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Article

Preparation and Characterization of Black Seed/Cassava Bagasse Fiber-Reinforced Cornstarch-Based Hybrid Composites

1
Advanced Engineering Materials and Composites Research Centre, Department of Mechanical and Manufacturing Engineering, Universiti Putra Malaysia, Serdang 43400, Selangor, Malaysia
2
Sustainable Waste Management Research Group (SWAM), School of Chemical and Energy Engineering, Faculty of Engineering, Universiti Teknologi Malaysia, Johor Bahru 81310, Johor, Malaysia
3
Centre for Advanced Composite Materials (CACM), Universiti Teknologi Malaysia, Johor Bahru 81310, Johor, Malaysia
4
Laboratory of Biocomposite Technology, Institute of Tropical Forest and Forest Products, Universiti Putra Malaysia, Serdang 43400, Selangor, Malaysia
5
Department of Aerospace Engineering, Universiti Putra Malaysia, Serdang 43400, Selangor, Malaysia
6
Advanced Facilities Engineering Technology Research Cluster, Malaysian Institute of Industrial Technology (MITEC), University Kuala Lumpur, Persiaran Sinaran Ilmu, Bandar Seri Alam, Masai 81750, Johor, Malaysia
7
Facilities Maintenance Engineering Section, Malaysian Institute of Industrial Technology, Universiti Kuala Lumpur, Persiaran Sinaran Ilmu, Bandar Seri Alam, Johor Bahru 81750, Johor, Malaysia
*
Author to whom correspondence should be addressed.
Sustainability 2022, 14(19), 12042; https://doi.org/10.3390/su141912042
Submission received: 19 August 2022 / Revised: 16 September 2022 / Accepted: 20 September 2022 / Published: 23 September 2022
(This article belongs to the Special Issue Advances in Sustainable Valorization of Natural Waste and Biomass)

Abstract

:
Great advances have been made in the preparation of bioplastics and crude oil replacements to create a better and more sustainable and eco-friendly future for all. Here, we used cassava bagasse fibers at different ratios as reinforcement material to enhance the properties of black seed w-cornstarch films using the facile solution casting technique. The reinforced films showed compact and relatively smoother structures without porosity. The crystallinity values increased from 34.6 ± 1.6% of the control to 38.8 ± 2.1% in sample CS-BS/CB 9%, which reflects the mechanical properties of the composite. A gradual increase in tensile strength and elastic modulus was observed, with an increase in loading amounts of 14.07 to 18.22 MPa and 83.65 to 118.32 MPa for the tensile strength and elastic modulus, respectively. The composite film also exhibited faster biodegradation in the soil burial test, in addition to lower water absorption capacity. Using bio-based reinforcement material could significantly enhance the properties of bio-based packaging materials. The prepared hybrid composite could have a promising potential in food packaging applications as a safe alternative for conventional packaging.

1. Introduction

The past few years witnessed greatly advanced in sustainable and ecologically friendly materials due to the huge environmental problems associated with conventional non-biodegradable plastics [1,2,3]. The conversion of biomass into valuable materials has attracted the attention of scientists, which has both substantial economic and environmental relevance [4,5,6,7,8]. Throughout the last two decades, several developments have been made on biocomposites, making them functioning and interesting alternatives to conventional materials [9,10,11,12]. Cornstarch (CS), among the biomaterials, is a highly preferable polysaccharide polymer in bioplastics and biomaterials fabrication due to its sustainability, high availability, and ability to form a continuous matrix [13,14,15,16,17]. Nevertheless, CS exhibits several drawbacks, including its relatively strong hydrophilic character, in addition to its poor mechanical properties, which limited its applications for packaging purposes [18,19].
Several attempts have used numerous bioresources and natural fibers to enhance the mechanical properties of biocomposites but still mimic that of synthetic and crude oil plastic [20,21,22,23]. Black seed (Nigella sativa) is a famous medicinal plant that has been used for centuries for therapeutic purposes due to its anti-microbial, anti-diabetic, anti-inflammatory, anti-cancer, and anti-hypertensive activities [24]. The large-scale black seed oil industry produces a significant amount of waste every year (about 70% of the raw material) [25,26]. Most of these wastes are landfilled and not being furtherly utilized. Thymoquinone is one of the main active compounds in black seed that possess most of the therapeutic activities of the seeds and is characterized by hydrophobic properties, making it poorly soluble in water [27]. It has been reported that most black seed oil extraction methods allow a significant loss of waste, making this waste highly valuable for further utilization [25,28]. Black seed fiber was used in this study to utilize as a protective material to resist soil acidity and microbial attack.
Cassava bagasse is another cheap and broadly available fiber of cassava plant (Manihot esculenta) in tropical countries, which is considered a byproduct of cassava starch production [29]. Cassava bagasse is mainly composed of cellulose fibers along with residual starch, which ranges 15 and 50 wt%, making it highly attractive in several industrial applications. The industrial exploitation of cassava mainly includes the elimination of soluble sugars in addition to fiber separation. This result in the formation of two materials; purified cassava starch and cassava bagasse fibers [30]. Apart from containing cellulose and hemicelluloses, cassava bagasse also contains a high amount of starch, a natural polymer that has a high polarity due to the presence of large amounts of hydroxyls in its macromolecules, which interact with lignocellulosic fibers, resulting in improved mechanical properties [31].
Hence, the present study aims to use cassava bagasse fibers (CB) as reinforcement material to improve the mechanical and biodegradability properties of black seed fiber/cornstarch films by using a facile solution casting technique. The morphological and mechanical properties were analyzed and related to water absorption and biodegradation profile. Surface morphology and crystallinity were also analyzed.

2. Materials and Methods

2.1. Materials

The Cornstarch was obtained from Thye Huat Chan Sdn. Bhd. located at Sungai Buloh, Selangor, Malaysia, while the black seed (Nigella sativa) was obtained from Berkat Madinah Sdn. Bhd. (Selangor, Malaysia), after extracting the oil from the seeds. Cassava bagasse was purchased from NSK Trade City Kuchai Lama (Kuala Lumpur, Malaysia).

2.2. Preparation of the Film

The composite films were prepared using the conventional solution casting technique; 10 g of pure cornstarch (CS) was dissolved in 180 mL distilled water and heated for 20 min at 85 °C with continuous stirring (using a thermal-magnetic mixture) to allow starch gelation. Two types of plasticizer (fructose, and glycerol) were added to the solution in a similar ratio of 30% (w/w powder starch) along with black seed (BS) 9% (w/w powder starch) [5]. Different loading of cassava bagasse fibers (0, 3, 6, 9%) of dry starch-based was used as a hybridized agent. The final mixture was heated for an additional 20 min with continuous stirring until a gelatinized solution formed, which was then discharged evenly in a thermal petri dish. The dish with a casted solution was desiccated in an air circulation oven for 15 h at 65 °C. The formed films were removed gently from the dishes and kept at ambient conditions for 7 days prior to characterization. The obtained films were labeled according to their compositions and concentration of cassava bagasse fibers (CB), as shown in Table 1.

2.3. Characterization of Prepared Films

2.3.1. Physical and Morphological Analysis

The thickness of each film was calculated by an electronic caliper (Mitutoyo-Co., Kanagawa, Japan), using an inch accuracy of ±0.001. The density was directly measured from the weight and volume. Moisture content (MC) was calculated by weighing a constant dimension of each film (20 × 15 mm) and placed for 24 h in the dehydration oven at 105 °C. Then, the samples were weighed again and the difference in weights was determined as the MC of the sample. The film solubility was calculated using the same dimensions and drying step mentioned earlier and following the method described in Shojaee-Aliabadi et al. [32]. SEM (Hitachi S-3400 N, Nara, Japan) was used to observe the surface morphology of all the prepared samples by coating them with a thin golden layer to conduct electricity.

2.3.2. Surface Functional Groups and X-ray Diffraction Analysis

Fourier Transform Infrared Spectroscopy (FTIR) type (Bruker vector 22, Lancashire, UK) was used to investigate the surface functional group of prepared films, using 16 scans per sample and over a frequency range of 400 to 4000 cm−1. In order to determine the crystallinity index of each sample, a 2500 X-ray diffractometer (Rigaku, Tokyo, Japan) was used to analyze the XRD diffraction and calculate the crystallinity index in the same method described by [33].

2.3.3. Mechanical Properties

The mechanical properties of the films were investigated by tensile test according to D882 (ASTM, 2002) standards. The test was performed at room temperature (30 °C) using 5KN INSTRON tensile machine. Constant strips (10 × 70 mm) were prepared from each film and then firmly mounted between tensile clamps. Five replicates for each sample were done, using 2 mm/min crosshead speed, tensile strength, elongation at break, and elastic modulus was finally calculated.

2.3.4. Thermal Properties

The thermal gravimetric analyzer (TGA) instrument type (Q500 V20.13 Build 39, Bellingham, WA, USA) was used to study the thermal stability of the prepared film samples. Each sample was subjected to a temperature ranging from room temperature to 600 °C at an ascending rate of 10 °C/min.

2.3.5. Water Absorption and Soil Burial Test

Water absorption was calculated at room temperature by preparing constant dimensions (20 × 15 mm) of all the films and oven dried them for 3 h at 105 °C to eliminate all the moisture. The samples then were immediately weighted and steeped in distilled water for 3 h and the excess was removed from the surface by using a soft cloth. Water absorption was then determined using the following equation:
  Water   absorption   % = water   loadedfilm   initial   weight   initial   weight × 100
A soil burial test was conducted in polyethylene vials at room temperature in normal soil with the same method in [34].

2.4. Statistical Analyses

The statistical analyses of the findings were performed using Microsoft Excel 365, and the obtained data were plotted using Origin® 8.5 software (OriginLab Corporation, Northampton, MA, USA) for the graphical presentation of the results.

3. Results and Discussion

3.1. Physical and Morphological Analysis

The results of physical properties including moisture content (MC), density, thickness, and water solubility of the prepared film samples are presented in Table 2. The control had the highest MC, density, and water solubility, but it exhibited the lowest thickness. The addition of 3% CB increased the MC of the film from 7.54 ± 0.6 to only 6.81 ± 0.4%, but it reduced over again to 6.40 ± 0.2 and 6.02 ± 0.3% for CS-BS/CB6% and CS-BS/CB6% respectively. This could be attributed to the interaction that occurred between the BS and the CB; at a small amount, the interaction was limited, which led to an insufficient amount of interaction that was enhanced with loading more CB. The thickness clearly increased with the increase in loading amount from 0.272 ± 0.01 to 0.35 ± 0.04 µm, which also result in the reduction of the density value of the samples. The solubility of the film decreased from 34.23 to 31.47 ± 1.1% as the CB concentration increased, which could be due to the interaction that occurred between the materials that led to resistance of the water diffusion and enhance the film integrity [35].
Figure 1 presents the scanning electron microscope (SEM) of the prepared film samples at same magnification. The difference in surface morphology between the control, which appeared more rough and porous compared with the reinforced ones, can be seen. Reinforced films showed compact and relatively smoother structures without porosity; the interaction between CB, BS and the CS could be the reason for the smooth surfaces and absence of porosity. The highest homogenous surface can be seen in the sample with the highest loading amount (CS-BS/CB9%), which supports our hypothesis. Although the CS-BS/CB3% sample was found to be more homogenous and smoother than the control, weak interfacial interaction, which is mainly related to the formation of hydrogen bonds through hydroxyl groups, could be the reason for this, compared with the higher loading samples [36,37]. The correspond results of mechanical and FTIR analysis to the increase of homogeneity will be remarked on in their own subsection.

3.2. Surface Functional Groups

Since the chemical composition and the portions of all the films are well known, the FT-IR spectra (Figure 2) exhibited characteristic absorption peaks associated with the three materials of the hybrid components. The well-dispersed fillers caused the formation of similar spectra patterns, indicating the formation of alike chemical bonds within all samples. All the films showed the typical characteristic bands of starch O-H stretching, C-H, and C-O stretching at 3298, 2998, and 1151 cm−1, with slight shifting among them. The peak at 989.48 cm−1 appeared in all the samples corresponding to alkenes, which are the characteristics of black seed active compounds in addition to the aliphatic amines at 1033 and 1089 cm−1 [38]. Although the reinforced films did not show a significant difference between the three loading amounts, the slight shifting of peaks between the control and CS-BS/CB9% can be observed, which could be due to the effect of interaction between the three materials in the film. Higher CB loading formed greater hydrogen bonds quantitatively generated higher peak intensity. The band 1423 cm−1 appeared in all the samples, which corresponds to glycerol, while the ones between 1944 and 1649 cm−1 refer to bound water [39].

3.3. X-ray Diffraction (XRD)

The XRD curves of the black seed/cassava bagasse fiber reinforced cornstarch film composites are presented in Figure 3. The difference between the control and the three reinforced samples can be observed; the control increased the intensity of the two main peaks at 17 and 20°. However, among the reinforced fibers, CS-BS/CB 9% had significantly higher intensity compared with the other two samples. Owing to the gelatinization of starch molecules, sharper peaks can be observed in CS-BS/CB 9% at angles 17.82° and 20.47° in addition to 22.72°, which is the typical pattern of A-type plant starches [40]. The crystallinity values of the control were only 34.6 ± 1.6%, which increased with the increase of reinforcement percentage to become 38.8 ± 2.1% in sample CS-BS/CB 9%. The difference in crystallinity values could be attributed to the effect of starch reinforcement on the structure, which was also explained earlier by the mechanical properties. Natural fibers of black seed are oriented materials; they are able to combine with the starch molecules and thus improve the crystallinity of the film composite [41].

3.4. Mechanical Properties

The mechanical properties of the film are very important in order to be applicable for most practical applications. In this study, tensile testing of the film composites was done to measure each tensile strength, elastic modulus, and elongation at the break. As illustrated in Figure 4, it can be observed that the lowest tensile strength was reported for the control with only 14.07 MPa, which increased to 15.04, 16.65, and 18.22 MPa for the CS-BS/CB3%, CS-BS/CB6% and CS-BS/CB9%, respectively. Similarly, the elastic modulus increased from 83.65 MPa to 118.32 MPa. The gradual increase in tensile strength and elastic modulus is due to the homogeneous mixture and the interaction that occurred between the three materials, leading to an increase in rigidness and stiffness of the composite film with less flexibility, which was confirmed by the reduction in elongation at the break values [42]. The enhancement in the mechanical properties could have occurred due to the relative crystallinity, as we reported earlier and described by Salaberria et al.; the increase in the crystallinity of the film promotes the rigidity and stiffness of the film, leading to a reduction in elongation at the peak and thus better performance [43]. Black seed fibers also play a significant role by bonding the hydroxyl group with both CS and CB, leading to better transfer of stress from the film matrix to the fibers and thus higher tensile strength [33]. Furthermore, the significant reduction in film elongation can be explained by rebuilding the intermolecular bonding of the film, which improves its stiffness and rigidity, as described by da Rosa Zavareze et al., and also decreases the composite film flexibility by eliminating chain mobility [44,45,46,47,48]. Table 3 expresses the tensile strength and elongation at the break of several starch-based composites.

3.5. Thermal Properties

Thermal degradation of the prepared film composites mainly occurs in three different stages (Figure 5). The first stage corresponds to the moisture removal and sample dehydration, which started from 52 ± 2.6 °C until 163.5 ± 3.2 °C. At this stage, a clear difference can be observed in weight loss between the control, which had the highest weight loss, and CS-BS/CB9%, which showed the lowest. The second stage corresponds to the decomposition of starch molecules within the films, which occurred between 282 and 340 °C. The initial decomposition at 282 °C is attributed to the amylopectin and amylose differential degradation rate [55,56]. A similar effect for the reinforcement can be observed at this stage; the addition of CB into the film enhanced its thermal stability and reduced the weight loss due to the interactions in the composite matrix between the three materials. The greatest differences between the four investigated samples were observed in the third phase of degradation, which correlated to several oxygen-based reactions of carbonaceous residues—known as “glowing combustion” [57]. The control had the most significant weight loss at this stage; however, the reinforcement enhanced the stability and reduce the decomposition, in a similar way to what was reported by Florencia et al. [1]. Higher reinforcement samples CS-BS/CB6% and CS-BS/CB9% were clearly more stable by 12% than the control, owing to their higher residual carbohydrate content.

3.6. Water Absorption and Soil Burial Test

Water absorption is an important characteristic in packaging materials and is considered a major drawback in many bio-based films. Figure 6 presents the results of the water absorption investigation in this study, in which can be seen the effect of reinforcement on the water sensitivity of the films. At the initial assay (20 min of immersion), CS-BS/CB3% exhibited more water absorption than the control, which then reduced after 40 min of immersion to 63% compared to the control, which reported 67%. However, after the films reached the maximum degree of water saturation (180 min of immersion), a huge difference can be observed: the control showed the highest water absorption, at 64.7%, followed by CS-BS/CB3%, at 62.8%. The 6 and 9% CB reinforcement significantly reduced the water absorption to 51 and 42%, respectively, which could be due to the hydrogen bonding that occurred, resulting in the slight hydrophobic nature of the films [58]. Furthermore, the reduction of water absorption rate caused by CB reinforcement could be also attributed to the creation of interfacial bonding in the hybrid composite, which was confirmed earlier by the results of mechanical analysis. Such interfacial bonding hinders the water penetration through the film matrix and thus reduces its water absorption [59].
A soil burial test was conducted in normal soil at room temperature over a period of 12 days. Figure 7 presents the results of films’ biodegradability, in which can be seen the difference between them in the degradation rate. The CB reinforcement enhanced the biodegradation rate of the films; the highest rate was reported for CS-BS/CB9% with 99% degradation after 12 days. A previous study reported that the degradation of cassava film is greater than the corn-based one [60]; in our study, the biodegradation enhancement that occurred by CB reinforcement could be due to Cola cordifolia, which was found in both cassava and corn. Furthermore, the consumption of hydrogen bonding makes the film highly sensitive to microbial attacks and thus biodegrades easily [61]. In the case of control and CS-BS/CB3%, which absorbed a higher amount of water, the microorganisms are known for CO2 and water production as a result of bio-based material consumption. However, the Solvation of CO2 in the soil leads to the formation of H2CO3, forming an acidic environment around the film, which eventually reduces the microbial activity and thus limits the film’s biodegradation [62]. Although the presence of black seeds fiber helps in resisting soil acidity and microbial attack [63], the significant biodegradability of CS-BS/CB9% could be due to their limited water absorption, which maintains microbial activity, and also to the crystalline structure of the CB reinforcement.

4. Conclusions

Intensive studies have been conducted on waste utilization and the development of enhanced materials able to mimic synthetic plastic to overcome its associated environmental issue. In this study, cassava bagasse fibers at different ratios were used as a reinforcement to enhance the properties of black seed fiber-cornstarch films. The addition of fibers significantly enhanced the mechanical properties of the film and a gradual increase in tensile strength and elastic modulus was observed with an increase in loading amount. The composite film also exhibited faster biodegradation in the soil burial test in addition to lower water absorption capacity. Using fibers as reinforcement could significantly enhance the properties of bioplastics in terms of mechanical, water absorption, and biodegradation properties. The prepared hybrid composite could have promising potential in food packaging applications as a safe alternative to conventional packaging.

Author Contributions

Conceptualization, W.A. and S.M.S.; methodology, W.A.; formal analysis, W.A. and S.M.S.; writing original draft preparation, W.A.; writing—review and editing, W.A., S.M.S., M.T.H.S., M.F.M.A. and R.A.I.; visualization, W.A.; project administration, W.A., S.M.S. and R.A.I.; funding acquisition, S.M.S., W.A. and R.A.I. All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by University Putra Malaysia for financial support through Geran Putra Berimpak (UPM/800-3/3/1/GPB/2019/9679800) and the grant Inisiatif Putra Siswazah (GP-IPS/2021/9697100). The authors would like express gratitude for the financial support received from the Universiti Teknologi Malaysia, the project “The impact of Malaysian bamboos’ chemical and fibre characteristics on their pulp and paper properties, grant number PY/2022/02318—Q.J130000.3851.21H99”. The research has been carried out under the program Research Excellence Consortium (JPT (BPKI) 1000/016/018/25 (57)) provided by the Ministry of Higher Education Malaysia (MOHE).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Not applicable.

Acknowledgments

The authors would like to thank University Putra Malaysia for financial support through Geran Putra Berimpak (UPM/800-3/3/1/GPB/2019/9679800) and the grant Inisiatif Putra Siswazah (GP-IPS/2021/9697100). The authors would like express gratitude for the financial support received from the Universiti Teknologi Malaysia, the project “The impact of Malaysian bamboos’ chemical and fibre characteristics on their pulp and paper properties, grant number PY/2022/02318—Q.J130000.3851.21H99”. The research has been carried out under the program Research Excellence Consortium (JPT (BPKI) 1000/016/018/25 (57)) provided by the Ministry of Higher Education Malaysia (MOHE).

Conflicts of Interest

The authors declare no conflict of interest.

References

  1. Florencia, V.; López, O.V.; García, M.A. Exploitation of by-products from cassava and ahipa starch extraction as filler of thermoplastic corn starch. Compos. Part B Eng. 2020, 182, 107653. [Google Scholar] [CrossRef]
  2. Tarique, J.; Sapuan, S.; Khalina, A.; Ilyas, R.; Zainudin, E. Thermal, flammability, and antimicrobial properties of arrowroot (Maranta arundinacea) fiber reinforced arrowroot starch biopolymer composites for food packaging applications. Int. J. Biol. Macromol. 2022, 213, 1–10. [Google Scholar] [CrossRef] [PubMed]
  3. Zentou, H.; Abidin, Z.Z.; Yunus, R.; Biak, D.R.A.; Issa, M.A. Optimization and modeling of the performance of polydimethylsiloxane for pervaporation of ethanol−water mixture. J. Appl. Polym. Sci. 2020, 138, 50408. [Google Scholar] [CrossRef]
  4. Rizal, S.; Olaiya, F.; Saharudin, N.; Abdullah, C.; Olaiya, M.K.; Haafiz, M.M.; Yahya, E.; Sabaruddin, F.; Ikramullah; Khalil, H.P.S.A. Isolation of Textile Waste Cellulose Nanofibrillated Fibre Reinforced in Polylactic Acid-Chitin Biodegradable Composite for Green Packaging Application. Polymers 2021, 13, 325. [Google Scholar] [CrossRef]
  5. Abotbina, W.; Sapuan, S.M.; Ilyas, M.T.H.; Alkbir, M.F.M.; Ilyas, R.A. Development and Characterization of Cornstarch-Based Bioplastics Packaging Film Using a Combination of Different Plasticizers. Polymers 2021, 13, 3487. [Google Scholar] [CrossRef]
  6. Ilyas, R.A.; Zuhri, M.Y.M.; Aisyah, H.A.; Asyraf, M.R.M.; Hassan, S.A.; Zainudin, E.S.; Sapuan, S.M.; Sharma, S.; Bangar, S.P.; Jumaidin, R.; et al. Natural Fiber-Reinforced Polylactic Acid, Polylactic Acid Blends and Their Composites for Advanced Applications. Polymers 2022, 14, 202. [Google Scholar] [CrossRef]
  7. Ilyas, R.A.; Zuhri, M.Y.M.; Norrrahim, M.N.F.; Misenan, M.S.M.; Jenol, M.A.; Samsudin, S.A.; Nurazzi, N.M.; Asyraf, M.R.M.; Supian, A.B.M.; Bangar, S.P.; et al. Natural Fiber-Reinforced Polycaprolactone Green and Hybrid Biocomposites for Various Advanced Applications. Polymers 2022, 14, 182. [Google Scholar] [CrossRef]
  8. Ilyas, R.A.; Aisyah, H.A.; Nordin, A.H.; Ngadi, N.; Zuhri, M.Y.M.; Asyraf, M.R.M.; Sapuan, S.M.; Zainudin, E.S.; Sharma, S.; Abral, H.; et al. Natural-Fiber-Reinforced Chitosan, Chitosan Blends and Their Nanocomposites for Various Advanced Applications. Polymers 2022, 14, 874. [Google Scholar] [CrossRef]
  9. Abotbina, W.; Sapuan, S.; Sultan, M.; Alkbir, M.; Ilyas, R. Extraction, Characterization, and Comparison of Properties of Cassava Bagasse and Black Seed Fibers. J. Nat. Fibers 2022, 1–14. [Google Scholar] [CrossRef]
  10. Nazrin, A.; Sapuan, S.M.; Zuhri, M.Y.M.; Tawakkal, I.S.M.A.; Ilyas, R.A. Water barrier and mechanical properties of sugar palm crystalline nanocellulose reinforced thermoplastic sugar palm starch (TPS)/poly(lactic acid) (PLA) blend bionanocomposites. Nanotechnol. Rev. 2021, 10, 431–442. [Google Scholar] [CrossRef]
  11. Syafiq, R.M.O.; Sapuan, S.M.; Zuhri, M.Y.M.; Othman, S.H.; Ilyas, R.A. Effect of plasticizers on the properties of sugar palm nanocellulose/cinnamon essential oil reinforced starch bionanocomposite films. Nanotechnol. Rev. 2022, 11, 423–437. [Google Scholar] [CrossRef]
  12. Nazrin, A.; Sapuan, S.M.; Zuhri, M.Y.M.; Tawakkal, I.S.M.A.; Ilyas, R.A. Flammability and physical stability of sugar palm crystalline nanocellulose reinforced thermoplastic sugar palm starch/poly(lactic acid) blend bionanocomposites. Nanotechnol. Rev. 2021, 11, 86–95. [Google Scholar] [CrossRef]
  13. Surya, I.; Olaiya, N.; Rizal, S.; Zein, I.; Sri Aprilia, N.A.; Hasan, M.; Yahya, E.B.; Sadasivuni, K.K.; Abdul Khalil, H.P.S. Plasticizer enhancement on the miscibility and thermomechanical properties of polylactic acid-chitin-starch composites. Polymers 2020, 12, 115. [Google Scholar] [CrossRef] [PubMed]
  14. Ganguly, S.; Maity, T.; Mondal, S.; Das, P.; Das, N.C. Starch functionalized biodegradable semi-IPN as a pH-tunable controlled release platform for memantine. Int. J. Biol. Macromol. 2017, 95, 185–198. [Google Scholar] [CrossRef] [PubMed]
  15. Goldshtein, J.; Margel, S. Synthesis and characterization of polystyrene/2-(5-chloro-2H-benzotriazole-2-yl)-6-(1,1- dimethylethyl)-4-methyl-phenol composite microspheres of narrow size distribution for UV irradiation protection. Colloid Polym. Sci. 2011, 289, 1863–1874. [Google Scholar] [CrossRef]
  16. Ganguly, S.; Mondal, S.; Das, P.; Bhawal, P.; Maity, P.P.; Ghosh, S.; Dhara, S.; Das, N.C. Design of psyllium-g-poly(acrylic acid-co-sodium acrylate)/cloisite 10A semi-IPN nanocomposite hydrogel and its mechanical, rheological and controlled drug release behaviour. Int. J. Biol. Macromol. 2018, 111, 983–998. [Google Scholar] [CrossRef]
  17. Medina, D.D.; Goldshtein, J.; Margel, S.; Mastai, Y. Enantioselective Crystallization on Chiral Polymeric Microspheres. Adv. Funct. Mater. 2007, 17, 944–950. [Google Scholar] [CrossRef]
  18. Ghanbarzadeh, B.; Almasi, H.; Entezami, A.A. Improving the barrier and mechanical properties of corn starch-based edible films: Effect of citric acid and carboxymethyl cellulose. Ind. Crops Prod. 2011, 33, 229–235. [Google Scholar] [CrossRef]
  19. Abotbina, W.; Sapuan, S.M.; Sulaiman, S.; Ilyas, R.A. Review of corn starch biopolymer. In Proceedings of the 7th Postgraduate Seminar on Natural Fibre Reinforced Polymer Composites; Institute of Tropical Forest and Forest Products (INTROP), Universiti Putra Malaysia: Serdang, Malaysia, 2020; Volume 2020, pp. 37–40. [Google Scholar]
  20. Norfarhana, A.; Ilyas, R.; Ngadi, N. A review of nanocellulose adsorptive membrane as multifunctional wastewater treatment. Carbohydr. Polym. 2022, 291, 119563. [Google Scholar] [CrossRef]
  21. Bangar, S.P.; Harussani, M.; Ilyas, R.; Ashogbon, A.O.; Singh, A.; Trif, M.; Jafari, S.M. Surface modifications of cellulose nanocrystals: Processes, properties, and applications. Food Hydrocoll. 2022, 130, 107689. [Google Scholar] [CrossRef]
  22. Ilyas, R.; Sapuan, S.; Harussani, M.; Hakimi, M.; Haziq, M.; Atikah, M.; Asyraf, M.; Ishak, M.; Razman, M.; Nurazzi, N.; et al. Polylactic Acid (PLA) Biocomposite: Processing, Additive Manufacturing and Advanced Applications. Polymers 2021, 13, 1326. [Google Scholar] [CrossRef] [PubMed]
  23. Haris, N.I.N.; Hassan, M.Z.; Ilyas, R.; Suhot, M.A.; Sapuan, S.; Dolah, R.; Mohammad, R.; Asyraf, M. Dynamic mechanical properties of natural fiber reinforced hybrid polymer composites: A review. J. Mater. Res. Technol. 2022, 19, 167–182. [Google Scholar] [CrossRef]
  24. Ahmad, M.F.; Ahmad, F.A.; Ashraf, S.A.; Saad, H.H.; Wahab, S.; Khan, M.I.; Ali, M.; Mohan, S.; Hakeem, K.R.; Athar, M.T. An updated knowledge of Black seed (Nigella sativa Linn.): Review of phytochemical constituents and pharmacological properties. J. Herb. Med. 2021, 25, 100404. [Google Scholar] [CrossRef] [PubMed]
  25. Barkah, N.N.; Wiryawan, K.G.; Retnani, Y.; Wibawan, W.T.; Wina, E. Physicochemical properties of products and waste of black seed produced by cold press method. IOP Conf. Ser. Earth Environ. Sci. 2021, 756, 012025. [Google Scholar] [CrossRef]
  26. Abotbina, W.; Sapuan, S.M.; Ilyas, M.T.H.; Alkbir, M.F.M.; Ilyas, R.A.; Harussani, M.M. A Short Review on Black Seed Fibre (Nigella Sativa) Reinforced. In Proceedings of the 8th Postgraduate Seminar on Natural Fibre Composites 2022; Institute of Tropical Forest and Forest Products (INTROP), Universiti Putra Malaysia: Serdang, Malaysia, 2022; pp. 14–17. [Google Scholar]
  27. Younus, H. Molecular and Therapeutic Actions of Thymoquinone: Actions of Thymoquinone; Springer: Berlin/Heidelberg, Germany, 2018; ISBN 9789811088001. [Google Scholar]
  28. Ahmad, R.; Ahmad, N.; Shehzad, A. Solvent and temperature effects of accelerated solvent extraction (ASE) coupled with ultra-high pressure liquid chromatography (UHPLC-DAD) technique for determination of thymoquinone in commercial food samples of black seeds (Nigella sativa). Food Chem. 2019, 309, 125740. [Google Scholar] [CrossRef]
  29. Vedove, T.M.; Maniglia, B.C.; Tadini, C.C. Production of sustainable smart packaging based on cassava starch and anthocyanin by an extrusion process. J. Food Eng. 2020, 289, 110274. [Google Scholar] [CrossRef]
  30. Travalini, A.P.; Lamsal, B.; Magalhães, W.L.E.; Demiate, I.M. Cassava starch films reinforced with lignocellulose nanofibers from cassava bagasse. Int. J. Biol. Macromol. 2019, 139, 1151–1161. [Google Scholar] [CrossRef]
  31. Farias, F.O.; Jasko, A.C.; Colman, T.A.D.; Pinheiro, L.A.; Schnitzler, E.; Barana, A.C.; Demiate, I.M. Characterisation of Cassava Bagasse and Composites Prepared by Blending with Low-Density Polyethylene. Braz. Arch. Biol. Technol. 2014, 57, 821–830. [Google Scholar] [CrossRef]
  32. Shojaee-Aliabadi, S.; Hosseini, H.; Mohammadifar, M.A.; Mohammadi, A.; Ghasemlou, M.; Ojagh, S.M.; Hosseini, S.M.; Khaksar, R. Characterization of antioxidant-antimicrobial κ-carrageenan films containing Satureja hortensis essential oil. Int. J. Biol. Macromol. 2013, 52, 116–124. [Google Scholar] [CrossRef]
  33. Ibrahim, M.I.J.; Sapuan, S.M.; Zainudin, E.S.; Zuhri, M.Y.M. Preparation and characterization of cornhusk/sugar palm fiber reinforced Cornstarch-based hybrid composites. J. Mater. Res. Technol. 2020, 9, 200–211. [Google Scholar] [CrossRef]
  34. Kumaravel, S.; Hema, R.; Lakshmi, R. Production of Polyhydroxybutyrate (Bioplastic) and its Biodegradation by Pseudomonas Lemoignei and Aspergillus Niger. E-J. Chem. 2010, 7, S536–S542. [Google Scholar] [CrossRef]
  35. Jumaidin, R.; Sapuan, S.M.; Jawaid, M.; Ishak, M.R.; Sahari, J. Thermal, mechanical, and physical properties of seaweed/sugar palm fibre reinforced thermoplastic sugar palm Starch/Agar hybrid composites. Int. J. Biol. Macromol. 2017, 97, 606–615. [Google Scholar] [CrossRef] [PubMed]
  36. Lodha, P.; Netravali, A.N. Characterization of interfacial and mechanical properties of “green” composites with soy protein isolate and ramie fiber. J. Mater. Sci. 2002, 37, 3657–3665. [Google Scholar] [CrossRef]
  37. Diyana, Z.; Jumaidin, R.; Selamat, M.; Ghazali, I.; Julmohammad, N.; Huda, N.; Ilyas, R. Physical Properties of Thermoplastic Starch Derived from Natural Resources and Its Blends: A Review. Polymers 2021, 13, 1396. [Google Scholar] [CrossRef]
  38. Sangeetha, S.; Archit, R.; SathiaVelu, A. Phytochemical testing, antioxidant activity, HPTLC and FTIR analysis of antidiabetic plants Nigella sativa, Eugenia jambolana, Andrographis paniculata and Gymnema sylvestre. Res. J. Biotechnol. 2014, 9, 65–72. [Google Scholar]
  39. Ma, X.; Cheng, Y.; Qin, X.; Guo, T.; Deng, J.; Liu, X. Hydrophilic modification of cellulose nanocrystals improves the physicochemical properties of cassava starch-based nanocomposite films. LWT 2017, 86, 318–326. [Google Scholar] [CrossRef]
  40. Silva, M.L.T.; Brinques, G.B.; Gurak, P.D. Desenvolvimento e caracterização de bioplásticos de amido de milho contendo farinha de subproduto de broto. Braz. J. Food Technol. 2020, 23. [Google Scholar] [CrossRef]
  41. Huang, M.-F.; Yu, J.-G.; Ma, X.-F. Studies on the properties of Montmorillonite-reinforced thermoplastic starch composites. Polymer 2004, 45, 7017–7023. [Google Scholar] [CrossRef]
  42. Dias, A.B.; Müller, C.M.; Larotonda, F.D.; Laurindo, J.B. Mechanical and barrier properties of composite films based on rice flour and cellulose fibers. LWT 2011, 44, 535–542. [Google Scholar] [CrossRef]
  43. Salaberria, A.M.; Labidi, J.; Fernandes, S.C. Chitin nanocrystals and nanofibers as nano-sized fillers into thermoplastic starch-based biocomposites processed by melt-mixing. Chem. Eng. J. 2014, 256, 356–364. [Google Scholar] [CrossRef]
  44. da Rosa Zavareze, E.; Pinto, V.Z.; Klein, B.; El Halal, S.L.M.; Elias, M.C.; Prentice-Hernández, C.; Dias, A.R.G. Development of oxidised and heat–moisture treated potato starch film. Food Chem. 2012, 132, 344–350. [Google Scholar] [CrossRef] [PubMed] [Green Version]
  45. Ilyas, R.A.; Sapuan, S.M.; Ishak, M.R.; Zainudin, E.S. Development and characterization of sugar palm nanocrystalline cellulose reinforced sugar palm starch bionanocomposites. Carbohydr. Polym. 2018, 202, 186–202. [Google Scholar] [CrossRef] [PubMed]
  46. Ilyas, R.A.; Sapuan, S.M.; Ibrahim, R.; Abral, H.; Ishak, M.; Zainudin, E.; Asrofi, M.; Atikah, M.S.N.; Huzaifah, M.R.M.; Radzi, A.M.; et al. Sugar palm (Arenga pinnata (Wurmb.) Merr) cellulosic fibre hierarchy: A comprehensive approach from macro to nano scale. J. Mater. Res. Technol. 2019, 8, 2753–2766. [Google Scholar] [CrossRef]
  47. Ilyas, R.; Sapuan, S.; Ibrahim, R.; Abral, H.; Ishak, M.; Zainudin, E.; Atikah, M.; Nurazzi, N.M.; Atiqah, A.; Ansari, M.; et al. Effect of sugar palm nanofibrillated cellulose concentrations on morphological, mechanical and physical properties of biodegradable films based on agro-waste sugar palm (Arenga pinnata (Wurmb.) Merr) starch. J. Mater. Res. Technol. 2019, 8, 4819–4830. [Google Scholar] [CrossRef]
  48. Syafri, E.; Yulianti, E.; Asrofi, M.; Abral, H.; Sapuan, S.M.; Ilyas, R.A.; Fudholi, A. Effect of sonication time on the thermal stability, moisture absorption, and biodegradation of water hyacinth (Eichhornia crassipes) nanocellulose-filled bengkuang (Pachyrhizus erosus) starch biocomposites. J. Mater. Res. Technol. 2019, 8, 6223–6231. [Google Scholar] [CrossRef]
  49. Edhirej, A.; Sapuan, S.M.; Jawaid, M.; Zahari, N.I. Preparation and characterization of cassava bagasse reinforced thermoplastic cassava starch. Fibers Polym. 2017, 18, 162–171. [Google Scholar] [CrossRef]
  50. Ibrahim, M.I.J.; Sapuan, S.M.; Zainudin, E.S.; Zuhri, M.Y.M. Potential of using multiscale corn husk fiber as reinforcing filler in cornstarch-based biocomposites. Int. J. Biol. Macromol. 2019, 139, 596–604. [Google Scholar] [CrossRef]
  51. Hazrol, M.D.; Sapuan, S.M.; Zainudin, E.S.; Wahab, N.I.A.; Ilyas, R.A. Effect of Kenaf Fibre as Reinforcing Fillers in Corn. Polymers 2022, 14, 1590. [Google Scholar] [CrossRef]
  52. Othman, S.H.; Tarmiti, N.A.N.; Shapi’I, R.A.; Zahiruddin, S.M.M.; Tawakkal, I.S.M.A.; Basha, R.K. Starch/banana pseudostem biocomposite films for potential food packaging applications. BioResources 2020, 15, 3984–3998. [Google Scholar] [CrossRef]
  53. Hazrati, K.; Sapuan, S.; Zuhri, M.; Jumaidin, R. Preparation and characterization of starch-based biocomposite films reinforced by Dioscorea hispida fibers. J. Mater. Res. Technol. 2021, 15, 1342–1355. [Google Scholar] [CrossRef]
  54. Sanyang, M.L.; Sapuan, S.M.; Jawaid, M.; Ishak, M.R.; Sahari, J. Effect of Sugar Palm-derived Cellulose Reinforcement on the Mechanical and Water Barrier Properties of Sugar Palm Starch Biocomposite Films. BioResources 2016, 11, 4134–4145. [Google Scholar] [CrossRef] [Green Version]
  55. López, O.; Versino, F.; Villar, M.; García, M. Agro-industrial residue from starch extraction of Pachyrhizus ahipa as filler of thermoplastic corn starch films. Carbohydr. Polym. 2015, 134, 324–332. [Google Scholar] [CrossRef] [PubMed]
  56. Ilyas, R.; Sapuan, S.M.; Ibrahim, R.; Abral, H.; Ishak, M.R.; Zainudin, E.S.; Atiqah, A.; Atikah, M.S.N.; Syafri, E.; Asrofi, M.; et al. Thermal, Biodegradability and Water Barrier Properties of Bio-Nanocomposites Based on Plasticised Sugar Palm Starch and Nanofibrillated Celluloses from Sugar Palm Fibres. J. Biobased Mater. Bioenergy 2020, 14, 234–248. [Google Scholar] [CrossRef]
  57. López, O.V.; Ninago, M.; Lencina, M.M.S.; García, M.A.; Andreucetti, N.A.; Ciolino, A.E.; Villar, M.A. Thermoplastic starch plasticized with alginate–glycerol mixtures: Melt-processing evaluation and film properties. Carbohydr. Polym. 2015, 126, 83–90. [Google Scholar] [CrossRef]
  58. Tavares, K.M.; de Campos, A.; Mitsuyuki, M.C.; Luchesi, B.R.; Marconcini, J.M. Corn and cassava starch with carboxymethyl cellulose films and its mechanical and hydrophobic properties. Carbohydr. Polym. 2019, 223, 115055. [Google Scholar] [CrossRef]
  59. Ramírez, M.G.L.; Satyanarayana, K.G.; Iwakiri, S.; de Muniz, G.I.B.; Tanobe, V.; Flores-Sahagun, T.S. Study of the properties of biocomposites. Part, I. Cassava starch-green coir fibers from Brazil. Carbohydr. Polym. 2011, 86, 1712–1722. [Google Scholar] [CrossRef]
  60. Zoungranan, Y.; Lynda, E.; Dobi-Brice, K.K.; Tchirioua, E.; Bakary, C.; Yannick, D.D. Influence of natural factors on the biodegradation of simple and composite bioplastics based on cassava starch and corn starch. J. Environ. Chem. Eng. 2020, 8, 104396. [Google Scholar] [CrossRef]
  61. Anugrahwidya, R.; Armynah, B.; Tahir, D. Bioplastics Starch-Based with Additional Fiber and Nanoparticle: Characteristics and Biodegradation Performance: A Review. J. Polym. Environ. 2021, 29, 3459–3476. [Google Scholar] [CrossRef]
  62. Emadian, S.M.; Onay, T.T.; Demirel, B. Biodegradation of bioplastics in natural environments. Waste Manag. 2017, 59, 526–536. [Google Scholar] [CrossRef]
  63. Sabbah, M.; Altamimi, M.; Di Pierro, P.; Schiraldi, C.; Cammarota, M.; Porta, R. Black Edible Films from Protein-Containing Defatted Cake of Nigella sativa Seeds. Int. J. Mol. Sci. 2020, 21, 832. [Google Scholar] [CrossRef] [Green Version]
Figure 1. Surface morphology black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Figure 1. Surface morphology black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
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Figure 2. FT−IR curves of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Figure 2. FT−IR curves of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
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Figure 3. X-ray diffraction curves of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Figure 3. X-ray diffraction curves of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
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Figure 4. The mechanical properties of black seed/cassava bagasse fiber-reinforced cornstarch hybrid composite film.
Figure 4. The mechanical properties of black seed/cassava bagasse fiber-reinforced cornstarch hybrid composite film.
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Figure 5. TGA curves of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Figure 5. TGA curves of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
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Figure 6. Water absorption of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Figure 6. Water absorption of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
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Figure 7. Soil burial test of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Figure 7. Soil burial test of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
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Table 1. Mixing proportion of different black seed/cassava bagasse fiber-reinforced cornstarch hybrid composite film.
Table 1. Mixing proportion of different black seed/cassava bagasse fiber-reinforced cornstarch hybrid composite film.
FilmFructose and Glycerol g/g Dry StarchStarch g/180 mL Distilled WaterBS g/100 g of Dry StarchCB g/100 g of Dry Starch
Control(CS/BS)0.31090
CS-BS/CB3%0.31093
CS-BS/CB6%0.31096
CS-BS/CB9%0.31099
Table 2. Physical characteristics of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Table 2. Physical characteristics of black seed/cassava bagasse fiber reinforced cornstarch hybrid composite film.
Sample NameMC (%)Density (g/cm3)Thickness (µm)Solubility (%)
Control7.546 ± 0.61.34 ± 0.020.272 ± 0.0134.23 ± 2.0
CS-BS/CB3%6.813 ± 0.41.31 ± 0.070.274 ± 0.0832.93 ± 1.4
CS-BS/CB6%6.406 ± 0.21.29 ± 0.010.332 ± 0.0532.45 ± 0.9
CS-BS/CB9%6.026 ± 0.31.25 ± 0.060.35 ± 0.0431.47 ± 1.1
Table 3. The tensile strength (TS) and elongation at break (E) of various starch-based composites.
Table 3. The tensile strength (TS) and elongation at break (E) of various starch-based composites.
PolymerFiberPlasticizerTSEReference
Cassava starchCassava bagasse
(6 wt.%)
Fructose10.78 MPa3.19 mm[49]
Corn starchCorn Husk
(8 wt.%)
Fructose12.84 MPa3.7%[50]
Corn starchKenaf fiber
(6 wt.%)
Sorbitol17.74 MPa48.79%[51]
Cassava starchBanana pseudostem powder
(10 wt.%)
-16 MPa113.5%[52]
Dioscorea hispida starchDioscorea hispida
Fiber (6 wt.%)
Sorbitol9.29 MPa25.44%[53]
Sugar palm starchSugar palm cellulose fiber (10 wt.%)Glycerol and sorbitol19.68 MPa32.8%[54]
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Abotbina, W.; Sapuan, S.M.; Ilyas, R.A.; Sultan, M.T.H.; Alkbir, M.F.M. Preparation and Characterization of Black Seed/Cassava Bagasse Fiber-Reinforced Cornstarch-Based Hybrid Composites. Sustainability 2022, 14, 12042. https://doi.org/10.3390/su141912042

AMA Style

Abotbina W, Sapuan SM, Ilyas RA, Sultan MTH, Alkbir MFM. Preparation and Characterization of Black Seed/Cassava Bagasse Fiber-Reinforced Cornstarch-Based Hybrid Composites. Sustainability. 2022; 14(19):12042. https://doi.org/10.3390/su141912042

Chicago/Turabian Style

Abotbina, Walid, S. M. Sapuan, R. A. Ilyas, M. T. H. Sultan, and M. F. M. Alkbir. 2022. "Preparation and Characterization of Black Seed/Cassava Bagasse Fiber-Reinforced Cornstarch-Based Hybrid Composites" Sustainability 14, no. 19: 12042. https://doi.org/10.3390/su141912042

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