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Biopolymers are natural polymers derived from plants and animals, which include a variety of polysaccharides, polypeptides, and polynucleotides [9], while biomonomers are small molecules (i.e., monomeric subunits) that can undergo ex situ chemocatalytic polymerization to produce biobased polymers [10]. The utilization of biopolymers is not limited to bioplastics but ranges from sustainable production of other materials such as biofuels, bio-implants, and medicinal products [11]. Seaweed is considered one of the most potential biopolymers. Kappaphycus alvarezii, a red seaweed, is an eco-friendly, abundant, sustainable, and low-cost bioresource. The chemical composition of Kappaphycus alvarezii was 65.20% carbohydrate, 11.57% ash, 3.40% protein, and 1.10% lipid contents [12]. In this sense, carrageenan is a natural carbohydrate (polysaccharide) and commercially essential phycocolloid generated from red seaweeds. The extraction and purification process of carrageenan is expensive, time-consuming, and requires abundant chemicals and water during processing [13]. To overcome these issues, raw red seaweed was used for the development of bioplastic films since it is cheaper and easier to process than pure carrageenan.
Recent studies have reported that raw seaweed can actually form a bioplastic film with adequate ultimate performance [12,14]. However, bioplastics suffer from several shortcomings, which were encountered as the majority of bioplastics are unable to stand if used alone. The hydrophilic nature of seaweed, with its poor water barrier and antimicrobial properties, has limited its use for packaging applications [15]. To overcome these challenges, either organic or inorganic fillers that are less hydrophilic or hydrophobic are blended with raw seaweed or seaweed-derived polymers to broaden their applications [16]. The effectiveness of introducing organic fillers to improve the seaweed-based bioplastic film has been previously reported [17]. Hence, the use of organic fillers derived from solid biowaste is an excellent candidate for reinforcing materials in seaweed films due to their cost-effective, abundant, and eco-friendly nature.
Surface morphologies by SEM and surface roughness by AFM of the bioplastic films for (a) control; unpurified and purified LNPs, (b,c) 1%, (d,e) 3%, (f,g) 5%, and (h,i) 7%.
Figure 4 shows the XRD measurement results of the control film and Kappaphycus alvarezii reinforced with unpurified and purified LNPs between 10 to 40 (2θ). According to the obtained diffraction patterns, all films achieved a broad peak between 20 to 25, indicating the amorphous characteristics of the matrix. It can be observed that the neat film showed several other bands at 29.56, 35.36, and 39.51, indicating the crystalline nature of Kappaphycus alvarezii. The crystalline band identified by XRD should be ascribed to the minerals (potassium chloride and sodium chloride) contained in the matrix. These findings were also consistent with previous works that reported similar phases of the red seaweed with the present work [44,45].
Hydrophobicity and physical properties of (a) contact angle, (b) water vapor permeability, and (c) water solubility of the LNP-reinforced bioplastic films. The same letters above the data bars indicate no significant difference in the values (p < 0.05).
The purified films showed a superior contact angle than the unpurified ones. This denotes that the LNPs with purification enhanced film compatibility and miscibility within the Kappaphycus alvarezii matrix. Consequently, a reduction of porosity was observed, and more organized layers with lesser gaps in the bioplastic were achieved by introducing purified LNPs. However, a decreased trend of contact angle value loading was observed after achieving the optimum value. The LNPs at higher loading may probably have agglomerated in the bioplastic film [51]. This finding is in line with the results of the morphological properties of bioplastic films by SEM and AFM.
Photographic images and diameter statistics of inhibition zone measurement results of control film and unpurified/purified LNP films at different loadings against (a,b) E. coli and (c,d) S. aureus. Means of inhibition zone diameter followed by different superscript letters indicate significant differences (p < 0.05).
The pure Kappaphycus alvarezii film exhibited no appearance of an inhibition zone against the investigated bacteria. An inhibition zone was clearly observed in the films incorporated with LNPs. This difference was significant (p < 0.05) where the addition of 1% unpurified and purified LNPs into the films demonstrated an inhibition zone diameter of 9.37 mm and 14.83 mm for Escherichia coli, and 8.82 mm and 15.24 mm for Staphylococcus aureus, respectively. A noticeable progressive inhibition trend of the observed bacteria test specimens was recorded as the fraction of both LNPs was increased in the bioplastics structure. This indicates that the activity of anti-bacteria referred to the bioplastic film forming with nanosized lignin and the uniform dispersion in the Kappaphycus alvarezii matrix network [59]. In the case of unpurified LNPs, the optimum diameter of the inhibition zone against Escherichia coli and Staphylococcus aureus was obtained with 7% filler loading as 16.96 mm and 19.71 mm, respectively. With the same loading fraction, the optimum inhibitory zones of purified LNPs against Escherichia coli and Staphylococcus aureus were recorded as 22.48 and 21.38 mm, respectively. There was an obvious sterile zone surrounding the films, and both Escherichia coli and Staphylococcus aureus showed almost similar inhibitory zones at equal filler loading for each LNP and clear inhibitory effects. However, it is important to note that the purified films presented superior antibacterial activity compared to the unpurified films. This should be attributable to the higher amount of bioactive compounds in purified LNPs than LNPs without purification [60,61].
Digital images and weight loss before and after soil burial of biodegradable plastic films at 0, 10, 20, 30, and 40 days. Means in the same column followed by the same superscript letters denote no significant difference (p < 0.05). 153554b96e
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