Sage Journals: Discover world-class research

Abstract

This work goal is to develop a valuable biodegradable material for sustainable packaging. The utilization of agriculture wastes to produce biodegradable packaging films based on carboxymethyl cellulose (CMC) will reduce its price. CMC was prepared from sugar cane bagasse, and used to prepare composite films with mandarin and cantaloupe peels extracts of different ratios. The effects of these extracts on the mechanical and antimicrobial properties of the prepared films were evaluated. Thus, the films incorporated with 10% concentration of mandarin and cantaloupe peels extract exhibited excellent antimicrobial properties against gram positive, gram negative bacteria and pathogenic yeast than the other lower concentrated films. The physiochemical properties of each developed biodegradable films were characterized using Fourier Transform Infra-Red (FTIR) spectroscopy, X-Ray diffraction analysis (XRD), Scanning Electron Microscopy (SEM) and antimicrobial. The reflected work is a novel approach, and which is vital in the conversion of organic waste to value-added product development.

Keywords

Active packaging carboxymethyl cellulose antimicrobial activity

Introduction

Due to the plastic’s risk to each human being, communities, and the entire ecosystem, the plastic's size is extremely important.^1,2 Due to unchecked population growth and unsustainable use of nonrenewable resources, a cumulative waste volume was produced. There are now only a few techniques for partially eliminating these wastes, such as landfills and ocean overflows of a variety of materials, some of which can decay in a certain amount of time while other detritus cannot disintegrate for hundreds of years.^3,4 Governments have proposed rules, such as limits or bans on single-use plastic bags and straws, in response to growing environmental concerns about sustainability and end-of-life disposal issues. Therefore, it is vital to switch to sustainable, biodegradable, or compostable materials for food packaging instead of utilizing plastic packaging. Additionally, the ongoing COVID-19 epidemic has disrupted manufacturing and transportation systems globally, necessitating the production of substantially more food packaging material to meet the demand for food preservation.⁵ As an alternative, the bio bags were thought to be just slightly different from conventional plastic bags.⁶ It compared to ordinary plastic with all these related problems, but biodegradable plastic preserves outstanding characteristic features and is more dependable nowadays.³

A family of natural carbohydrate polymers known as cellulose can be found in an almost endless supply of raw materials, including plants, agricultural waste, marine species' shells, and microbes.^4,7–9 Depending on the origin of the plants, the plant cell wall of cellulose fibers comprises varying amounts of cellulose embedded as microfibrils in a matrix of hemicellulose, lignin, pectin, ash, and other extractives.^4,5

The current project's goal is to create cellulose-based food packaging films. It might be one of the finest options for filling the hole left by the worldwide restriction on ordinary plastic.

There is a huge need for food packaging materials right now across several industries. Food packaging materials have a significant role in the preservation of food across the whole distribution chain. During marketing, food must be protected from mechanical damage and contamination. Antibacterial properties in materials have recently been developed. The most promising method for active packaging systems is antimicrobial packaging.^4,8,10 Food preservation up until delivery to the buyer is an essential step. The key elements that the packaging materials affect during storage and distribution depend on their mechanical strength, microbiological activity, etc. Recyclability, material prices, disposable nature, and sustainability are further important considerations.¹¹ These biodegradable polymers are projected to take the place of conventional polymeric products in packaging applications in the next years.^4,8,12,13

Nowadays, there is a regent need for effective antioxidants to prevent deterioration caused by microbes, besides; there has been considerable interest in recycling inexpensive agricultural wastes as sources for new by-products applications in order to pose positive environmental impact. Peels remain as primary waste and a main by-product of food processing which give rise to a serious environmental pollution. Citrus and melons are important crops in Egypt used mainly in food industries. Mandarin and cantaloupe are two of the most consumed fruits. Citrus peel which represents almost half of the fruit mass, containing more functional compounds than the edible parts, being a rich source of bioactive constituents including pectin, hesperidin, naringin, rutin, carotenoids and high concentration of flavonoids and phenolic acids is discarded as wastes.^14,15 Citrus peel extract showed potent antibacterial activity against pathogens.^16,17 So it is reasonable to be used in the formulation of antimicrobial by-products, similarly, melon is reported to have valuable activities.¹⁸ This work was conducted to study the phytochemical content of mandarin and cantaloupe fruits peel and to assess their in vitro antimicrobial potential after in corporation with biodegradable carboxymethyl cellulose (CMC) based material. The physiochemical properties of the developed biodegradable films were characterized using Fourier Transform Infra-Red (FTIR) spectroscopy, XRD and SEM.

Materials and methods

All the methods in this study were carried out in accordance with relevant Institutional guidelines and regulations.

Quena Company for Paper Industry (Quena, Egypt) provided sugarcane bagasse (SS). Sigma-Aldrich (St. Louis, MO, USA) provided the paraffin oil. All materials and reagents were used without being purified further.

Cantaloupe and mandarin extractions

Fresh fruits (mandarin (M) (Citrus reticulata) and cantaloupe (C) (Cucumis melo)) were purchased from local market. Peels were separated, carefully washed under running tap water then by distilled water, cut into small pieces, dried in hot air flow oven at 40–50°C, grounded into fine powder and sieved. The two peels powder was separately extracted with 95% methanol. The extracts were filtered and evaporated using a rotary evaporator to obtain dry concentrates, which were kept at 4°C for further analysis.¹⁹

Phytochemical screening

Each crude fruit peels extract (M and C) was tested qualitatively for the phytochemical compounds, alkaloids, carotenoids, saponins, flavonoids and tannins.

Carboxymethyl cellulose

SC (150 g) was prehydrolyzed through treatment with HCl (1.5%; 1570.3 mL) for 2 h at 120°C in stainless steel autoclave of 2 L capacity and electrically heated. The prehydrolyzed SC was washed with water. After that, 100 g of prehydrolyzed SC was treated with NaOH (20 g of NaOH in 300 mL water) at 170 °C for 2 h, to produce pulp. The produced pulp was brown cotton like shape in contrast to the straw shape of SC raw material. To remove lignin, the pulp (80 g) was bleached with HClO₂ (3%; 2.4 g in 4750 mL water) in the presence of acetic acid (1.7 mL) for 2 h at 80°C. During the reaction process, the pH increased to 10–12. So, acetic acid was added to make the pH equal to 1–3 (acidic) to obtain pure α-cellulose. The obtained pure α-cellulose (2.5 g in 75 mL isopropanol) was treated with NaOH (40%; 3 g in 7.5 mL water) and monochloroacetic acid (3 g) for 3.5 h at 55 °C with stirring. The resulting CMC was mixed in 70% ethanol before being filtrated and dried.^4,20

Preparation of Carboxymethyl cellulose/cantaloupe and Carboxymethyl cellulose/mandarin edible films

1 g of CMC was dissolved in 20 mL H₂O to form a gel solution. The mandarin (M) and cantaloupe (C) concentrates were ultrasonicated in 5 mL H₂O separately with different ratios of M and C (i.e., 2.5, 5, and 10%) which denoted as M2.5%, M5% and M10% for mandarin concentrate ratios, as well as, C2.5%, C5% and C10% for cantaloupe concentrate ratios and poured separately onto a teflon plate and dried at 40°C to attain a film of constant weight.

Characterization

The prepared samples were characterized by FTIR spectroscopy which was recorded by Mattson-5000 (Unicam, Somerset, United Kingdom) employing the KBr disk method in the wavenumber range of 4000–1000 cm⁻¹.

The mercerization depth (M_D) was calculated according to the following Equation:

M_{D} = \frac{A_{1375}}{A_{1325}}

(1)

where A₁₃₇₅ and A₁₃₂₅ refer to the intensity of 1375 and 1325 cm⁻¹ peaks of the FTIR spectra.²⁰

Determination of the degree of substitution of Carboxymethyl cellulose

The degree of substitution (DS) value of CMC was estimated through our previous procedure.²⁰

The tensile properties of the prepared films were measured by Universal Testing Machine- LLOYD LR 10 k, England. The tensile strength (TS), Elongation at break (EB %), and Young’s Modulus (Y %) of the films, were determined according to ASTM D-638 at a crosshead speed of 5 mm/min. The samples were cut into blocks of 100 × 3 × 20 mm³ (longitudinal × radial × tangential). Five specimens were tested for each sample, and the average value was listed.

XRD analysis was recorded by Bruker D8 Advance X-ray diffractometer (Karlsruhe, Germany) using copper (Kα) radiation (1.5406 Å) at a 40 kV voltage and a 40 mA current.

Both of crystallinity index Cr.I. (%) and $∆$ Cr.I. (%) were determined using Equations (2) and (3).

Cr . I . (%) = (A_{C} / A_{t}) \times 100

(2)

∆ Cr . I . (%) = \frac{(CrI) moified sample - (CrI) pure sample}{(CrI) pure sample} \times 100

(3)

where A_C is the crystalline peak area and A_t is the total area (Tohamy et al., 2022a; b; e).

d (nm) = \frac{0.9 λ}{β Cos θ}

(4)

where λ is the wavelength, β and θ are full widths at half maxima and Bragg’s angle of the XRD peak, respectively.^7,20,21

Mechanical test

The tensile properties of the fabric specimens were measured by Universal Testing Machine- LLOYD LR 10 k, England. The tensile strength (TS), Elongation at break (EB %), and Young’s Modulus (Y %) of the films, were determined according to ASTM D-638 at a crosshead speed of 5 mm/min.

Reproducibility of the tests

To avoid sources of error inherent in a given measurement, every experiment was repeated 3 times.

Antimicrobial activity

The qualitative evaluations were done in nutrient broth according to Mustafa et al. 2016 and El-Anssary et al. 2021. All the methods were carried out in accordance with relevant Institutional guidelines and regulations. Inoculations of pathogenic microorganisms included the gram-positive bacteria Micrococcus leutus (ATCC 10240) and Staphylococcus aureus (ATCC 6538), the gram-negative bacteria Escherichia coli (ATCC25922) and Pseudomonas aeruginosa (ATCC27853) and the pathogenic yeast Candida albicans (ATCC 10231). These were made from fresh overnight broth cultures using nutrient broth medium that were incubated at 37°C. The size of the inoculum of the strain was designed and adjusted to approximately 0.5 McFarland standards (1.5 × 10⁸ CFU/ml) (McFarland 1907). 25 µL inoculum size of each microorganism strain was separately injected into each plate comprising 20 mL sterile nutrient agar medium (NA). In addition, to each 100 mL conical flask with 25 mL of sterile nutrient broth medium (NB), 25 µL of both bacterial and fungal suspensions were inoculated separately.

The samples were splitted into two main groups; the first group was applied on 0.9 cm well of previously inoculated agar plates which were prepared using 1.0 cm cork borer applying (Disc diffusion method) and allowed to cool and solidify. In this method, disks of 1 cm² of films (CMC, M₁, M₂, M₃ and C₁, C₂, C₃) were arranged on the surface of the seeded plates. After placing these plates in the refrigerator for an hour for complete diffusion of the samples, and then incubation at 35 ± 2°C for 24 h, the inhibition zones (ZI) diameters were measured in mm. Analysis was performed in three replicates and duplicates. The second part was applied throughout the shake flask method (diffusion in liquid medium), a cut of 1 cm² of films (CMC, M₁, M₂, M₃ and C₁, C₂, C₃) was immersed in 60 mL of NB in an Erlenmeyer flask. The flasks were shook at 150 r/min at 35 ± 2°C. Calculation of the (%) reduction of colony forming unit (CFU) of the tested strains after treatment with the films, with comparison to the cells of the microorganisms that survive in the control flask after the incubation period for bacteria and pathogenic yeast; the reduction growth rate R (%) for the samples which were treated in relation to the control (untreated) was measured and were also compared to the gentamicin as a reference.²² The entire experiment was performed in triplicate. The results obtained were expressed according to the following equation:²³

Relative [Reduction (%)] = (A - B / A) \times 100

Notice that: A is the number of microorganisms in the control flask containing pathogenic strains only without any treatment. B is the number of microorganisms in tested flasks after applying the treating sample.

Statistical analysis

Results were taken triplicate and expressed as a mean with standard deviation (mean ± SD). Analysis was conducted with Student’s t test with significance p value ≤.05.

Results and Discussion

Qualitative analysis of crude extracts

The preliminary phytochemical analysis of mandarin peels extract revealed the presence of alkaloids, carotenoids, saponins, flavonoids and tannins, which were previously detected.²⁴ The cantaloupe peels extract showed the presence of flavonoids which is in accordance with the phenolic and flavonoid compounds, including chlorogenic acid being previously identified.²⁵

Fourier Transform Infra-Red spectroscopy

The DS of CMC was 0.76. Figure 1 shows the FTIR spectra of the blank and different film samples. The characteristic bands of CMC at 3344, 2910, 1598, and 1417 cm⁻¹ correlated to the stretching -OH, CH₂ stretching, the anti-symmetric and symmetric stretching vibrations of COO⁻, respectively.^4,20 A broad band at 3349–3365 cm⁻¹ is attributed to O–H groups for mandarin, M1, M2, M3, cantaloupe, C1, C2, and C3. Spectrum peaks near 1577–1618 cm⁻¹ region corresponds to C=O. Peaks near 2915–2931 cm⁻¹ corresponds to the stretching vibrational frequencies of C–H bonds can be characterized as the presence of methoxy groups.²⁰ Absorption peaks at 781–844, 910–921, and 1402–1411 cm⁻¹ can show presence of gallic acid and peaks at 1025–1039, 1261–1324, 1402–1411, and 1589–1602 cm⁻¹ can show presence of tannic acid.²⁶

Figure 1.

FTIR spectra of blank CMC film, Cantaloupe and Mandarin extract.

H-bonded OH stretching vibration of CMC appeared at 3344 cm⁻¹ was shifted to lower frequency at 3309, 3030, 3034, 3330, 3311, and 3286 cm⁻¹ for M2.5%, M5%, M10%, C2.5%, C5% and C10%, respectively. The change of the absorbance value of OH stretching vibration may be due to higher intermolecular H-bonding.^8,20,21 The RAs of the O–H were 0.86, 0.74, 0.74, 0.73, 0.72, 0.78, and 0.82 for CMC blank, M2.5%, M5%, M10%, C2.5%, C5% and C10%, respectively. It is clear that the RAs of the O–H strongly decreased compared to that of CMC blank. This means that the cross-linking reaction takes place between the OH group of CMC blank and M.^4,8

SEM analysis

The surface morphology of the blank CMC film, C10%, and M10% are presented in Figure 2 and show the effect of the extracts addition on the morphology of the films. The pore size of the synthesized blank CMC film (515 nm) was increased after the addition of extracts (i.e. 4.32 µm for C10% and 2.20 µm for M10%). The extracts are inter-located between CMC which in turn increase pore size. The increasing of pore size helps in exchanging of O₂, CO₂ between packaged fruits and the outer environment to prevent their damage. As it seen the pore size of M3 is lower than C3 but still higher than blank CMC film.

Figure 2.

SEM analysis of blank CMC film, C10% and M10%.

Mechanical properties

The blank CMC film’s tensile strength properties were examined, and the findings are shown in Table 1 and Figure 3. According to the results, the addition of cantaloupe and mandarin extracts led to decrease in TS (∼– 60.27% at 2.5% cantaloupe loading, i.e. C2.5% and – 75.00% at 10% mandarin loading, i.e. M10%), which was followed by an increase at higher cantaloupe loading (i.e. increase in TS∼ 135.10 and 153.19% for C5% and C10%, respectively), while, an increase at lower mandarin loading (i.e. increase in TS∼ 116.75 and 101.59% for M2.5% and M5%, respectively) were observed. On the other hand, the addition of cantaloupe and mandarin more noticeably enhanced the YM% of the C2.5%, C5%, C10%, M2.5%, M5% and M10% films compared to blank CMC film, particularly for C10% and M2.5%, where the rise in YM% was 243.49 and 262.84%, respectively. This might result from the characteristics of stiffness increasing with rising cantaloupe concentration. While for mandarin, the high concentration decreases stiffness. The enhancement of the mechanical properties of the C10% and M2.5% films suggests high compatibility between the CMC matrix and the surface of cantaloupe and mandarin (for a specific concentration, i.e. M2.5%). Similarly, H–bonding between the OH groups on the extracts surface and the C=O bonds of the CMC matrix may enhance the films’ mechanical properties.

Table 1.

Mechanical properties of blank CMC film, C2.5%, C5%, C10%, M2.5%, M5% and M10%.

Sample	TS (MPa)	EB (%)	YM (MPa)
Blank CMC film	3.76	78.13	18.30
C2.5%	2.27	88.11	22.55
C5%	5.08	96.58	39.26
C10%	5.76	103.40	44.65
M2.5%	4.39	63.54	48.10
M5%	3.82	67.41	35.80
M10%	2.82	70.37	26.01

Figure 3.

Mechanical analysis for blank CMC film, C2.5%, C5%, C10%, M2.5%, M5% and M10%.

Concerning EB%, it was typically seen that EB% increased with the addition of cantaloupe; for C2.5%, C5% and C10%, the rise varied from 112.77 to 132.34%. Cantaloupe has been shown to be effective plasticizers for CMC films due to their ability to enhance film EB % which make it a good plastic bag for food products. In contrary, increasing mandarin to higher loadings led to a decrease in the EB % (EB∼ – 68.52, – 81.32 and – 86.27% for M2.5%, M5% and M10%, respectively). This may be due to the strong interaction between CMC matrix and mandarin which suppress the mobility of the CMC chains. The rigidity of M10% was increased and allowed less flexibility, which is good for the rigid packaging applications for fragile food products such as yogurt.⁴ The M extract contains epoxy and OH groups while C extract contains NH₂ groups which interact differently with the free OH of CMC. C reacts with CMC via =NH- group which is reversible (i.e. elastic) while M when reacts with CMC give irreversible -O- group (i.e. rigid).

XRD analysis

The XRD pattern of the blank CMC film, as shown in Figure 4, indicates reflections at 13, 19 and 21°θ. The broadening of 19 and 21°θ peaks indicates the amorphous structure of CMC.^4,20 The crystallinity indexes (Cr. I %) calculated for blank CMC film, C10% and M10% were 43.82, 54.71 and 45.42%, respectively. It is clear that Cr. l (%) of C10% and M10% increase compared with that blank CMC film. This may be due to the H–bonding between cantaloupe and/or mandarin with CMC matrix. This is proved also by the high TS and YM calculated in the mechanical section, as well as, the OH peaks shifting in the FTIR which proved the presence of H–bonds. As shown in Table 2, d (nm) of C10% is increased compared to M10%. This is also proved by the high EB (%) calculated for them in the mechanical section.

Figure 4.

XRD spectra of blank CMC film, C3, and M3.

Table 2.

The crystallinity of the blank CMC film, C3 and M3.

Sample	Crl (%)	$∆$ Crl (%)	d (nm)
Blank CMC film	43.82	–	16.58
C10%	54.71	24.85	0.28
M10%	45.42	3.65	0.27

Antimicrobial properties

In the disc diffusion method, the inhibition zone is related to the growth absence of the microorganism and the diffusion of antimicrobial factor in the medium. Table 3 and Figure 5 show that the blank CMC, C1, C2, C3, M1, M2 and M3 have excellent antimicrobial activity toward gram-positive bacteria (Micrococcus leutus), which was improved by adding C and M extracts. Furthermore, antimicrobial activity of the C1, C2 and C3 films showed 0, 19 and 21 mm while M1, M2 and M3 films showed clear inhibition zone diameters 15, 13, and 11 mm surrounding the films, compared to gentamicin which showed 25 mm inhibition zone diameter.

Table 3.

Inhibition zone diameter (millimeter) of the blank CMC film, C2.5%, C5%, C10%, M2.5%, M5% and M10%.

Test bacteria		Samples
		Treated sample
		Blank	C2.5%	C5%	C10%	M2.5%	M5%	M10%	Reference^**
		Blank	C2.5%	C5%	C10%	M2.5%	M5%	M10%	CN
1-	Escherichia coli	NiL*	NiL	NiL	NiL	NiL	NiL	NiL	15.0
2-	Pseudomonas aeruginosa	NiL	NiL	NiL	NiL	NiL	NiL	NiL	13.0
3-	Micrococcus leutus	NiL	NiL	19.0	21.0	15.0	13.0	11.0	25.0
4-	Staphyllococcus aureus	NiL	NiL	NiL	NiL	NiL	NiL	NiL	21.0
5-	Candida albicans	NiL	NiL	NiL	NiL	NiL	NiL	NiL	ــــــــــــ

Figure 5.

Antimicrobial activity of the blank CMC film, C2.5%, C5%, C10%, M2.5%, M5% and M10%.

CFU % of the tested strains after treatment with the films, with comparison to the cells of the microorganisms that survive in the control flask after the incubation period for bacteria and pathogenic yeast are given in Table 4, which shows inhibition efficacy for the films of both mandarin and cantaloupe against the tested strains increasing with higher concentration manner

Table 4.

(%) CFU reduction of tested strains after incubation applying the test films using shake flask method.

Tested strains	Films
Tested strains	C2.5%	C5%	C10%	M2.5%	M5%	M10%
Escherichia coli	56.43	51.99	95.43	87.83	51.02	69.72
Pseudomonas aeruginosa	80.15	80.99	77.42	46.24	75.86	80.85
Micrococcus leutus	78.88	98.96	99.66	98.94	95.74	92.11
Staphyllococcus aureus	64.77	65.71	82.32	78.11	41.95	90.75
Candida albicans	64.73	72.98	89.32	69.58	73.26	86.14

Citrus are widely popular all over the world. Common varieties of citrus include oranges, limes, lemons, grapefruits and mandarin. Their essential oil and extracts have shown inhibitory effects on the growth of some bacteria in the food industry, and those related to food spoilage. It was found that the mandarin essential oil to possess the broadest spectrum of actions, and played a direct role in its antibacterial mechanism.^27,28 The bacterial cells treated with the films incorporated with 10% concentration of mandarin are likely found to be severely damaged and the original integrity of the cell membrane which is a pivotal structural component of a bacteria cell, is completely disappeared leading to the leakage of nucleic acids, protein and other intracellular substances. This may be attributed to the tannin-rich methanol extract, which caused the depolarization of the cells exposed to it, resulting in abnormal metabolic activities, structural distortion and serious destruction of the cells.²⁹ This effect confirms that mandarin extract can penetrate the bacterial membrane and act on the cell membrane to kill it, thus establishing its potential as a representative natural antimicrobial agent for food preservation.^30,31 Cantaloupe is one of the most commonly consumed fruits worldwide because of its fine aroma and nutritional benefits, its peel can be used as a potential resource of various health-promoting compounds,³² especially pectin which is a structurally complex macromolecule of partially esterified α (1-4) linked d-galacturonic acid units. It is used alone or in combination with other biopolymers in food industry as a food additive, gelling agent, thickener, texturizer, emulsifier, stabilizing agent, and fat-replacer showing high binding capacity.³³ Pectin also exhibits antimicrobial activities that can contribute to more effective functional films for food packaging.^34,35 It has a bactericidal effect on the most widely distributed pathogenic and opportunistic microorganisms.^36,37

Conclusion

CMC film was blended with C and M by ultrasonication. FTIR spectra shows that the relative absorbance of the O–H decreased compared to the blank CMC which means the crosslinking between C or M with CMC. SEM analysis shows increased pore size by addition of extracts. X-ray diffraction show that the crystallinity indexes increased due to H–bonding which occurs as a result of crosslinking. From mechanical tests it was shown that C acts as a plasticizer for CMC film due to the increased EB % values which make it a good plastic bag for food products, while M increased the rigidity of CMC which make it good for packaging fragile food products. From these results we can say that the effect of M on CMC film is different than the effect of C.

Footnotes

Acknowledgments

The authors appreciate the National Research Center, Egypt, for supporting this work.

Author contributions

M.E.-S.: Conceptualization, Validation, Formal analysis, Data curation, Visualization, Supervision, and Project administration. H.-A.S.T.: Conceptualization, Methodology, Sofware, Validation, Formal analysis, Data curation, writing— original draft preparation, Visualization, and prepared figures. M.M.A.: Conceptualization, Methodology, Validation, Formal analysis, Data curation, writing—original draft preparation, and Supervision. M.E.-M.: Conceptualization, Methodology, Formal analysis, Data curation, and writing— original draft preparation. All authors have read and agreed to the published version of the manuscript.

Declaration of conflicting interests

The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.

Funding

The author(s) received no financial support for the research, authorship, and/or publication of this article.

ORCID iD

Mohamed El-Sakhawy

Data Availability Statement

will be made available on request from the corresponding author (elsakhawym@gmail.com).

References

Mateos-Cárdenas

O’Halloran

van Pelt

, et al. Rapid fragmentation of microplastics by the freshwater amphipod Gammarus duebeni (Lillj.). Sci Rep 2020; 10: 12799.

Gerritse

Leslie

de Tender

, et al. Fragmentation of plastic objects in a laboratory seawater microcosm. Sci Rep 2020; 10: 10945.

Yaradoddi

Banapurmath

Ganachari

, et al. Biodegradable carboxymethyl cellulose based material for sustainable packaging application. Sci Rep 2020; 10: 21960.

Tohamy

H-AS

. Reinforced modified carboxymethyl cellulose films with graphene oxide/silver nanoparticles as antimicrobial agents. Egypt J Chem 2022; 65: 509–518.

Jiang

Ngai

. Recent advances in chemically modified cellulose and its derivatives for food packaging applications: A review. Polymers 2022; 14: 1533.

Fernández-Braña

Feijoo-Costa

Dias-Ferreira

. Looking beyond the banning of lightweight bags: analysing the role of plastic (and fuel) impacts in waste collection at a Portuguese city. Environ Sci Pollut Control Ser 2019; 26: 35629–35647.

Tohamy

HAS

. Oil dispersing and adsorption by carboxymethyl cellulose–oxalate nanofibrils/nanocrystals and their kinetics. J Surfactants Deterg. 2023; 1. doi:10.1002/jsde.12706

Tohamy

H-AS

El-Sakhawy

El-Masry

, et al. Preparation of hydroxyethyl cellulose/mangiferin edible films and their antimicrobial properties. BMC chemistry 2022; 16: 1–7.

Mowafi

Tohamy

H-AS

. Application of electro-spun nano-fibers based on agriculture cellulosic biomaterial wastes for removal of dye and heavy metal from polluted water. J Text Inst. 2023; 1–10. doi:10.1080/00405000.2023.2235495, In press.

10.

Rajeswari

Christy

EJS

Swathi

, et al. Fabrication of improved cellulose acetate-based biodegradable films for food packaging applications. Environmental Chemistry and Ecotoxicology 2020; 2: 107–114.

11.

Attaran

Hassan

Wahit

. Materials for food packaging applications based on bio-based polymer nanocomposites: A review. J Thermoplast Compos Mater 2017; 30: 143–173.

12.

Yaradoddi

Patil

Ganachari

, et al. Biodegradable plastic production from fruit waste material and its sustainable use for green applications. Int J Pharmaceut Res Allied Sci 2016; 5: 72–81.

13.

Moreno

Atarés

Chiralt

, et al. Starch-gelatin antimicrobial packaging materials to extend the shelf life of chicken breast fillets. Lwt 2018; 97: 483–490.

14.

Lee

Kim

. Antioxidant activities of premature and mature mandarin (Citrus unshiu) peel and juice extracts. Food Sci Biotechnol 2022; 31: 627–633.

15.

Choi

M-H

Kim

K-H

Yook

H-S

. Antioxidant and antibacterial activity of premature Mandarin. J. Korean Soc. Food Sci. Nutr 2019. 48: 622–662.

16.

Mehmood

Dar

Ali

, et al. In vitro assessment of antioxidant, antibacterial and phytochemical analysis of peel of Citrus sinensis. Pak J Pharm Sci 2015; 28: 231–239.

17.

Shetty

Mahin-Syed-Ismail

Varghese

, et al. Antimicrobial effects of Citrus sinensis peel extracts against dental caries bacteria: An in vitro study. Journal of clinical and experimental dentistry 2016; 8: e71.

18.

Saleh

El-Gendi

El-Fakharany

, et al. Exploitation of cantaloupe peels for bacterial cellulose production and functionalization with green synthesized Copper oxide nanoparticles for diverse biological applications. Sci Rep 2022; 12: 19241.

19.

Šafranko

Ćorković

Jerković

, et al. Green extraction techniques for obtaining bioactive compounds from mandarin peel (Citrus unshiu var. Kuno): Phytochemical analysis and process optimization. Foods 2021; 10: 1043.

20.

Tohamy

H-AS

El-Sakhawy

Elnasharty

. Carboxymethyl cellulose membranes blended with carbon nanotubes/ag nanoparticles for eco-friendly safer lithium-ion batteries. Diam Relat Mater 2023; 138: 110205.

21.

Tohamy

H-AS

. Cellulosic nitrogen doped carbon quantum dots hydrogels with fluorescence/visco-elastic properties for pH-and temperature-sensitivity. Diam Relat Mater 2023; 136: 110027.

22.

Ghanem

Yassin

Rabie

, et al. Investigation of water sorption, gas barrier and antimicrobial properties of polycaprolactone films contain modified graphene. J Mater Sci 2021; 56: 497–512.

23.

McFarland

. The nephelometer: an instrument for estimating the number of bacteria in suspensions used for calculating the opsonic index and for vaccines. Journal of the American Medical Association 1907; 49: 1176–1178.

24.

Santoso

Prasetyaningsih

Madyaningrana

. Potency of Citrus reticulata Peel Extract as Active Compound of NonAlcohol Based Gel Hand Sanitizer. Sciscitatio 2020; 1: 79–86.

25.

Ganji

Singh

Friedman

. Phenolic content and antioxidant activity of extracts of 12 melon (Cucumis melo) peel powders prepared from commercial melons. J Food Sci 2019; 84: 1943–1948.

26.

Kaur

Panesar

Chopra

. Standardization of ultrasound-assisted extraction of bioactive compounds from kinnow Mandarin peel. Biomass Conversion and Biorefinery 2021; 13, 8853–8863.

27.

Espina

Somolinos

Lorán

, et al. Chemical composition of commercial citrus fruit essential oils and evaluation of their antimicrobial activity acting alone or in combined processes. Food Control 2011; 22: 896–902.

28.

Song

Liu

Wang

, et al., Antibacterial effects and mechanism of Mandarin (Citrus reticulata L.) essential oil against Staphylococcus aureus. Molecules 2020, 25(21): 4956.

29.

Wang

, et al. Tannin-Rich Fraction from Pomegranate Rind Damages Membrane of Listeria monocytogenes. Foodb Pathog Dis 2014; 11: 313–319.

30.

Viuda-Martos

Ruiz-Navajas

Fernández-López

, et al. Antibacterial activity of lemon (Citrus lemon L.), mandarin (Citrus reticulata L.), grapefruit (Citrus paradisiL.) and orange (Citrus sinensis L.) essential oils. J Food Saf 2008; 28: 567–576.

31.

Zhang

Liu

Wang

, et al. Antibacterial activity and mechanism of cinnamon essential oil against Escherichia coli and Staphylococcus aureus. Food Control 2016; 59: 282–289.

32.

Vella

Cautela

Laratta

, Characterization of polyphenolic compounds in Cantaloupe Melon by-products. Foods 2019; 8(6): 196.

33.

Kazemi

Samani

Ezzati

, et al., High-quality pectin from cantaloupe waste: eco-friendly extraction process, optimization, characterization and bioactivity measurements. J Sci Food Agric 2021; 101(15): 6552–6562.

34.

Calce

Mignogna

Bugatti

, et al. Pectin functionalized with natural fatty acids as antimicrobial agent. Int J Biol Macromol 2014; 68: 28–32.

35.

Trejo-González

Rodríguez-Hernández

A-I

López-Cuellar

Mdel R

, et al. Antimicrobial pectin-gellan films: effects on three foodborne pathogens in a meat medium, and selected physical-mechanical properties. CyTA - J Food 2018; 16(1): 469–476.

36.

Guo

, et al. Active-intelligent film based on pectin from watermelon peel containing beetroot extract to monitor the freshness of packaged chilled beef. Food Hydrocolloids 2021; 119: 106751.

37.

Gao

Wang

Lin

, et al. Separation, structural identification and antibacterial activity of pectin oligosaccharides derived from seed melon. Food Biosci 2023; 53: 102616.

Biodegradable carboxymethyl cellulose based material for sustainable/active food packaging application

Abstract

Keywords

Introduction

Materials and methods

Cantaloupe and mandarin extractions

Phytochemical screening

Carboxymethyl cellulose

Preparation of Carboxymethyl cellulose/cantaloupe and Carboxymethyl cellulose/mandarin edible films

Characterization

Determination of the degree of substitution of Carboxymethyl cellulose

Mechanical test

Reproducibility of the tests

Antimicrobial activity

Statistical analysis

Results and Discussion

Qualitative analysis of crude extracts

Fourier Transform Infra-Red spectroscopy

SEM analysis

Mechanical properties

XRD analysis

Antimicrobial properties

Conclusion

Footnotes

Acknowledgments

Author contributions

Declaration of conflicting interests

Funding

ORCID iD

Data Availability Statement

References