
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3 pollutants. It etches the fibre surface, enhancing the action of the binding agent for improved
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adhesion.19 It can also render the surface rough through material ablation, enhancing adhesion.
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8 Moreover, it introduces free radicals and can alter the chemical structure. Low-pressure cold
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10 plasma modifies the fibre surface without changing the material volume. Additionally, it
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eliminates the need for chemical solvents and reduces process time.20
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15 Existing studies lack a comprehensive examination of the biodegradability of plasma-modified
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17 fibres. This article investigates the influence of low-temperature plasma treatment on the
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19 biodegradation of cellulose and its composite. The results provide insights into assessing the
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22 biodegradability of other materials. The study underscores the potential of plasma treatment in
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24 enhancing the quality of natural and synthetic fibres. Low-temperature plasma treatment of
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26 cellulose-based materials is employed for this purpose.
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Most studies note that low-temperature plasma treatment is a progressive and rather effective
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31 method since it can change the chemical composition of the fibre surface and the physical
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33 structure of molecules while maintaining the bulk material properties. Utilizing low-
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temperature and low-pressure plasma treatment demands a lesser amount of gasoline when
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38 contrasted with alternative techniques, leading to a near-total mitigation of waste generation.
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40 However, there are limited data on the biodegradability of plasma-treated fibres. The empirical
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42 evidence that fibre materials can partially or completely decompose after plasma treatment and
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45 that it affects the rate of biodegradation can serve as justification for the use of plasma treatment
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47 with a wider range of natural and synthetic fibres.
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49 This study aims to measure the biodegradability of plasma-treated wood fibre-reinforced
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polypropylene composites to determine whether plasma modification alters the rate of
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54 biodegradation. The secondary objectives of the study are (1) to examine the low molecular
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56 weight components of wood fibre-reinforced polypropylene composites during biodegradation;
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and (2) to explore the composition and properties of substances isolated from the plasma-treated
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3 samples. Finally, the study attempts to experimentally substantiate the mechanism behind the
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plasma-induced decomposition of cellulose fibres and theoretically determine the
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8 biodegradation time of materials under study.
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Methods and materials
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15 The flowchart of the experimental part is shown in Figure 1.
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43 Figure 1. The flow-chart of the experimental part
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48 The production of wood fibre-reinforced polypropylene composites
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50 This study addresses natural fibres of the finest coniferous wood species and cellulose-
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containing materials as experimental objects. These were unbleached softwood sulfate pulp and
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55 softwood sulfate lignin. The sample of natural wood fibres was analyzed using a scanning
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57 electron microscope. The SEM analysis method included the following steps: sample
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preparation, sample loading, vacuum chamber, and electron beam directed at the sample. The
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3 latter interacted with the sample, causing electron emission from the sample surface. Electron
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detection: a detector located in the SEM chamber identified electrons emitted by the sample.
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8 These signals were then processed and used to create an image of the sample’s surface
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10 topography and morphology.
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The results demonstrated that the average length of wood fibres was 190 µm (range, 100 to 400
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15 µm; standard deviation: 63 µm) and that the average width was 50 µm (range, 20 to 100 µm;
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17 standard deviation: 19 µm).
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19 Table 1 shows the approximate composition of fibre samples.21
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22 Table 1. The approximate composition of fibre samples.

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24 The composition, % Natural fibre Cellulose composite
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26 cellulose 46-48 18-20
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29 hexosans 10-12 12-14

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31 pentosanes 8-10 8-9
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33 lignin 28-30 21-23
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36 organic acids 4-5 3-4

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38 polypropylene - 35-37
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43 The production of polypropylene/cellulose composites requires using a solid-state shear
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45 pulverization. The sheared polymer method helped to reduce the particle size of cellulose
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47 materials. The cellulose fibres were mixed by ourselves with a polypropylene matrix in a plastic
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50 mixer (Haake Rheocord 9000, Germany) with a rotor velocity of 60 rpm at 185°C for 8 minutes.
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52 The resulting blend underwent compression molding at 185°C at a pressure of 10 MPa for 15
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54 min. Before being used, the samples rested at room temperature for 5 days.
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Figure 2 shows the scheme of the reactor.
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27 Figure 2. The reactor’s scheme
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The plasma reactor consists of a solenoid or radio-frequency induction coil (A) wound around
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34 a borosilicate glass tube (B). There will be a supply of gas (C) in the vacuum, and a vacuum
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36 pump valve (D) will keep the gas inside. The induction coil is to store energy within a magnetic
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field, which is numerically equal to that produced by the source to induce a current in the
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41 winding, generating a magnetic field of the solenoid. Inside the external glass tube, there is a
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43 partially open glass tube (E). It contains fibres that a stepper motor rotates (F) throughout the
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entire plasma treatment process.
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48 Low-pressure and low-power plasma does not cause excessive surface heating, and the glass
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50 tube is warm to the touch. Therefore, there is no excessive thermal exposure, thermal
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52 degradation of the fibres, or their incineration to be expected.
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55 The parameters of low-temperature plasma are as follows: I = 4.8–5.2 mA; U = 25-28 kW; gas
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57 medium: sulfur hexafluoride (SF6); additional medium – water (Н2О); exposure time = 10-30
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59 min; Р = 102 Pa.
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The plasma treatment procedure is described below
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8 1) The glass tube and the sample holder are cleaned with an air gun and disinfected with
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10 isopropyl alcohol to eliminate any contamination of the vacuum and plasma. All individuals
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involved in the experiment are required to wear nitrile gloves to prevent contamination.
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15 2) A 5-gram sample of investigated fibres is weighed and placed on the sample holder (internal
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17 glass tube (E) as shown in Figure 2). The tube is inserted into the reactor and attached to the
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19 axis of the stepper motor for further rotation of the sample.
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22 3) Once the reactor is closed, the air is evacuated by a vacuum pump. The pump must be
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24 connected to the reactor through a chamber equipped with a diaphragm valve. The latter opens
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26 slowly at the evacuation starts to prevent fibres from being absorbed in.
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4) As soon as the pressure falls below 10 Pa, the stepper motor starts rotating, causing the
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31 sample holder to rotate and the fibres to mix. A short-term increase in pressure occurs due to
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33 the release of accumulated gas.
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5) The selected process gas (partially or fully ionized; with no signs of being polymerized) is
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38 introduced into the chamber using a needle valve or mass flow controller. During pumping, the
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40 pressure increases to almost 102 Pa for 2 min, and then the gas supply is over. The procedure is
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42 repeated after 2-5 min of further pumping. This ensures a faster decrease in pressure as moisture
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45 transport occurs and guarantees enough gas in the tube.
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47 6) Finally, the system is pumped down to an atmospheric pressure of about 10-1 Pa. Because
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49 fluorocarbon bonds are sensitive to X-ray, the following sequence was followed: initial phase:
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250-350 eV; final phase: 0-1,150 eV; high-resolution oxygen spectrum, binding energy: 526 to
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54 540 eV.
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56 The equipment used here includes a gas chromatograph СhroZen UHPLC, a gas
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chromatograph-mass spectrometer GCMSQP2010 Plus, a thermal desorber TD-20, an ATR-
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3 8200HA attachment (Pike Tech), a scanning electron microscope (SEM) Sigma VP ZEISS, and
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a probe microscope MultiMode 8. The chemical analysis was compliant with GOST.22 Results
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8 were analyzed by gas chromatography using gas chromatograph Agilent 7820.
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Mechanical Testing
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15 Tensile testing (ISO 527) was carried out using a universal testing machine (UTM) with a
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17 gauge length of 6 cm and a speed of 5 mm/min. All the mechanical results were obtained with
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19 an average of 10 samples.
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24 Biodegradability testing
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26 The biodegradability test assessed the resulting cellulose composite’s ability to decompose
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under the influence of microorganisms within certain environmental conditions. The samples
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31 were buried in the soil for 30 days. This method is widely used for assessing the ability to
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33 decompose since it provides a simulated environment similar to natural decomposition.
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During testing, the samples were buried to a depth of 10-15 centimetres and covered with soil.
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38 The monitoring of soil humidity and temperature ensured that they remained within a certain
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40 range for microbial activity (25-75% and 15-25 °C, respectively). After 30 days, samples were
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42 excavated from the soil and analyzed for the presence and amount of material residues. The
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45 degradation degree was then identified by measuring mass loss.
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49 Statistics analysis
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Statistical analysis was performed using a One-way Analysis of Variance, with significance
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54 reported at p≤0.05. All findings were presented as means ± standard deviations of at least five
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56 experiments.
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3 Results and discussion
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Plasma modification of the fibre surface is one of the most elaborated methods for improving
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8 the quality characteristics of materials. Plasma treatment can affect the surface properties of
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10 materials, such as the ability to bond dissimilar fibres. The adhesion of materials is often used
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to metalize, paint, or glue surfaces to obtain composites. This method also makes it possible to
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15 develop a range of properties less typical for unprocessed natural fabrics, such as hydrophilicity,
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17 dirt and dust repellency, antistatic properties, and so forth. In addition, plasma removes fat and
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19 other organics from fur and wool. It improves the absorption of dye pigments.23,24
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22 The essence of the plasma treatment method is to treat a material with a plasma medium
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24 (ionized gas) at low or atmospheric pressure. This causes surface reactions and modifications
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26 up to a change in the functional groups of molecules and a change in surface energy. Plasma is
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an ionized gas, in which free electrons and ions coexist. Plasma is produced by heating a gas to
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31 extremely high temperatures or by subjecting it to strong electromagnetic fields. Both of these
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33 processes may result in the release of electrons from atoms and molecules. The electrons have
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enough kinetic energy to remove additional electrons in case of a collision with other
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38 molecules.25 These collisions induce cascade ionization. A release of new ions and electrons
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40 occurs, balanced by the recombination of material molecules until plasma reaches equilibrium.
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42 The results obtained by Hamad26 show that plasma treatment of keratin-containing materials,
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45 such as wool and fur, at reduced pressure, opens the fibre cuticle, caused by the mutual
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47 repulsion of multiple charged jets. This allows effective removal of organic compounds from
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49 the merino wool fibres, without changing the fibre structure and physical properties.27 Zille28
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evaluated the effects of plasma surface treatment of flax, cotton, and animal-based fibres (wool,
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54 pile) on the tensile load resistance. Plasma treatment activates the surface of various synthetic
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56 materials, such as ultra-high modulus polyethylene, thereby improving their ability to absorb
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3 or completely repel moisture. This occurs due to the increase in surface tension of the fibres
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immersed in various gaseous media.9,11,13
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8 It is worth mentioning that some scientists29-32 agree that plasma treatment reduces the total
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10 energy consumption associated with the production of synthetic fibres by 25% as compared to
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other treatment methods. Research demonstrates that the modification of natural fibres requires
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15 14 to 50% less energy than the production of synthetic fibres. The real value in this broad range
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17 depends on a myriad of plant growth factors and plasma processing parameters.
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19 The results of determining the mechanical strength of the obtained fibers are given in Table 2.
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22 Table 2. Results of mechanical testing

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24 Sample Tensile strength, MPa
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26 Nature fiber 18
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29 Reinforced fiber 21
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31 Plasma treated nature fiber 25
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33 Plasma treated reinforced fiber 29
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38 Analyzing the data presented, we can come to the conclusion that strengthening fibers with
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40 cellulose leads to a significant improvement in mechanical strength. In particular, such an
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43 indicator as mechanical strength increased from 18 to 21 MPa, or by 16.7%. Treatment of
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45 natural fibers with low-temperature plasma led to an increase in mechanical strength from 18
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47 to 25 MPa, or by 33.3%. Treatment of reinforced fibers with low-temperature plasma led to an
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even greater increase in mechanical strength, namely from 18 to 29 MPa or by 50%.
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52 The electron microscopy of cellulose samples revealed some differences in cell wall
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54 microfibrils between plasma-treated and non-treated samples (Figure 3). The non-treated fibres
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were found to have chips and voids. Meantime, the plasma-treated fibres show structural
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59 changes in certain regions which resemble wood charring.
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29 Figure 3. Microscopic examinations of cellulose: (a, c) – no plasma treatment, (b, d) – plasma

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36 Interestingly, following plasma treatment, certain segments of the cellulose fibre exhibited a
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38 hollowed morphology. In contrast, the control sample displayed increased fragility due to the
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41 presence of voids and ruptures in the cell walls. This implies that plasma treatment influenced
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43 the microfibril structure of cellulose. Typically, reinforcing elements of microfibrils were
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45 diminished as a result of plasma treatment, enhancing flexibility and disrupting structural
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integrity.
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50 When investigating the composite of polypropylene fibres reinforced with cellulose (Figure
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52 4), a distinct behaviour was observed following plasma treatment. The fibres of the treated
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54 composite exhibited fewer visible defects and were predominantly embedded within the
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57 polypropylene matrix. Importantly, no slip lines or voids were evident on the fracture surface.
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3 Instead, the images displayed polymer adhesion to the fibres at multiple points, indicating a
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noteworthy transformation of material composition and interactions.
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Figure 4. The surface morphology of cellulose-reinforced polypropylene: (A, C) – no plasma

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38 treatment, (B, D) – plasma treatment.
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42 High interfacial shear strength and, consequently, a stronger interaction between fibres and
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matrices can significantly decelerate the biodegradation of composite materials. Plasma
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47 changes the structure of cellulose, with the latter completely dissolved in a solution of sodium
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49 hydroxide and simply in water. Low molecular weight components occur during
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51 depolymerization. Nearly 50 products were generated through the plasma-chemical
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54 decomposition of fibres; some (19%) are listed in Table 3. By comparing the quantitative
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56 composition of components in the table, significant differences between the degradation
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58 products of plasma-treated and untreated fibres can be identified. Specifically, several
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3 compounds exhibit changes in molecular mass and percentage yield as a result of plasma
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treatment. For instance, compounds such as C6H10O5, 3-deoxyglucofuranose, and C6H6O3
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8 display altered molecular masses and percentage yields following plasma treatment, indicating
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10 the influence of plasma on the degradation process. These variations underscore that plasma
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treatment affects the molecular structure, which, in turn, may impact the biodegradation of
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15 composites.
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17 Table 3. Products resulting from the biodegradation of plasma-treated and non-treated fibres
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Compound name Plasma treatment No plasma treatment
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22 Percent Percent
23 Molar mass, g/mol Molar mass, g/mol
24 yield,% yield,%
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26 С6Н10О5 162 ±0.4 7.92 172 ±0.8 8.12
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29 3-dezoxyglukozenone 144 ±0.9 10.1 150 ±0.4 11.3

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31 Мetylmaltol 142 ±0.6 6.12 149 ±0.3 7.3
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С6H6O3 126 ±0.7 20.1 136 ±0.1 21.4
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36 1,6-angydryd-3,4-
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38 didezoxy-Р-0-pyranoz-3- 126 ±0.6 4.56 114±0.2 5.3
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40 an-2-one
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43 C6H6O 110 ±0.2 1.12 126 ±0.6 1.96
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45 C5H6O2 98 ±0.3 5.11 102 ±0.7 6.23
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47 2-acetyl-5-methylfuran 98 ±0.5 1.52 134 ±0.9 1.91
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50 C5H4O2 96 ±0.6 2.79 117 ±0.8 3.18
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52 γ-krotonolactone 84 ±0.9 1.12 101 ±0.2 1.78
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2-methylfuran 82 ±0.4 0.56 95±0.9 0.95
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57 C4H4O 68 ±0.2 1.52 84 ±0.4 1.87
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59 CH₃COOH 60 ±0.1 0.25 75 ±0.6 0.54
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3 CH₂O₂ 46 ±0.6 0.25 57 ±0.7 0.62
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8 The yield of levoglucosan (C6H10O5) was 7.92%, suggesting the achievement of stability after
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10 plasma treatment. A rather large amount (10.1%) of 3-dioxyglucosenone is released with a
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molecular weight of 144 g/mol during cellulose dehydration. The concentration of methyl
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15 maltol is lower (6.12%) but its molar mass is almost the same as that of 3-dioxyglucosenone.
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17 Two substances with the same molar mass of 126 g/mol, pyrogallol and anhydrosucrose,
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account for 4.56 and 20.1% of the yield, respectively. A furan aldehyde called furforol (C5H6O2)
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22 is released in the amount of 5.11%; part of furfural can be released with the participation of
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24 xylane. All molecules with a mass below 90 Da are marked as decay products of O2 and CO2.
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26 Plasma does not affect sulfate lignin. The plasma-treated natural fibres were 21% lignin,
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29 whereas the composites had a lignin content of 18%. The study results show that the
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31 dehydration and decomposition velocities of non-composites are almost 2 times lower as
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33 compared to composites. In natural conditions, lignin is strongly influenced by filamentous
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fungi, which have the power to cause the degradation of complex polymers by enzymes; in
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38 these conditions, materials decompose faster.
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40 Judging by data concerning the degradation products of plasma-treated fibres, the chemical
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42
processes associated with the biodegradation of natural cellulose are similar to those occurring
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45 in untreated samples. The structural changes to microfibrils, however, caused the
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47 biodegradation time of plasma-treated cellulose to accelerate.
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49 In the case of plasma-treated specimens, biodegradation commenced on the 12th day of the
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52 experiment, while for untreated specimens, it occurred a week later, specifically after 19 days.
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54 The buried plasma-treated material changed and became brittle and thinner than the control. At
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56 the end of the 30-day biodegradation test, prominent changes were detected in the samples.
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1
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3 The biodegradation of natural fibre-reinforced composites can occur through a variety of
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mechanisms; the choice depends on the type of natural filler used, its quality, and its chemical
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8 composition. The plasma-treated cellulose-reinforced polypropylene composites exhibit clear
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10 signs of decomposition. This finding coincides with previous research. It also suggests that
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plasma-treated fibre materials can decompose, partially or completely, and that plasma
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15 treatment can alter the rate of biodegradation.
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17 This study aligns with previous research emphasizing the significance of incorporating
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19 environmentally degradable components into composite materials.33 Earlier investigations
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22 examined fibre degradation alongside polylactic acid and clay silicates, revealing that the
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24 quantity and nature of natural constituents influence composite biodegradation.33
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26 Correspondingly, analogous burial-based studies.34-36 echo our findings, showcasing the
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accelerated degradation of triple compositions compared to double ones due to increased
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31 biodegradable content. Moreover, experts in plasma treatment advocate its efficacy in
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33 preserving textile properties and enhancing mechanical attributes of biodegradable composites,
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considering it more sustainable than chemical methods.37-41

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38 The choice between plasma and chemical treatment hinges on material requisites.39-41 Plasma
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40 treatment surpasses chemical counterparts in efficacy, transforming material surfaces,
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42 enhancing adhesion, and durability.42-44 This approach is particularly useful for biodegrading
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45 recalcitrant materials by promoting microbial interaction.45-47 Similarly, studies focusing on
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47 fibre-modified bioplastics suggest enhanced fibre-matrix adhesion.39,40 Cold plasma emerges
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49 as an efficient, eco-friendly alternative,38-41 fostering sustainable composite markets.
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This holistic exploration of plasma-treated materials showcases their potential in renewable and
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54 biodegradable materials research.45,48,49 Industrial use of plasma-modified materials
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56 necessitates eco-conscious biodegradability. Consequently, leveraging natural fibres for
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polymer matrix composites aligns with environmental awareness and promotes renewable
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1
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3 resources.33,50,51 Such studies aid in curbing waste and toxic releases, ensuring safer
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decompositions and material cycles. This research contributes to reducing environmental
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8 impact while bolstering sustainable material applications.
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Conclusions
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15 Through the utilization of scanning electron microscopy (SEM), the study demonstrated that
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17 plasma treatment has a substantial impact on both the process of biodegradation and the
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19 structure of the material. Scanning electron microscopy (SEM) enabled a thorough
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22 investigation of the procedural stages, with a specific emphasis on the interaction between
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24 electrons and the specimen. The methodological aspect of the study encompassed the selection
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26 of the research subject, fabrication of composites, application of low-temperature plasma
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treatment, and evaluation of the biodegradability and mechanical strength of the samples. The
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31 incorporation of cellulose fibers results in a substantial enhancement of mechanical strength.
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33 Specifically, the mechanical strength indication rose from 18 to 21 MPa, representing a 16.7%
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increase. Application of low-temperature plasma to natural fibers resulted in a 33.3%

36
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38 enhancement in mechanical strength, increasing it from 18 to 25 MPa. Reinforced fibers
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40 subjected to low-temperature plasma treatment exhibited a significant enhancement in
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42 mechanical strength, namely from 18 to 29 MPa, or a 50% increase. The electron microscopy
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45 analysis of the samples unveiled significant disparities in cell wall microfibrils between the
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47 plasma-treated and non-treated samples. Chips and cavities were seen in the untreated fibers.
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49 Meanwhile, the fibres that have undergone plasma treatment exhibit structural alterations in
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specific areas that bear resemblance to the charring of wood. The cellulose cell walls of treated
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54 and untreated samples showed differences in the microfibrils, including changes in structure
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56 after plasma treatment. Furthermore, there were also observed alterations in composites
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including polypropylene fiber and cellulose. The fibres that underwent plasma treatment
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1
2
3 showed improved integration, as evidenced by the lack of slip lines on the fracture surface.
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The table displaying the quantitative measurement of biodegradation products indicates notable
7
8 variations in composition between the treated and untreated fibers. These modifications
9
10 demonstrate the impact of plasma on chemical reactions and biodegradation. Plasma treatment
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can speed up the process of biodegradation and alter the properties of materials. This has the
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15 potential to create composites that are more long-lasting and resistant, which is important for
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17 the production of environmentally sustainable materials and the efficient use of waste.
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19
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22 References
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24 1. Ameer MH, Shaker K, Ashraf M, et al. Interdependence of moisture, mechanical properties,
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26 and hydrophobic treatment of jute fibre-reinforced composite materials. J Text Inst
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8 10.1177/0040517519883954.
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8 32. Nguyen Thi H, Vu Thi Hong K, Ngo Ha T, et al. Application of plasma activation in flame-
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33 36. Gibeop N, Lee DW, Prasad CV, et al. Effect of plasma treatment on mechanical properties
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42 resource for development of eco-friendly composites: A comprehensive review. Front Mater
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47 38. Vinod A, Vijay R, Singaravelu DL, et al. Characterization of untreated and alkali treated
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49 natural fibres extracted from the stem of Catharanthus roseus. Mater Res Express 2019; 6:
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54 39. Lahouioui M, Ben Arfi R, Fois M, et al. Investigation of fibre surface treatment effect on
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15 41. Sumesh KR, Kanthavel K, Kavimani V. Peanut oil cake-derived cellulose fibre: extraction,
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17 application of mechanical and thermal properties in pineapple/flax natural fibre composites. Int
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19 J Biol Macromol 2020; 150: 775–785. DOI: 10.1016/j.ijbiomac.2020.02.118
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22 42. Vijay R, Lenin Singaravelu D, Vinod A, et al. Characterization of raw and alkali treated
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24 new natural cellulosic fibres from Tridax procumbens. Int J Biol Macromol 2019; 125: 99–108.
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26 DOI: 10.1016/j.ijbiomac.2018.12.056
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31 treated new natural cellulosic fibres extracted from the aerial roots of banyan tree. Int J Biol
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33 Macromol 2019; 138: 573–581. DOI: 10.1016/j.ijbiomac.2019.07.136
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38 cellulose-based fibres and their interfacial interaction in composite systems. BioResources
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40 2017; 12: 5449-5461.
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42 45. Ojha AR, Biswal SK. Thermo physico-mechanical behavior of palm stalk fibre reinforced
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45 epoxy composites filled with granite powder. Compos Commun 2019; 16: 158–161. DOI:
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47 10.1016/j.coco.2019.10.003
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49 46. Krishnan T, Jayabal S, Krishna VN. Tensile, flexural, impact, and hardness properties of
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alkaline-treated Sunnhemp fibre reinforced polyester composites. J Nat Fibres 2020; 17: 326–
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54 336. DOI: 10.1080/15440478.2018.1492488
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3 47. Mohana Krishnudu D, Sreeramulu D, et al. Alkali treatment effect: mechanical, thermal,
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morphological, and spectroscopy studies on Abutilon indicum fibrereinforced composites. J
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8 Nat Fibres 2020; 17: 1775-1784. DOI: 10.1080/15440478.2019.1598917.
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10 48. Premnath AA. Impact of surface treatment on the mechanical properties of sisal and jute
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reinforced with epoxy resin natural fibre hybrid composites. J Nat Fibres 2019; 16: 718–728.
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15 DOI: 10.1080/15440478.2018.1432002
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17 49. Saba N, Alothman OY, Almutairi Z, et al. Magnesium hydroxide reinforced kenaf
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19 fibres/epoxy hybrid composites: mechanical and thermomechanical properties. Constr Build
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24 50. Artamonov V, Vorona-Slivinskaya L, Medvedeva A. The algorithm of sustainable
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26 development of organizations: A social aspect. Procedia Eng 2016; 165: 1192–1196. DOI:
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31 51. Voskresenskaya E, Vorona-Slivinskaya L, Achba L. Digital economy: Theoretical and legal
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33 enforcement issues in terms of regional aspect. E3S Web Conf 2020; 164: 09016. DOI:
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3 The biodegradation of natural fibre-reinforced composites after cold plasma treatments
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8 Abstract
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10 This study investigates the application of plasma treatment as a means to enhance
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biodegradation and modify the structural characteristics of fibrous composites. The
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15 methodological component of the study includes the selection of the research object; production
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17 of composites; low-temperature plasma treatment, and treatment of biodegradability and
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19 mechanical strength of samples. The strengthening of fibers with cellulose leads to a significant
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22 improvement in mechanical strength. Such an indicator as mechanical strength increased from

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24 18 to 21 MPa, or by 16.7%. Treatment of natural fibers with low-temperature plasma led to an
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26 increase in mechanical strength from 18 to 25 MPa, or by 33.3%. Treatment of reinforced fibers
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with low-temperature plasma led to an even greater increase in mechanical strength, namely
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31 from 18 to 29 MPa or by 50%. The electron microscopy of samples revealed some differences
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33 in cell wall microfibrils between plasma-treated and non-treated samples. The non-treated
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fibres were found to have chips and voids. Meantime, the plasma-treated fibres show structural
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38 changes in certain regions which resemble wood charring. Through a comprehensive analysis,
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40 this research underscores the substantial impact of plasma treatment on the degradation kinetics
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42 and morphological features of cellulose-based composites. The results reveal distinct alterations
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45 in the composition and behaviour of plasma-treated fibres, signifying a shift towards enhanced
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47 biodegradability. The natural fibres examined in this study contained 28-30% lignin, whereas
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49 the composites exhibited a lower lignin content of 21-23%. These findings corroborate the
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inference that plasma treatment induces significant changes in fibre structure, accelerating the
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54 biodegradation process by 7 days.
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56 Keywords: biodegradability, composites, degradation, discharge, fibres, plasma.
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1
2
3 Introduction
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6
The lightweight materials industry is a strategically important sector of the economy in many
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8 countries. Due to the growing population, the demand for clothing, footwear, and other textile
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10 products increases each year. At the same time, lightweight materials industry products must
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meet strict requirements related to hygiene, durability, and performance properties such as
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15 adhesion, water resistance, and so forth. Compliance and product quality largely depend on the
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17 methods and technologies used to manufacture and process natural and synthetic materials.1,2
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19 The textile industry makes use of both natural and synthetic materials. Man-made fibres are
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22 used to create new non-woven and artificial materials or impart specific properties to those
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24 materials. Synthetic fibres are superior to some products and inferior to others; hence, the choice
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26 of synthetics may be justified. However, polymeric materials do not decompose easily, and
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represent a serious threat to the environment in countries with intense production. According
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31 to recent reports, nearly 30% of polymer waste is subjected to incineration, some 30% is
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33 recycled, and the remaining 30% is left undisposed.3-5
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Scholars are actively engaged in the advancement of novel synthetic polymers designed for
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38 degradation by bacteria and other microorganisms within the natural ecological milieu.6,7 These
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40 polymers can be useful in many industries, including packaging, the textile industry, medical
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42 equipment, the automotive industry, and so forth.8 Recent studies have also investigated the use
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45 of plasma for processing synthetic polymers to increase their biodegradation. Plasma treatment
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47 can change the surface structure of the polymer, thereby providing a more efficient
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49 decomposition of the synthetic material by biological processes.9-11
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52
The study of biodegradation of synthetic polymers exhibits certain gaps. Unexplored areas
53
54 encompass the pathways of biodegradation for various polymer types, factors influencing
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56 biodegradation, resultant products, and novel biodegradation methods.12 Some researchers posit
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that successful biodegradation of the synthetic component within a natural-synthetic blend
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1
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3 occurs when the natural polymer is chemically attached (grafted) to the synthetic polymer.
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6
Bacterial activity initiates the degradation of the natural polymer chain, which subsequently
7
8 extends into the synthetic segment.13-15
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10 The work16 uses epoxy as a matrix material, and polymer composites with reinforcement from
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untreated and alkali-treated Zanthoxylum acanthopodium bark fibres (5–25 wt.%). Hand lay-
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15 up was used in the development of the epoxy composites. The mechanical characteristics and
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17 water absorption rates of the produced epoxy composites were evaluated following ASTM
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19 standards. Epoxy composites containing 20 wt.% of alkali-treated Zanthoxylum
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21
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22 acanthopodium bark fibres had excellent mechanical qualities, including an ultimate tensile
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24 strength of 47.3 MPa, according to the test findings. However, there was a positive correlation
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26 between fibre loading and water absorption. The fibre bonding and void properties of the
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investigated composites were viewed with a scanning electron microscope.
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31 In the work,17 Vachellia farnesiana fibres were selected and extracted by the manual retting
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33 process. The obtained Vachellia farnesiana fibres were chemically treated with hydrochloric
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acid (HCl) and sodium hydroxide (NaOH) solutions. The chemically treated and
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38 untreated Vachellia farnesiana fibres were characterized for physical, chemical, tensile,
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40 morphological, and thermal properties. Test results showed that the cellulose content was
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42 47.8 ± 0.697 wt % for NaOH-treated Vachellia farnesiana fibres with reduced moisture and
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45 amorphous contents. HCl-treated Vachellia farnesiana fibre showed more cellulose content
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47 removal, which resulted in the degradation of its properties due to the acidic nature of HCl.
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49 Plasma treatment is recognized as a dry and clean process. The utilization of low-pressure cold
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plasma for the pre-treatment of natural fibres is becoming increasingly prevalent as a novel
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54 method for surface modification.18 This approach offers advantages compared to traditional
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56 chemical treatment, as it does not require water or chemicals, rendering it environmentally
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friendly and cost-effective. Plasma modification substantially reduces the number of chemical
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3 pollutants. It etches the fibre surface, enhancing the action of the binding agent for improved
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adhesion.19 It can also render the surface rough through material ablation, enhancing adhesion.
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8 Moreover, it introduces free radicals and can alter the chemical structure. Low-pressure cold
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10 plasma modifies the fibre surface without changing the material volume. Additionally, it
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eliminates the need for chemical solvents and reduces process time.20
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15 Existing studies lack a comprehensive examination of the biodegradability of plasma-modified
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17 fibres. This article investigates the influence of low-temperature plasma treatment on the
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19 biodegradation of cellulose and its composite. The results provide insights into assessing the
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22 biodegradability of other materials. The study underscores the potential of plasma treatment in
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24 enhancing the quality of natural and synthetic fibres. Low-temperature plasma treatment of
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26 cellulose-based materials is employed for this purpose.
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Most studies note that low-temperature plasma treatment is a progressive and rather effective
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31 method since it can change the chemical composition of the fibre surface and the physical
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33 structure of molecules while maintaining the bulk material properties. Utilizing low-
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temperature and low-pressure plasma treatment demands a lesser amount of gasoline when
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38 contrasted with alternative techniques, leading to a near-total mitigation of waste generation.
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40 However, there are limited data on the biodegradability of plasma-treated fibres. The empirical
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42 evidence that fibre materials can partially or completely decompose after plasma treatment and
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45 that it affects the rate of biodegradation can serve as justification for the use of plasma treatment
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47 with a wider range of natural and synthetic fibres.
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49 This study aims to measure the biodegradability of plasma-treated wood fibre-reinforced
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polypropylene composites to determine whether plasma modification alters the rate of
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54 biodegradation. The secondary objectives of the study are (1) to examine the low molecular
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56 weight components of wood fibre-reinforced polypropylene composites during biodegradation;
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and (2) to explore the composition and properties of substances isolated from the plasma-treated
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3 samples. Finally, the study attempts to experimentally substantiate the mechanism behind the
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plasma-induced decomposition of cellulose fibres and theoretically determine the
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8 biodegradation time of materials under study.
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Methods and materials
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15 The flowchart of the experimental part is shown in Figure 1.
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43 Figure 1. The flow-chart of the experimental part
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48 The production of wood fibre-reinforced polypropylene composites
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50 This study addresses natural fibres of the finest coniferous wood species and cellulose-
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containing materials as experimental objects. These were unbleached softwood sulfate pulp and
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55 softwood sulfate lignin. The sample of natural wood fibres was analyzed using a scanning
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57 electron microscope. The SEM analysis method included the following steps: sample
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preparation, sample loading, vacuum chamber, and electron beam directed at the sample. The
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3 latter interacted with the sample, causing electron emission from the sample surface. Electron
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detection: a detector located in the SEM chamber identified electrons emitted by the sample.
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8 These signals were then processed and used to create an image of the sample’s surface
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10 topography and morphology.
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The results demonstrated that the average length of wood fibres was 190 µm (range, 100 to 400
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15 µm; standard deviation: 63 µm) and that the average width was 50 µm (range, 20 to 100 µm;
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17 standard deviation: 19 µm).
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19 Table 1 shows the approximate composition of fibre samples.21
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22 Table 1. The approximate composition of fibre samples.

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24 The composition, % Natural fibre Cellulose composite
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26 cellulose 46-48 18-20
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29 hexosans 10-12 12-14

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31 pentosanes 8-10 8-9
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33 lignin 28-30 21-23
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36 organic acids 4-5 3-4

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38 polypropylene - 35-37
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43 The production of polypropylene/cellulose composites requires using a solid-state shear
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45 pulverization. The sheared polymer method helped to reduce the particle size of cellulose
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47 materials. The cellulose fibres were mixed by ourselves with a polypropylene matrix in a plastic
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50 mixer (Haake Rheocord 9000, Germany) with a rotor velocity of 60 rpm at 185°C for 8 minutes.
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52 The resulting blend underwent compression molding at 185°C at a pressure of 10 MPa for 15
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54 min. Before being used, the samples rested at room temperature for 5 days.
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Figure 2 shows the scheme of the reactor.
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27 Figure 2. The reactor’s scheme
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The plasma reactor consists of a solenoid or radio-frequency induction coil (A) wound around
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34 a borosilicate glass tube (B). There will be a supply of gas (C) in the vacuum, and a vacuum
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36 pump valve (D) will keep the gas inside. The induction coil is to store energy within a magnetic
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field, which is numerically equal to that produced by the source to induce a current in the
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41 winding, generating a magnetic field of the solenoid. Inside the external glass tube, there is a
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43 partially open glass tube (E). It contains fibres that a stepper motor rotates (F) throughout the
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entire plasma treatment process.
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48 Low-pressure and low-power plasma does not cause excessive surface heating, and the glass
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50 tube is warm to the touch. Therefore, there is no excessive thermal exposure, thermal
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52 degradation of the fibres, or their incineration to be expected.
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55 The parameters of low-temperature plasma are as follows: I = 4.8–5.2 mA; U = 25-28 kW; gas
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57 medium: sulfur hexafluoride (SF6); additional medium – water (Н2О); exposure time = 10-30
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59 min; Р = 102 Pa.
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The plasma treatment procedure is described below
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8 1) The glass tube and the sample holder are cleaned with an air gun and disinfected with
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10 isopropyl alcohol to eliminate any contamination of the vacuum and plasma. All individuals
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involved in the experiment are required to wear nitrile gloves to prevent contamination.
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15 2) A 5-gram sample of investigated fibres is weighed and placed on the sample holder (internal
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17 glass tube (E) as shown in Figure 2). The tube is inserted into the reactor and attached to the
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19 axis of the stepper motor for further rotation of the sample.
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22 3) Once the reactor is closed, the air is evacuated by a vacuum pump. The pump must be
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24 connected to the reactor through a chamber equipped with a diaphragm valve. The latter opens
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26 slowly at the evacuation starts to prevent fibres from being absorbed in.
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4) As soon as the pressure falls below 10 Pa, the stepper motor starts rotating, causing the
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31 sample holder to rotate and the fibres to mix. A short-term increase in pressure occurs due to
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33 the release of accumulated gas.
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5) The selected process gas (partially or fully ionized; with no signs of being polymerized) is
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38 introduced into the chamber using a needle valve or mass flow controller. During pumping, the
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40 pressure increases to almost 102 Pa for 2 min, and then the gas supply is over. The procedure is
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42 repeated after 2-5 min of further pumping. This ensures a faster decrease in pressure as moisture
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45 transport occurs and guarantees enough gas in the tube.
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47 6) Finally, the system is pumped down to an atmospheric pressure of about 10-1 Pa. Because
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49 fluorocarbon bonds are sensitive to X-ray, the following sequence was followed: initial phase:
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250-350 eV; final phase: 0-1,150 eV; high-resolution oxygen spectrum, binding energy: 526 to
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54 540 eV.
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56 The equipment used here includes a gas chromatograph СhroZen UHPLC, a gas
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chromatograph-mass spectrometer GCMSQP2010 Plus, a thermal desorber TD-20, an ATR-
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3 8200HA attachment (Pike Tech), a scanning electron microscope (SEM) Sigma VP ZEISS, and
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a probe microscope MultiMode 8. The chemical analysis was compliant with GOST.22 Results
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8 were analyzed by gas chromatography using gas chromatograph Agilent 7820.
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Mechanical Testing
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15 Tensile testing (ISO 527) was carried out using a universal testing machine (UTM) with a
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17 gauge length of 6 cm and a speed of 5 mm/min. All the mechanical results were obtained with
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19 an average of 10 samples.
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24 Biodegradability testing
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26 The biodegradability test assessed the resulting cellulose composite’s ability to decompose
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under the influence of microorganisms within certain environmental conditions. The samples
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31 were buried in the soil for 30 days. This method is widely used for assessing the ability to
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33 decompose since it provides a simulated environment similar to natural decomposition.
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During testing, the samples were buried to a depth of 10-15 centimetres and covered with soil.
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38 The monitoring of soil humidity and temperature ensured that they remained within a certain
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40 range for microbial activity (25-75% and 15-25 °C, respectively). After 30 days, samples were
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42 excavated from the soil and analyzed for the presence and amount of material residues. The
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45 degradation degree was then identified by measuring mass loss.
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Statistical analysis was performed using a One-way Analysis of Variance, with significance
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54 reported at p≤0.05. All findings were presented as means ± standard deviations of at least five
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56 experiments.
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3 Results and discussion
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Plasma modification of the fibre surface is one of the most elaborated methods for improving
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8 the quality characteristics of materials. Plasma treatment can affect the surface properties of
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10 materials, such as the ability to bond dissimilar fibres. The adhesion of materials is often used
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to metalize, paint, or glue surfaces to obtain composites. This method also makes it possible to
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15 develop a range of properties less typical for unprocessed natural fabrics, such as hydrophilicity,
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17 dirt and dust repellency, antistatic properties, and so forth. In addition, plasma removes fat and
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19 other organics from fur and wool. It improves the absorption of dye pigments.23,24
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22 The essence of the plasma treatment method is to treat a material with a plasma medium
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24 (ionized gas) at low or atmospheric pressure. This causes surface reactions and modifications
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26 up to a change in the functional groups of molecules and a change in surface energy. Plasma is
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an ionized gas, in which free electrons and ions coexist. Plasma is produced by heating a gas to
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31 extremely high temperatures or by subjecting it to strong electromagnetic fields. Both of these
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33 processes may result in the release of electrons from atoms and molecules. The electrons have
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enough kinetic energy to remove additional electrons in case of a collision with other
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38 molecules.25 These collisions induce cascade ionization. A release of new ions and electrons
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40 occurs, balanced by the recombination of material molecules until plasma reaches equilibrium.
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42 The results obtained by Hamad26 show that plasma treatment of keratin-containing materials,
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45 such as wool and fur, at reduced pressure, opens the fibre cuticle, caused by the mutual
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47 repulsion of multiple charged jets. This allows effective removal of organic compounds from
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49 the merino wool fibres, without changing the fibre structure and physical properties.27 Zille28
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evaluated the effects of plasma surface treatment of flax, cotton, and animal-based fibres (wool,
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54 pile) on the tensile load resistance. Plasma treatment activates the surface of various synthetic
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56 materials, such as ultra-high modulus polyethylene, thereby improving their ability to absorb
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3 or completely repel moisture. This occurs due to the increase in surface tension of the fibres
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immersed in various gaseous media.9,11,13
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8 It is worth mentioning that some scientists29-32 agree that plasma treatment reduces the total
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10 energy consumption associated with the production of synthetic fibres by 25% as compared to
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other treatment methods. Research demonstrates that the modification of natural fibres requires
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15 14 to 50% less energy than the production of synthetic fibres. The real value in this broad range
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17 depends on a myriad of plant growth factors and plasma processing parameters.
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22 Table 2. Results of mechanical testing

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24 Sample Tensile strength, MPa
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26 Nature fiber 18
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29 Reinforced fiber 21
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31 Plasma treated nature fiber 25
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33 Plasma treated reinforced fiber 29
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38 Analyzing the data presented, we can come to the conclusion that strengthening fibers with
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40 cellulose leads to a significant improvement in mechanical strength. In particular, such an
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43 indicator as mechanical strength increased from 18 to 21 MPa, or by 16.7%. Treatment of
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45 natural fibers with low-temperature plasma led to an increase in mechanical strength from 18
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47 to 25 MPa, or by 33.3%. Treatment of reinforced fibers with low-temperature plasma led to an
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even greater increase in mechanical strength, namely from 18 to 29 MPa or by 50%.
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52 The electron microscopy of cellulose samples revealed some differences in cell wall
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54 microfibrils between plasma-treated and non-treated samples (Figure 3). The non-treated fibres
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were found to have chips and voids. Meantime, the plasma-treated fibres show structural
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59 changes in certain regions which resemble wood charring.
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29 Figure 3. Microscopic examinations of cellulose: (a, c) – no plasma treatment, (b, d) – plasma

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36 Interestingly, following plasma treatment, certain segments of the cellulose fibre exhibited a
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38 hollowed morphology. In contrast, the control sample displayed increased fragility due to the
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41 presence of voids and ruptures in the cell walls. This implies that plasma treatment influenced
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43 the microfibril structure of cellulose. Typically, reinforcing elements of microfibrils were
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45 diminished as a result of plasma treatment, enhancing flexibility and disrupting structural
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integrity.
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50 When investigating the composite of polypropylene fibres reinforced with cellulose (Figure
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52 4), a distinct behaviour was observed following plasma treatment. The fibres of the treated
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54 composite exhibited fewer visible defects and were predominantly embedded within the
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57 polypropylene matrix. Importantly, no slip lines or voids were evident on the fracture surface.
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3 Instead, the images displayed polymer adhesion to the fibres at multiple points, indicating a
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noteworthy transformation of material composition and interactions.
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Figure 4. The surface morphology of cellulose-reinforced polypropylene: (A, C) – no plasma

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38 treatment, (B, D) – plasma treatment.
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42 High interfacial shear strength and, consequently, a stronger interaction between fibres and
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matrices can significantly decelerate the biodegradation of composite materials. Plasma
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47 changes the structure of cellulose, with the latter completely dissolved in a solution of sodium
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49 hydroxide and simply in water. Low molecular weight components occur during
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51 depolymerization. Nearly 50 products were generated through the plasma-chemical
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54 decomposition of fibres; some (19%) are listed in Table 3. By comparing the quantitative
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56 composition of components in the table, significant differences between the degradation
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58 products of plasma-treated and untreated fibres can be identified. Specifically, several
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1
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3 compounds exhibit changes in molecular mass and percentage yield as a result of plasma
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treatment. For instance, compounds such as C6H10O5, 3-deoxyglucofuranose, and C6H6O3
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8 display altered molecular masses and percentage yields following plasma treatment, indicating
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10 the influence of plasma on the degradation process. These variations underscore that plasma
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treatment affects the molecular structure, which, in turn, may impact the biodegradation of
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15 composites.
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17 Table 3. Products resulting from the biodegradation of plasma-treated and non-treated fibres
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Compound name Plasma treatment No plasma treatment
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22 Percent Percent
23 Molar mass, g/mol Molar mass, g/mol
24 yield,% yield,%
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26 С6Н10О5 162 ±0.4 7.92 172 ±0.8 8.12
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29 3-dezoxyglukozenone 144 ±0.9 10.1 150 ±0.4 11.3

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31 Мetylmaltol 142 ±0.6 6.12 149 ±0.3 7.3
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С6H6O3 126 ±0.7 20.1 136 ±0.1 21.4
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36 1,6-angydryd-3,4-
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38 didezoxy-Р-0-pyranoz-3- 126 ±0.6 4.56 114±0.2 5.3
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40 an-2-one
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43 C6H6O 110 ±0.2 1.12 126 ±0.6 1.96
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45 C5H6O2 98 ±0.3 5.11 102 ±0.7 6.23
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47 2-acetyl-5-methylfuran 98 ±0.5 1.52 134 ±0.9 1.91
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50 C5H4O2 96 ±0.6 2.79 117 ±0.8 3.18
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52 γ-krotonolactone 84 ±0.9 1.12 101 ±0.2 1.78
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2-methylfuran 82 ±0.4 0.56 95±0.9 0.95
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57 C4H4O 68 ±0.2 1.52 84 ±0.4 1.87
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59 CH₃COOH 60 ±0.1 0.25 75 ±0.6 0.54
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3 CH₂O₂ 46 ±0.6 0.25 57 ±0.7 0.62
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8 The yield of levoglucosan (C6H10O5) was 7.92%, suggesting the achievement of stability after
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10 plasma treatment. A rather large amount (10.1%) of 3-dioxyglucosenone is released with a
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molecular weight of 144 g/mol during cellulose dehydration. The concentration of methyl
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15 maltol is lower (6.12%) but its molar mass is almost the same as that of 3-dioxyglucosenone.
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17 Two substances with the same molar mass of 126 g/mol, pyrogallol and anhydrosucrose,
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account for 4.56 and 20.1% of the yield, respectively. A furan aldehyde called furforol (C5H6O2)
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22 is released in the amount of 5.11%; part of furfural can be released with the participation of
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24 xylane. All molecules with a mass below 90 Da are marked as decay products of O2 and CO2.
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26 Plasma does not affect sulfate lignin. The plasma-treated natural fibres were 21% lignin,
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29 whereas the composites had a lignin content of 18%. The study results show that the
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31 dehydration and decomposition velocities of non-composites are almost 2 times lower as
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33 compared to composites. In natural conditions, lignin is strongly influenced by filamentous
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fungi, which have the power to cause the degradation of complex polymers by enzymes; in
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38 these conditions, materials decompose faster.
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40 Judging by data concerning the degradation products of plasma-treated fibres, the chemical
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processes associated with the biodegradation of natural cellulose are similar to those occurring
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45 in untreated samples. The structural changes to microfibrils, however, caused the
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47 biodegradation time of plasma-treated cellulose to accelerate.
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49 In the case of plasma-treated specimens, biodegradation commenced on the 12th day of the
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52 experiment, while for untreated specimens, it occurred a week later, specifically after 19 days.
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54 The buried plasma-treated material changed and became brittle and thinner than the control. At
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56 the end of the 30-day biodegradation test, prominent changes were detected in the samples.
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1
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3 The biodegradation of natural fibre-reinforced composites can occur through a variety of
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mechanisms; the choice depends on the type of natural filler used, its quality, and its chemical
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8 composition. The plasma-treated cellulose-reinforced polypropylene composites exhibit clear
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10 signs of decomposition. This finding coincides with previous research. It also suggests that
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plasma-treated fibre materials can decompose, partially or completely, and that plasma
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15 treatment can alter the rate of biodegradation.
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17 This study aligns with previous research emphasizing the significance of incorporating
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19 environmentally degradable components into composite materials.33 Earlier investigations
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22 examined fibre degradation alongside polylactic acid and clay silicates, revealing that the
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24 quantity and nature of natural constituents influence composite biodegradation.33
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26 Correspondingly, analogous burial-based studies.34-36 echo our findings, showcasing the
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accelerated degradation of triple compositions compared to double ones due to increased
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31 biodegradable content. Moreover, experts in plasma treatment advocate its efficacy in
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33 preserving textile properties and enhancing mechanical attributes of biodegradable composites,
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considering it more sustainable than chemical methods.37-41

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38 The choice between plasma and chemical treatment hinges on material requisites.39-41 Plasma
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40 treatment surpasses chemical counterparts in efficacy, transforming material surfaces,
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42 enhancing adhesion, and durability.42-44 This approach is particularly useful for biodegrading
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45 recalcitrant materials by promoting microbial interaction.45-47 Similarly, studies focusing on
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47 fibre-modified bioplastics suggest enhanced fibre-matrix adhesion.39,40 Cold plasma emerges
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49 as an efficient, eco-friendly alternative,38-41 fostering sustainable composite markets.
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This holistic exploration of plasma-treated materials showcases their potential in renewable and
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54 biodegradable materials research.45,48,49 Industrial use of plasma-modified materials
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56 necessitates eco-conscious biodegradability. Consequently, leveraging natural fibres for
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polymer matrix composites aligns with environmental awareness and promotes renewable
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1
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3 resources.33,50,51 Such studies aid in curbing waste and toxic releases, ensuring safer
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decompositions and material cycles. This research contributes to reducing environmental
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8 impact while bolstering sustainable material applications.
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Conclusions
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15 Through the utilization of scanning electron microscopy (SEM), the study demonstrated that
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17 plasma treatment has a substantial impact on both the process of biodegradation and the
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19 structure of the material. Scanning electron microscopy (SEM) enabled a thorough
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22 investigation of the procedural stages, with a specific emphasis on the interaction between
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24 electrons and the specimen. The methodological aspect of the study encompassed the selection
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26 of the research subject, fabrication of composites, application of low-temperature plasma
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treatment, and evaluation of the biodegradability and mechanical strength of the samples. The
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31 incorporation of cellulose fibers results in a substantial enhancement of mechanical strength.
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33 Specifically, the mechanical strength indication rose from 18 to 21 MPa, representing a 16.7%
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increase. Application of low-temperature plasma to natural fibers resulted in a 33.3%

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38 enhancement in mechanical strength, increasing it from 18 to 25 MPa. Reinforced fibers
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40 subjected to low-temperature plasma treatment exhibited a significant enhancement in
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42 mechanical strength, namely from 18 to 29 MPa, or a 50% increase. The electron microscopy
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45 analysis of the samples unveiled significant disparities in cell wall microfibrils between the
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47 plasma-treated and non-treated samples. Chips and cavities were seen in the untreated fibers.
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49 Meanwhile, the fibres that have undergone plasma treatment exhibit structural alterations in
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specific areas that bear resemblance to the charring of wood. The cellulose cell walls of treated
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54 and untreated samples showed differences in the microfibrils, including changes in structure
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56 after plasma treatment. Furthermore, there were also observed alterations in composites
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including polypropylene fiber and cellulose. The fibres that underwent plasma treatment
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1
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3 showed improved integration, as evidenced by the lack of slip lines on the fracture surface.
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The table displaying the quantitative measurement of biodegradation products indicates notable
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8 variations in composition between the treated and untreated fibers. These modifications
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10 demonstrate the impact of plasma on chemical reactions and biodegradation. Plasma treatment
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can speed up the process of biodegradation and alter the properties of materials. This has the
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15 potential to create composites that are more long-lasting and resistant, which is important for
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17 the production of environmentally sustainable materials and the efficient use of waste.
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22 References
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24 1. Ameer MH, Shaker K, Ashraf M, et al. Interdependence of moisture, mechanical properties,
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26 and hydrophobic treatment of jute fibre-reinforced composite materials. J Text Inst
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2017; 108(10): 1768-1776, DOI: 10.1080/00405000.2017.1285201
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31 2. Nawab Y, Kashif M, Asghar MA et al. Development & characterization of green composites
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33 using nNovel 3D woven preforms. Appl Compos Mater 2018; 25: 747–759. DOI:
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10.1007/s10443-018-9720-2
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38 3. Cordeiro RC. Plasma Treatment of Natural Fibres to Improve Fibre-matrix Compatibility.
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40 UFRJ/COPPE, 2016.
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42 4. Ershov IP, Sergeeva EA, Zenitova LA and Abdullin ISh. Modification of synthetic fibres and
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45 threads. Overview. Bull Kazan Technol Univer 2012; 15(18): 136–143.
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47 5. Islam MD, Mohammad Ziaul Hyder MK, Masudur Rhaman M, et al. Application of lignin-
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49 based biomaterials in textile wastewater. In: Muthu SS and Khadir A (eds) Textile Wastewater
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8 32. Nguyen Thi H, Vu Thi Hong K, Ngo Ha T, et al. Application of plasma activation in flame-
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47 38. Vinod A, Vijay R, Singaravelu DL, et al. Characterization of untreated and alkali treated
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54 39. Lahouioui M, Ben Arfi R, Fois M, et al. Investigation of fibre surface treatment effect on
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56 thermal, mechanical and acoustical properties of date palm fibre-reinforced cementitious
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47 10.1016/j.coco.2019.10.003
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49 46. Krishnan T, Jayabal S, Krishna VN. Tensile, flexural, impact, and hardness properties of
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morphological, and spectroscopy studies on Abutilon indicum fibrereinforced composites. J
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8 Nat Fibres 2020; 17: 1775-1784. DOI: 10.1080/15440478.2019.1598917.
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10 48. Premnath AA. Impact of surface treatment on the mechanical properties of sisal and jute
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reinforced with epoxy resin natural fibre hybrid composites. J Nat Fibres 2019; 16: 718–728.
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17 49. Saba N, Alothman OY, Almutairi Z, et al. Magnesium hydroxide reinforced kenaf
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19 fibres/epoxy hybrid composites: mechanical and thermomechanical properties. Constr Build
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24 50. Artamonov V, Vorona-Slivinskaya L, Medvedeva A. The algorithm of sustainable
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26 development of organizations: A social aspect. Procedia Eng 2016; 165: 1192–1196. DOI:
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33 enforcement issues in terms of regional aspect. E3S Web Conf 2020; 164: 09016. DOI:
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3 Reviewer: 1
4
5 Comments to the Author
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7 The manuscript is not recommended to publish in the Journal of Industrial Textiles. This manuscript
8 should be reorganized logically and thoroughly and is not enough to meet a research article now.
9
10
1) English should be modified.
11
2) Introduction section is too long and should be reorganized briefly, several sentences would be
12
13
enough rather than paragraphs in somewhere.
14 Answer. We significantly shortened the Introduction section.
15 3) Too much detailed description in the Methods and materials section and other sections, it should be
16 reorganized. For example, you do not need to introduce SEM analysis and tell readers how it works (the
17 first paragraph in the Results and discussion section).
18 Answer. We reorganized the Methods and materials section, included the flow-chart of investigation and
19 removed the first paragraph of the Results and Discussion section to the Methods and Materials section.
20
21 1. Selection of the research object
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22 (natural softwood fibers, cellulose).

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24
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2. Production of composites
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(grinding, mixing, molding, curing).
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32 3. Low-temperature plasma
33 treatment.
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38 4. Treatment of biodegradability of
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39 samples.
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41 4) Figures of biodegradation results (contents of Table 2) should be added in the Results and discussion
42 section.
43 Answer. Unfortunately, the content of Table 2 (now Table 3) is too big for several figures and should be
44 placed in the Table.
45 5) Data (results and discussion) is not enough to support conclusions.
46 Answer. We significantly enhanced the Results and Discussion Section.
47
48
additional suggestions:
49
50
51
This research cannot be considered original research and needs reorganization and rewriting‫ﺯ‬More deep
52 consideration is necessary for the research.
53
54 1. Some sentences like these should be written in more clear and appropriate manner, “An extensive
55 group of materials called ‘natural fibers’ are fibers that occur in nature in finished form. No humans are
56 involved in their production” (on page 3), as humans are always involved in harvesting crops and other
57 processing operations. Another example is “Many synthetic fibers are air-tight and hydrophobic” on page
58 6. Such sentences should be rewritten throughout whole paper.
59 2. The main focus of this paper is natural fiber composites (especially cellulosic), literature should me
60 more focused on natural fibers only rather than leather, wool etc. for example a sentence “Along with all
the advantages of natural fibers, there are some difficulties associated with the processing and preparation
1
2 of the materials for the production of end products. For example, “it is still challenging to remove organic
3 compounds from the surface when desizing leather and fur, dyeing wool, coping with significant
4 shrinkage of cotton fabrics and linen wrinkling, and so forth” on page 5 and “In addition, plasma removes
5 fat and other organics from fur and wool.” On page 8 and “plasma treatment of keratin-containing
6 materials, such as wool and fur, at reduced pressure opens the fiber cuticle” on page 9.
7 Answer. We significantly corrected the Introduction section.
8
9 3. More relevant literature needs to be cited, for example “10.1007/978-3-030-11155-7_108-1,
10
10.1007/978-3-031-20597-2_1, 10.1080/00405000.2017.1285201, 10.1007/s10443-018-9720-2,
11
10.1177/1528083716654468.
12
13
Answer. We added some references in the Introduction section.
14 [1] Shaker K, Nawab Y, Jabbar M. Bio-composites: Eco-friendly Substitute of Glass Fiber
15 Composites. In: Kharissova, O., Martínez, L., Kharisov, B. (eds) Handbook of Nanomaterials and
16 Nanocomposites for Energy and Environmental Applications. Springer, Cham. 2020. DOI: 10.1007/978-
17 3-030-11155-7_108-1
18 [2] Ameer MH, Shaker K, Ashraf M, Karahan M, Nawab Y, Ahmad S, Ali Nasir M. Interdependence
19 of moisture, mechanical properties, and hydrophobic treatment of jute fibre-reinforced composite materials.
20 The Journal of The Textile Institute, 2017, 108 (10): 1768-1776, DOI: 10.1080/00405000.2017.1285201
21 [3] Nawab Y, Kashif M, Asghar MA et al. Development & Characterization of Green Composites
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22 Using Novel 3D Woven Preforms. Appl Compos Mater 2018, 25, 747–759. DOI: 10.1007/s10443-018-
23 9720-2
24
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4. The sentence “structural changes to microfibrils however, caused the biodegradation time of plasma-
26
treated cellulose to accelerate” on page 16, suggests that mechanical properties of the composites may
27
28
have enhanced or reduced due to plasma treatment. Please also discuss this according to the findings.
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29 SEM images can be used to discuss composite interface, or if available, mechanical tests can be added
30 and discussed to support the claims.
31 Answer. We added this information.
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32 Mechanical Testing
33 Tensile testing (ISO 527) was carried out using a universal testing machine (UTM) with gauge length of 6
34 cm and speed of 5 mm/min. All the mechanical results were obtained with an average of 10 samples.
35 ***
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37 [Table 2 here]
38 Analyzing the data presented, we can come to the conclusion that strengthening fibers with cellulose leads
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39 to a significant improvement in mechanical strength. In particular, such an indicator as mechanical strength

40 increased from 18 to 21 MPa, or by 16.7%. Treatment of natural fibers with low-temperature plasma led to
41 an increase in mechanical strength from 18 to 25 MPa, or by 33.3%. Treatment of reinforced fibers with
42 low-temperature plasma led to an even greater increase in mechanical strength, namely from 18 to 29 MPa
43 or by 50%.
44 5. After a thorough review, I have noted certain aspects that necessitate further refinement. Specifically,
45
there is a requirement to standardize units of measurement throughout the manuscript.
46
Answer. We standardized units of measurement throughout the manuscript.
47
48
49 Reviewer: 2
50
52
53 The scientific work presented in the manuscript entitle " The biodegradation of natural fibre-reinforced
54 composites after cold plasma treatments" is investigating results concerning the biodegradation of natural
55 fibre-reinforced composites after cold plasma treatments. However, although the effect of cold plasma on
56 natural fibre-reinforced is studied, but this manuscript does not meet the main criteria of the standard
57 article, which confirms the structure and shape of materials. This article is not a complete article and has
58 many shortcomings. In my opinion, this manuscript is not acceptable in this form.
59
60 1. The abstract should be rewritten by summarizing the problem, the method, the results, and the
conclusions.
1
2 Answer. We corrected the Abstract section.
3 This study investigates the application of plasma treatment as a means to enhance biodegradation and
4 modify the structural characteristics of fibrous composites. The rationale for selecting plasma treatment lies
5 in its significant capacity to influence biodegradation processes. Current challenges in the realm of
6 biodegradable materials underscore the need for innovative solutions. The methodological component of
7 the study includes the selection of the research object (natural softwood fibers, cellulose); production of
8 composites (grinding, mixing, molding, curing); low-temperature plasma treatment, and treatment of
9 biodegradability and mechanical strength of samples. The strengthening fibers with cellulose leads to a
10
significant improvement in mechanical strength. In particular, such an indicator as mechanical strength
11
increased from 18 to 21 MPa, or by 16.7%. Treatment of natural fibers with low-temperature plasma led to
12
13
an increase in mechanical strength from 18 to 25 MPa, or by 33.3%. Treatment of reinforced fibers with
15 or by 50%. The electron microscopy of samples revealed some differences in cell wall microfibrils between
16 plasma-treated and non-treated samples. The non-treated fibres were found to have chips and voids.
17 Meantime, the plasma-treated fibres show structural changes in certain regions which resemble wood
18 charring. Through a comprehensive analysis, this research underscores the substantial impact of plasma
19 treatment on the degradation kinetics and morphological features of cellulose-based composites. The results
20 reveal distinct alterations in the composition and behaviour of plasma-treated fibres, signifying a shift
21 towards enhanced biodegradability. The natural fibres examined in this study contained 28-30% lignin,
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22 whereas the composites exhibited a lower lignin content of 21-23%. These findings corroborate the
23 inference that plasma treatment induces significant changes in fibre structure, accelerating the
24 biodegradation process by 7 days. As a recommendation, future investigations could focus on optimizing
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25 plasma treatment parameters to finely tune the biodegradability of composite materials.

26
27 2. This manuscript is not a clear work, whether it is a review or research paper.
28
ee
Answer. We significantly corrected all sections of the article in order to meet the requirements of this
29
journal.
30
3. Why the particular In and fibre-reinforced composites was chosen? Why it is superior as compared to
31
the other composites?
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32
33 Answer. There is information in the article about it.
34 The production of biodegradable polymers currently moves toward the use of polymer blends with
35 desired properties. These blends usually consist of biodegradable naturally occurring polymers such as
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36 starch, cellulose, and chitin or they may include synthetic ones; the mixture is then added to a synthetic
37 polymer binder. In this study, the selected natural polymer was cellulose (99%, LVJIAN, China). Another
38 ingredient was the polypropylene (100%, Wanhongruiquan, China) homopolymer according to State
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39 Standard (GOST) No. 26996-86 [33].

40 5. XRD, XPS and BET analysis must be undertaken for the composition analysis.
41 Answer. We used a serious set of modern equipment and techniques in our investigations.
42 The equipment used here includes a gas chromatograph СhroZen UHPLC, a gas chromatograph-mass
43 spectrometer GCMSQP2010 Plus, a thermal desorber TD-20, an ATR-8200HA attachment (Pike Tech), a
44 scanning electron microscope (SEM) Sigma VP ZEISS, and a probe microscope MultiMode 8. The
45 chemical analysis was compliant with GOST [33]. Results were analyzed by gas chromatography using gas
46 chromatograph Agilent 7820.
47
48 6. Summarize the major findings and future perspectives of the present work in conclusion section.
49
Answer. We corrected the Conclusion section.
50
Conclusions
51
52
The study, based on analysis using scanning electron microscopy (SEM), revealed that plasma treatment
53 exerts a significant influence on both the biodegradation process and the material's structure. SEM analysis
54 facilitated a detailed examination of the methodological steps, focusing on the interaction between electrons
55 and the specimen. The methodological component of the study included the selection of the research object,
56 production of composites, low-temperature plasma treatment, and treatment of biodegradability and
57 mechanical strength of samples. The strengthening fibers with cellulose lead to a significant improvement
58 in mechanical strength. In particular, such an indicator as mechanical strength increased from 18 to 21 MPa,
59 or by 16.7%. Treatment of natural fibers with low-temperature plasma led to an increase in mechanical
60 strength from 18 to 25 MPa, or by 33.3%. Treatment of reinforced fibers with low-temperature plasma led
to an even greater increase in mechanical strength, namely from 18 to 29 MPa or by 50%. The electron
1
2 microscopy of samples revealed some differences in cell wall microfibrils between plasma-treated and non-
3 treated samples. The non-treated fibres were found to have chips and voids. Meantime, the plasma-treated
4 fibres show structural changes in certain regions which resemble wood charring. Comparison of
5 microfibrils in the cellulose cell walls of treated and untreated samples exhibited distinctions, including
6 structural alterations following plasma treatment. Moreover, composites comprising polypropylene fibre
7 and cellulose also showcased modifications. Plasma-treated fibres exhibited enhanced integration, with the
8 absence of slip lines on the fracture surface. The quantitative analysis of biodegradation products presented
9 in the table revealed significant compositional differences between treated and untreated fibres. These
10
alterations indicate the influence of plasma on chemical processes and biodegradation. Plasma treatment
11
can accelerate biodegradation and modify materials, holding potential for the development of more durable
12
13
and resilient composites, which holds significance for ecologically sustainable materials and waste
14 utilization.
15
16 additional suggestions:
17 1#please verify page 2 line 5: Are man-made fibres just used to create nonwoven fabrics?
18 Answer. We deleted this phrase.
19 2#page 6 line 36: please insert a reference about this sentence.
20 Answer. We deleted this sentence.
21 3#about the “Fiber modification methods” section it is important to insert references about the three
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22 categories mentioned.
23 Answer. We deleted this section.
24 4#page 12 line 33: what means RF?
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25 Answer. We described this abbreviation.

26 radio-frequency induction coil
27 5#about the “Biodegradability testing” section it was interesting insert a picture to illustrated the process.
28
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Answer. Unfortunately we could not make photos underground.

29
6#In the Figure 4 it was interesting to use the same magnitude to compare the pictures, for example in C
30
and D letters.
31
Answer. The different dimensions in Figures C and D were specifically chosen to evaluate the effect of
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33 plasma treatment at different levels of the structure.
34
35 Reviewer: 3
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36
38
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39
40 The manuscript "The biodegradation of natural fibre-reinforced composites after cold plasma treatments"
41 is incomplete in several aspects. So, not recommend for publication. Please see the attached file for the
42 reasons to reject the paper.
43
44 additional suggestions:
45
46 - The manuscript is too long. It should be shortened an expressed clearly.
47 Answer. We significantly shortened the article.
48 - The "Introduction" part includes a lot of contents in the “Literature review”. It should be revised in more
49
understandable and celar manner..
50
Answer. We significantly revised and shortened the Introduction section.
51
52
- The effect of plasma treatment on the mechanical properties of composite material should be included in
53 the manuscript.
58 ***
60 [Table 2 here]
1
7 or by 50%.
8
9 - Introduction and literature review part lengthy may be rewrite as required.
10
Answer. We significantly shortened the Introduction and Literature Review sections.
11
12
13
14 Reviewer: 4
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17 I don't recommend the paper titled “The biodegradation of natural fibre reinforced composites after cold
18 plasma treatments” for publication in JIT due to lack of scientific contribution. Authors should consider
19 the following main questions and comments:
20
21 Main question
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22 1. The article's general and unclear nature makes it challenging for the reader to comprehend.
23 Answer. We significantly rewrite this paper.
24 2. The work lacks novelty or is not explained clearly to the audience.
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25 Answer. We corrected the abstract and concludes of the article.

26 3. Many topics that are not necessary to write in a scientific article are given in “Literature review”.
27 Answer. We significantly shortened the Literature Review section.
28
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4. The English language of the manuscript needs to be considered and improved.

29
5. This work does not contain any indications of statistical analysis. How do you make a scientific
30
conclusion by relying on the results obtained from just one sample?
31
Answer. There is a statistical analysis of our investigation. All findings were presented as means ± standard
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33 deviations of at least five experiments.
35 Statistical analysis was performed using a One-way Analysis of Variance, with significance reported at
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36 p≤0.05. All findings were presented as means ± standard deviations of at least five experiments.
37
38 6. The conclusion, like the whole text, does not reflect the result and the novelty of the work.
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39 Quantitative values are not analysed in the discussion. The results of biodegradability testing and
40 comparison with the results of previous works are rare in “Results and discussion”.
41 Answer. We corrected the Conclusion section.
42 Conclusions
43 The study, based on analysis using scanning electron microscopy (SEM), revealed that plasma treatment
44 exerts a significant influence on both the biodegradation process and the material's structure. SEM analysis
45 facilitated a detailed examination of the methodological steps, focusing on the interaction between electrons
46 and the specimen. The methodological component of the study included the selection of the research object,
47 production of composites, low-temperature plasma treatment, and treatment of biodegradability and
48 mechanical strength of samples. The strengthening fibers with cellulose lead to a significant improvement
49
in mechanical strength. In particular, such an indicator as mechanical strength increased from 18 to 21 MPa,
50
or by 16.7%. Treatment of natural fibers with low-temperature plasma led to an increase in mechanical
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strength from 18 to 25 MPa, or by 33.3%. Treatment of reinforced fibers with low-temperature plasma led
53 to an even greater increase in mechanical strength, namely from 18 to 29 MPa or by 50%. The electron
54 microscopy of samples revealed some differences in cell wall microfibrils between plasma-treated and non-
55 treated samples. The non-treated fibres were found to have chips and voids. Meantime, the plasma-treated
56 fibres show structural changes in certain regions which resemble wood charring. Comparison of
57 microfibrils in the cellulose cell walls of treated and untreated samples exhibited distinctions, including
58 structural alterations following plasma treatment. Moreover, composites comprising polypropylene fibre
59 and cellulose also showcased modifications. Plasma-treated fibres exhibited enhanced integration, with the
60 absence of slip lines on the fracture surface. The quantitative analysis of biodegradation products presented
in the table revealed significant compositional differences between treated and untreated fibres. These
1
2 alterations indicate the influence of plasma on chemical processes and biodegradation. Plasma treatment
3 can accelerate biodegradation and modify materials, holding potential for the development of more durable
4 and resilient composites, which holds significance for ecologically sustainable materials and waste
5 utilization.
6
7
8 7. The effect of plasma treatment on the mechanical properties of the composite is important and should
9 be considered.
10
Answer. We added this information.
11
Mechanical Testing
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Tensile testing (ISO 527) was carried out using a universal testing machine (UTM) with a gauge length of
14 6 cm and a speed of 5 mm/min. All the mechanical results were obtained with an average of 10 samples.
15 ***
17 [Table 2 here]
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23 or by 50%.
24
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25
26 Additional suggestions
27
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1. Improve Table 1.
29
Answer. We improved the Table 1.
30
2. Make copyright permission for the pictures.
31
Answer. We deleted the Figure 1.
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33 3. Explanation more SEM analysis. It is recommended to add XRD, FTIR.
34 Answer. We added more explanation about SEM and other analysis.
35 The SEM analysis method included the following steps: sample preparation, sample loading, vacuum
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36 chamber, and electron beam directed at the sample. The latter interacted with the sample, causing electron
37 emission from the sample surface. Electron detection: a detector located in the SEM chamber identified
38 electrons emitted by the sample. These signals were then processed and used to create an image of the
iew
39 sample’s surface topography and morphology.

40 ***
41 The equipment used here includes a gas chromatograph СhroZen UHPLC, a gas chromatograph-mass
46
47 The manuscript entitled "The biodegradation of natural fibre-reinforced composites after cold plasma
48 treatments" submitted to Journal of Industrial Textiles reports the application of plasma treatment as a
49
means to enhance biodegradation and modify the structural characteristics of fibrous composites. This
50
work is very general and fails to explain and analyze the biodegradation process and mechanism of cold
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plasma. I do not agree to being accepted by the journal.
53 1. The title of the manuscript does not match the content of the article. The title of the article is “The
54 biodegradation of natural fibre-reinforced composites after cold plasma treatments”, but the low
55 temperature treatment method is not mentioned in the full text analysis.
56 Answer. There id description of low-temperature plasma in the article.
57 The plasma reactor consists of a solenoid or radio-frequency induction coil (A) wound around a borosilicate
58 glass tube (B). There will be a supply of gas (C) in the vacuum, and a vacuum pump valve (D) will keep
59 the gas inside. The induction coil is to store energy within a magnetic field, which is numerically equal to
60 that produced by the source to induce a current in the winding, generating a magnetic field of the solenoid.
1
2 Inside the external glass tube, there is a partially open glass tube (E). It contains fibers that a stepper motor
3 rotates (F) throughout the entire plasma treatment process.
4 Low-pressure and low-power plasma does not cause excessive surface heating, and the glass tube is warm
5 to the touch. Therefore, there is no excessive thermal exposure, thermal degradation of the fibers, or their
6 incineration to be expected.
7 The parameters of low-temperature plasma are as follows: I = 4.8–5.2 mA; U = 25-28 kW; gas medium:
8 sulfur hexafluoride (SF6); additional medium – water (Н2О); exposure time = 10-30 min; Р = 102 Pa.
9
10
The plasma treatment procedure is described below.
11
1) The glass tube and the sample holder are cleaned with an air gun and disinfected with isopropyl alcohol
12
13
to eliminate any contamination of the vacuum and plasma. All individuals involved in the experiment are
14 required to wear nitrile gloves to prevent contamination.
15 2) A 5-gram sample of investigated fibers is weighed and placed on the sample holder (internal glass tube
16 (E) as shown in Figure 2). The tube is inserted into the reactor and attached to the axis of the stepper motor
17 for further rotation of the sample.
18 3) Once the reactor is closed, the air is evacuated by a vacuum pump. The pump must be connected to the
19 reactor through a chamber equipped with a diaphragm valve. The latter opens slowly at the evacuation
20 starts to prevent fibers from being absorbed in.
21 4) As soon as the pressure falls below 10 Pa, the stepper motor starts rotating, causing the sample holder to
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22 rotate and the fibers to mix. A short-term increase in pressure occurs due to the release of accumulated gas.
23 5) The selected process gas (partially or fully ionized; with no signs of being polymerized) is introduced
24 into the chamber using a needle valve or mass flow controller. During pumping, the pressure increases to
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25 almost 102 Pa for 2 min, and then the gas supply is over. The procedure is repeated after 2-5 min of further
26 pumping. This ensures a faster decrease in pressure as moisture transport occurs and guarantees enough gas
27 in the tube.
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6) Finally, the system is pumped down to an atmospheric pressure of about 10-1 Pa. Because fluorocarbon
29
bonds are sensitive to X-ray, the following sequence was followed: initial phase: 250-350 eV; final phase:
30
0-1,150 eV; high-resolution oxygen spectrum, binding energy: 526 to 540 eV.
31
The equipment used here includes a gas chromatograph СhroZen UHPLC, a gas chromatograph-mass
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37
38 2. Does the author license the image in Figure 1? If the use of these images is approved. Please add
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39 copyright license information.

40 Answer. We deleted Figure 1 from the article.
41 3. In the full text, there are many statements in which the authors get the current conclusion, but lack of
42 literature support. For example, on page 4 “The removal of lignin from the fiber increases the flexibility
43 of the material. This is due to the improved mobility of individual structures of flax fibers under the
44 action of hemicellulose.” On page 5 “Another advantage of natural fibers is the potential to have their
45 physical properties changed under the influence of various physical and chemical factors. Besides, natural
46 fibers are renewable and are considered the most affordable raw material. They are sold at lower prices
47 than synthetic fibers. Occasionally, they are recycled as waste from other industries.” On page 5 “Due to
48 their flexibility and wear resistance, lignocellulosic fibers are associated with lower maintenance costs as
49
compared to other materials, such as glass fibers.” And so on.
50
Answer. We corrected the Introduction section and Literature Review.
51
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4. On page 7, the author introduces the current fiber modification methods, but lacks the literature support
53 for each method.
54 Answer. We deleted this part.
55 5. On page 10, the author mentioned that the natural wood fiber samples were analyzed by SEM, but the
56 SEM images could not be found.
57 Answer. The SEM images are shown in Figures 3, 4.
58 6. On page 11, table 1 shows the composition of natural fiber samples. These are the manufacturer's data,
59 but how to obtain the composition of the sample is not mentioned.
60 Answer. These are the manufacturer`s data
1
2 7. On page 14, holes appear in areas 2 and 3 of Figure 3, and voids also appear in Figure 3a, but are not
3 marked.
4 Answer. We corrected the text in the article about it.
5 The electron microscopy of cellulose samples revealed some differences in cell wall microfibrils between
6 plasma-treated and non-treated samples (Figure 3). The non-treated fibers were found to have chips and
7 voids. Meantime, the plasma-treated fibers show structural changes in certain regions which resemble wood
8 charring.
9 [Figure 3 here]
10
Interestingly, following plasma treatment, certain segments of the cellulose fibre exhibited a hollowed
11
morphology. In contrast, the control sample displayed increased fragility due to the presence of voids and
12
13
ruptures in the cell walls. This implies that plasma treatment influenced the microfibril structure of
14 cellulose. Typically, reinforcing elements of microfibrils were diminished as a result of plasma treatment,
15 enhancing flexibility and disrupting structural integrity.
16 8. On page 14, Figure 3 is not a comparison picture of the same part before and after plasma treatment,
17 which cannot prove the effect of plasma treatment on fibers.
18 Answer. We corrected the text in the article about it.
19 The electron microscopy of cellulose samples revealed some differences in cell wall microfibrils between
20 plasma-treated and non-treated samples (Figure 3). The non-treated fibers were found to have chips and
21 voids. Meantime, the plasma-treated fibers show structural changes in certain regions which resemble wood
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22 charring.
23 [Figure 3 here]
24 Interestingly, following plasma treatment, certain segments of the cellulose fibre exhibited a hollowed
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25 morphology. In contrast, the control sample displayed increased fragility due to the presence of voids and
26 ruptures in the cell walls. This implies that plasma treatment influenced the microfibril structure of
27 cellulose. Typically, reinforcing elements of microfibrils were diminished as a result of plasma treatment,
28
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enhancing flexibility and disrupting structural integrity.

29
9. In Figure 4 C and D on page 14, due to the different magnification of the pictures, no obvious adhesion
30
of the polymer to the fiber can be seen in Figure D, so Figure D cannot be used as a basis to prove that the
31
polymer adheres to the fiber.
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33 Answer. We corrected the article about it.
34 When investigating the composite of polypropylene fibres reinforced with cellulose (Figure 4), a distinct
35 behaviour was observed following plasma treatment. The fibres of the treated composite exhibited fewer
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36 visible defects and were predominantly embedded within the polypropylene matrix. Importantly, no-slip
37 lines or voids were evident on the fracture surface. Instead, the images displayed polymer adhesion to the
38 fibres at multiple points, indicating a noteworthy transformation of material composition and interactions.
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39
40 10. On page 16, “The burned plasma treated material changed and became brittle and thinner than the
41 control.” is mentioned. In the full text, no comparison picture or analysis before and after the sample is
42 found.
47 ***
49
[Table 2 here]
50
Analyzing the data presented, we can come to the conclusion that strengthening fibers with cellulose leads
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52
to a significant improvement in mechanical strength. In particular, such an indicator as mechanical strength
56 or by 50%.
57 11. On page 14, the tests of gas chromatography-mass spectrometry and pyrolyzer were mentioned, but
58 only SEM analysis was used in the results and discussion. It is suggested to supplement XRD, FTIR and
59 other test analysis.
60 Answer. We deleted these phrases.
1
2 12. On page 14, tests such as gas chromatography-mass spectrometry and thermal desorption were
3 mentioned, but only SEM analysis was used in the results and discussion. It is suggested to supplement
4 XRD, FTIR and other test analysis.
5 Answer. We deleted these phrases.
6 13. In the results and analysis of this paper, only some test data are briefly explained, and the processing
7 mechanism and other important aspects are not analyzed.
8 Answer. We added a mechanism in the article.
9 Plasma modification of the fiber surface is one of the most elaborated methods for improving the quality
10
characteristics of materials. Plasma treatment can affect the surface properties of materials, such as the
11
ability to bond dissimilar fibers. The adhesion of materials is often used to metalize, paint, or glue surfaces
12
13
to obtain composites. This method also makes it possible to develop a range of properties less typical for
14 unprocessed natural fabrics, such as hydrophilicity, dirt and dust repellency, antistatic properties, and so
15 forth. In addition, plasma removes fat and other organics from fur and wool. It improves the absorption of
16 dye pigments [21, 23].
17 The essence of the plasma treatment method is to treat a material with a plasma medium (ionized gas) at
18 low or atmospheric pressure. This causes surface reactions and modifications up to a change in the
19 functional groups of molecules and a change in surface energy. Plasma is an ionized gas, in which free
20 electrons and ions coexist. Plasma is produced by heating a gas to extremely high temperatures or by
21 subjecting it to strong electromagnetic fields. Both of these processes may result in the release of electrons
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22 from atoms and molecules. The electrons have enough kinetic energy to remove additional electrons in case
23 of a collision with other molecules [26]. These collisions induce cascade ionization. A release of new ions
24 and electrons occurs, balanced by the recombination of material molecules until plasma reaches
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25 equilibrium.
26 The results obtained by Hamad [14] show that plasma treatment of keratin-containing materials, such as
27 wool and fur, at reduced pressure opens the fiber cuticle, caused by the mutual repulsion of multiple charged
28
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jets. This allows the effective removal of organic compounds from the Merino wool fibers, without
29
changing the fiber structure and physical properties [27]. Zille [28] evaluated the effects of plasma surface
30
treatment of flax, cotton, and animal-based fibers (wool, pile) on the tensile load resistance. Plasma
31
treatment activates the surface of various synthetic materials, such as ultra-high modulus polyethylene,
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33 thereby improving their ability to absorb or completely repel moisture. This occurs due to the increase in
34 surface tension of the fibers immersed in various gaseous media [5, 7, 8].
35 It is worth mentioning that some scientists [29-32] agree that plasma treatment reduces the total energy
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36 consumption associated with the production of synthetic fibers by 25% as compared to other treatment
37 methods. Research demonstrates that the modification of natural fibers requires 14 to 50% less energy than
38 the production of synthetic fibers. The real value in this broad range depends on a myriad of plant growth
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39 factors and plasma processing parameters.

40 14. In the article, "fibre" or "fiber" is recommended to verify its correctness and unity.
41 Answer. We replaced in the text “fiber” to “fibre”.
42 Conclusion: 1. Some text or content supporting materials are insufficient, and it is recommended to
43 supplement. 2. There are too few illustrations to support the point of view. 3. It is suggested that all the
44 experimental results should be analyzed and processed, and the processing mechanism should be
45 analyzed. 4. It is suggested to correct the grammatical errors in the text. The author does not seem to have
46 solved all the problems raised by the previous reviewers. And there are many unclear points in this article.
47 Therefore, I do not agree with its publication
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Journal of Industrial Textiles

The biodegradation of natural fibre-reinforced composites

Journal: Journal of Industrial Textiles

Manuscript Type: Original Manuscript

This study investigates the application of plasma treatment as a means

to enhance biodegradation and modify the structural characteristics of

mechanical strength of samples. The strengthening of fibers with

16.7%. Treatment of natural fibers with low-temperature plasma led to

or by 50%. The electron microscopy of samples revealed some

certain regions which resemble wood charring. Through a comprehensive

22 improvement in mechanical strength. Such an indicator as mechanical strength increased from

22 Table 1. The approximate composition of fibre samples.

29 hexosans 10-12 12-14

36 organic acids 4-5 3-4

22 Table 2. Results of mechanical testing

29 Figure 3. Microscopic examinations of cellulose: (a, c) – no plasma treatment, (b, d) – plasma

Figure 4. The surface morphology of cellulose-reinforced polypropylene: (A, C) – no plasma

29 3-dezoxyglukozenone 144 ±0.9 10.1 150 ±0.4 11.3

considering it more sustainable than chemical methods.37-41

increase. Application of low-temperature plasma to natural fibers resulted in a 33.3%

22 9. Pirsa S, Mohammadi B. Conducting/biodegradable chitosan-polyaniline film; Antioxidant,

22 ahead of print 24 April 2023. DOI: 10.1007/s13399-023-04240-7

124580. DOI: 10.1016/j.matchemphys.2021.124580.

44. Valášek P, Müller M, Šleger V. Influence of plasma treatment on mechanical properties of

22 Mater 2019; 201: 138–148. DOI: 10.1016/j.conbuildmat.2018.12.182

22 improvement in mechanical strength. Such an indicator as mechanical strength increased from

22 Table 1. The approximate composition of fibre samples.

29 hexosans 10-12 12-14

36 organic acids 4-5 3-4

22 Table 2. Results of mechanical testing

29 Figure 3. Microscopic examinations of cellulose: (a, c) – no plasma treatment, (b, d) – plasma

Figure 4. The surface morphology of cellulose-reinforced polypropylene: (A, C) – no plasma

29 3-dezoxyglukozenone 144 ±0.9 10.1 150 ±0.4 11.3

considering it more sustainable than chemical methods.37-41

increase. Application of low-temperature plasma to natural fibers resulted in a 33.3%

22 9. Pirsa S, Mohammadi B. Conducting/biodegradable chitosan-polyaniline film; Antioxidant,

22 ahead of print 24 April 2023. DOI: 10.1007/s13399-023-04240-7

124580. DOI: 10.1016/j.matchemphys.2021.124580.

44. Valášek P, Müller M, Šleger V. Influence of plasma treatment on mechanical properties of

22 Mater 2019; 201: 138–148. DOI: 10.1016/j.conbuildmat.2018.12.182

22 (natural softwood fibers, cellulose).

39 to a significant improvement in mechanical strength. In particular, such an indicator as mechanical strength

25 plasma treatment parameters to finely tune the biodegradability of composite materials.

39 Standard (GOST) No. 26996-86 [33].

25 Answer. We described this abbreviation.

Answer. Unfortunately we could not make photos underground.

25 Answer. We corrected the abstract and concludes of the article.

4. The English language of the manuscript needs to be considered and improved.

39 sample’s surface topography and morphology.

36 chromatograph Agilent 7820.

39 copyright license information.

enhancing flexibility and disrupting structural integrity.

39 factors and plasma processing parameters.

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