Production and Potential Uses of Biopolymers from Natural Sources and Agro-Industrial Waste

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biomacromolecules, Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: closed (25 June 2023) | Viewed by 23405

Special Issue Editors

Special Issue Information

Dear Colleagues,

The interest in research on polymers from natural sources has grown in recent years. In addition, the need for innovative products is now combined with the interest in low environmental impact production systems. From this perspective, scientific research has focused on obtaining production processes that involve the use of agro-industrial waste of little interest to obtain innovative products with high added value. Many of these products can be counted among biopolymers. The great variety of chemical structures offered by nature allows for the classification of various types of molecules as "biopolymers": from enzymes to polysaccharides such as inulin and bacterial exopolysaccharides, to microbial polyesters such as polyhydroxyalkanoates, to polyphenolic-based polymers such as lignin and tannins. The fields of application are equally varied. They range from biotransformations mediated by enzymes to medical and cosmetic applications, and from bioplastics to food packaging and bioremediation through the uptake of pollutants.

The Special Issue “Production and Potential Uses of Biopolymers from Natural Sources and Agro-Industrial Waste” therefore aims to collect and present the most recent advances in the field of biopolymers, from production to innovative properties, to any applications. The natural sources covered by this Special Issue belong to both the plant kingdom and microorganisms, whereas agro-industrial waste mainly refers to but is not limited to biomass that is currently poorly exploited. We would like to invite researchers of the sector to take part in this Special Issue by submitting a contribution in their field of expertise. Both original research papers or reviews are welcome.

Dr. Giuseppe Squillaci
Dr. Alessandra Morana
Guest Editors

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Keywords

  • agro-industrial waste
  • bioplastics
  • biopolymers
  • biomaterials
  • enzymes
  • exopolysaccharides
  • food-packaging
  • polyhydroxyalkanoates
  • tannins

Published Papers (10 papers)

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Research

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15 pages, 4626 KiB  
Article
Production and Characterization of Cellulosic Pulp from Mango Agro-Industrial Waste and Potential Applications
by Maribel García-Mahecha, Herlinda Soto-Valdez, Elizabeth Peralta, Elizabeth Carvajal-Millan, Tomás Jesús Madera-Santana, María Guadalupe Lomelí-Ramírez and Citlali Colín-Chávez
Polymers 2023, 15(15), 3163; https://doi.org/10.3390/polym15153163 - 26 Jul 2023
Cited by 1 | Viewed by 1674
Abstract
The growing demand for cellulosic pulp presents an opportunity to explore alternatives to this material, focusing on utilizing agro-industrial residues. Mango’s tegument is a rich source of cellulose, making it a valuable raw material for manufacturing single-use articles or blends with biopolymers. In [...] Read more.
The growing demand for cellulosic pulp presents an opportunity to explore alternatives to this material, focusing on utilizing agro-industrial residues. Mango’s tegument is a rich source of cellulose, making it a valuable raw material for manufacturing single-use articles or blends with biopolymers. In this sense, employing conventional alkaline and acid chemical treatments, the mango’s tegument was treated to obtain cellulosic pulp. The teguments were subjected to treatment with alkaline solutions (2% and 4% NaOH w/v) at 80 °C for 1 or 2 h or with an acetic acid solution (1:1 or 1:2 CH3COOH:H2O2) at 60–70 °C for 1 or 2 h. After treatment, an evaluation was conducted to assess the yield, color, chemical analysis, and structural, thermal, and morphological properties. The alkali treatments produced cellulosic pulps with a light color with 37–42% yield and reduced hemicellulose content. The acid treatments produced orange–brown cellulosic pulp with 47–48% yield and higher hemicellulose content. The acid pulps were thermally more stable (maximum decomposition at 348–357 °C) than the alkali pulps (maximum decomposition at 316–321 °C). The crystallinity index demonstrated that both treatments increased the crystallinity of the cellulose pulps compared with the untreated tegument. The thermal stability of cellulosic pulp at the processing temperatures of disposable tableware (50–120 °C) revealed that plates, bowls, trays, and cups could be produced. Another potential application is as a component of blends with biopolymers to make straws or rigid food packaging (trays) with reinforced structures. Full article
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15 pages, 3058 KiB  
Article
Microwave Assisted Extraction of Raw Alginate as a Sustainable and Cost-Effective Method to Treat Beach-Accumulated Sargassum Algae
by Aleksandra Nesic, Maria Valeria De Bonis, Giovanni Dal Poggetto, Gianpaolo Ruocco and Gabriella Santagata
Polymers 2023, 15(14), 2979; https://doi.org/10.3390/polym15142979 - 08 Jul 2023
Cited by 3 | Viewed by 1686
Abstract
This paper highlights the potential of Sargassum algae, recovered from raw beach seaweed wastes, as a valid source of valuable sodium alginate. Alginate is a biodegradable, highly attractive polysaccharide widely used in food, pharmaceuticals, and biomedicine applications. The aim of this work is [...] Read more.
This paper highlights the potential of Sargassum algae, recovered from raw beach seaweed wastes, as a valid source of valuable sodium alginate. Alginate is a biodegradable, highly attractive polysaccharide widely used in food, pharmaceuticals, and biomedicine applications. The aim of this work is to employ a new eco-sustainable and cost-effective extractive method to obtain alginate as a raw material from pollutant organic Sargassum seaweeds. Algae were exposed to microwave pre-treatment under static and dynamic conditions, and three different extractive protocols were followed: (a) conventional, (b) hot water and (c) alkaline method. All samples were characterized by GPC, SEM, FTIR/ATR and TGA. It was found that alginate’s best performances were obtained by the microwave dynamic pre-treatment method followed by alkaline extractive protocol. Nevertheless, the microwave pre-treatment of algae allowed the easiest breaking of their cell walls and the following fast releasing of sodium alginate. The authors demonstrated that microwave-enhanced extraction is an effective way to obtain sodium alginate from Sargassum-stranded seaweed waste materials in a cost-effective and eco-sustainable approach. They also assessed their applications as mulching films for agricultural applications. Full article
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11 pages, 2743 KiB  
Article
Bilayer Films of Poly(lactic acid) and Cottonseed Protein for Packaging Applications
by Atanu Biswas, Huai N. Cheng, Gary Kuzniar, Zhongqi He, Sanghoon Kim, Roselayne F. Furtado, Carlucio R. Alves and Brajendra K. Sharma
Polymers 2023, 15(6), 1425; https://doi.org/10.3390/polym15061425 - 13 Mar 2023
Cited by 3 | Viewed by 1798
Abstract
Poly(lactic acid) (PLA) is a common biobased film-former made from renewable biomass, such as polysaccharides from sugarcane, corn, or cassava. It has good physical properties but is relatively expensive when compared to the plastics used for food packaging. In this work, bilayer films [...] Read more.
Poly(lactic acid) (PLA) is a common biobased film-former made from renewable biomass, such as polysaccharides from sugarcane, corn, or cassava. It has good physical properties but is relatively expensive when compared to the plastics used for food packaging. In this work, bilayer films were designed, incorporating a PLA layer and a layer of washed cottonseed meal (CSM), an inexpensive agro-based raw material from cotton manufacturing, where the main component is cottonseed protein. These bilayer films were made through the solvent casting method. The combined thickness of the PLA/CSM bilayer film was between 47 and 83 μm. The thickness of the PLA layer in this film was 10%, 30%, or 50% of the total bilayer film’s thickness. Mechanical properties of the films, opacity, water vapor permeation, and thermal properties were evaluated. Since PLA and CSM are both agro-based, sustainable, and biodegradable, the bilayer film may be used as an eco-friendlier food packaging material, which helps reduce the environmental problems of plastic waste and microplastics. Moreover, the utilization of cottonseed meal may add value to this cotton byproduct and provide a potential economic benefit to cotton farmers. Full article
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18 pages, 2446 KiB  
Article
Optimization of Biocomposite Film Based on Whey Protein Isolate and Nanocrystalline Cellulose from Pineapple Crown Leaf Using Response Surface Methodology
by Fitriani Fitriani, Sri Aprilia, Muhammad Roil Bilad, Nasrul Arahman, Anwar Usman, Nurul Huda and Rovina Kobun
Polymers 2022, 14(15), 3006; https://doi.org/10.3390/polym14153006 - 25 Jul 2022
Cited by 5 | Viewed by 2252
Abstract
This study employed response surface methodology to optimize the preparation of biocomposites based on whey protein isolate, glycerol, and nanocrystalline cellulose from pineapple crown leaf. The effects of different concentrations of nanocrystalline cellulose as a filler and glycerol as a plasticizer on the [...] Read more.
This study employed response surface methodology to optimize the preparation of biocomposites based on whey protein isolate, glycerol, and nanocrystalline cellulose from pineapple crown leaf. The effects of different concentrations of nanocrystalline cellulose as a filler and glycerol as a plasticizer on the thickness, the tensile strength, and the elongation at break on the resulting biocomposite films were investigated. The central composite design was used to determine the optimum preparation conditions for biocomposite films with optimum properties. The regression of a second-order polynomial model resulted in an optimum composition consisting of 4% glycerol and 3.5% nanocrystalline cellulose concentrations, which showed a desirability of 92.7%. The prediction of the regression model was validated by characterizing the biocomposite film prepared based on the optimum composition, at which the thickness, tensile strength, and elongation at break of the biocomposite film were 0.13 mm, 7.16 MPa, and 39.10%, respectively. This optimum composition can be obtained in range concentrations of glycerol (4–8%) and nanocrystalline cellulose (3–7%). Scanning electron microscope images showed that nanocrystalline cellulose dispersed well in the pure whey protein isolate, and the films had a relatively smooth surface. In comparison, a rough and uneven surface results in more porous biocomposite films. Fourier transform infrared spectroscopy revealed that nanocrystalline cellulose and glycerol showed good compatibility with WPI film by forming hydrogen bonds. The addition of nanocrystalline cellulose as a filler also decreased the transparency, solubility, and water vapor permeability and increased the crystallinity index of the resulting biocomposite film. Full article
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14 pages, 2765 KiB  
Article
Biosorbents Based on Biopolymers from Natural Sources and Food Waste to Retain the Methylene Blue Dye from the Aqueous Medium
by Alexandra Cristina Blaga, Alexandra Maria Tanasă, Ramona Cimpoesu, Ramona-Elena Tataru-Farmus and Daniela Suteu
Polymers 2022, 14(13), 2728; https://doi.org/10.3390/polym14132728 - 03 Jul 2022
Cited by 10 | Viewed by 1984
Abstract
The use of a biosorbent based on residual biomass from brewing industry (Saccharomyces pastorianus) immobilized in a natural biopolymer (sodium alginate) was investigated for Methylene Blue removal from aqueous medium. Saccharomyces pastorianus, immobilized by a simple entrapment technique and by [...] Read more.
The use of a biosorbent based on residual biomass from brewing industry (Saccharomyces pastorianus) immobilized in a natural biopolymer (sodium alginate) was investigated for Methylene Blue removal from aqueous medium. Saccharomyces pastorianus, immobilized by a simple entrapment technique and by microencapsulation in alginate was characterized using SEM, EDAX, pHPZC and the biosorption behavior toward organic pollutant, such as cationic dye. The biosorption experiments were studied by assessing, in a first stage, the influence of the most important operational physical parameters on the efficiency of the biosorbent: the initial concentration of the dye, the contact time between phases, the temperature, the dye solution pH, the biosorbent granule size, and the amount of biosorbent. The highest sorption capacity was obtained for the biosorbent obtained by microencapsulation, at pH 9, at biosorbent dose of 5.28 g/L and a contact time of about 100 min. The biosorption equilibrium was then studied by modeling the data on the Langmuir, Freundlich and Dubinin- Radushkevich isotherms. The Langmuir model is best suited for experimental data on both particle sizes leading to a maximum biosorption capacity of 188.679 mg/g at room temperature. The values of the adsorption energy, E, obtained with the help of the Dubinin-Radushkevich model-suggest that the type of mechanism (physical or chemical) involved in the biosorption process depends on the particle size of the biosorbent. The results confirm that the residual microbial biomass of Saccharomyces pastorianus immobilized in a polymeric matrix such as sodium alginate, can be considered an efficient biosorbent in retaining cationic organic dyes present in aqueous solutions in moderate concentrations. Full article
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22 pages, 37213 KiB  
Article
An Innovative Preparation, Characterization, and Optimization of Nanocellulose Fibers (NCF) Using Ultrasonic Waves
by Abdullah K. Alanazi
Polymers 2022, 14(10), 1930; https://doi.org/10.3390/polym14101930 - 10 May 2022
Cited by 1 | Viewed by 2060
Abstract
Recently, environmental and ecological concerns have become a major issue owing to the shortage of resources, high cost, and so forth. In my research, I present an innovative, environmentally friendly, and economical way to prepare nanocellulose from grass wastes with a sodium hypochlorite [...] Read more.
Recently, environmental and ecological concerns have become a major issue owing to the shortage of resources, high cost, and so forth. In my research, I present an innovative, environmentally friendly, and economical way to prepare nanocellulose from grass wastes with a sodium hypochlorite (NaClO) solution of different concentrations (1–6% mol) at different times 10–80 min, washed with distilled water, and treated with ultrasonic waves. The optimum yield of the isolated cellulose was 95%, 90%, and 87% NaClO at 25 °C for 20 min and with NaOH and H2SO4 at 25 °C with 5% M, respectively. The obtained samples were characterized by dynamic light scattering (DLS), Fourier-transform infrared (FT-IR) spectroscopy, and X-ray diffraction (XRD). The effect of test temperature and reaction times on the crystallinity index (IC) of GNFC with different treated mediums was carried out and investigated. The IC was analyzed using the diffraction pattern and computed according to the Segal empirical method (method A), and the sum of the area under the crystalline adjusted peaks (method B) and their values proved that the effect of temperature is prominent. In both methods, GNFC/H2SO4 had the highest value followed by GNFC/NaOH, GNFC/NaClO and real sample nano fiber cellulose (RSNFC). The infrared spectral features showed no distinct changes of the four cellulose specimens at different conditions. The particle size distribution data proved that low acid concentration hydrolysis was not sufficient to obtain nano-sized cellulose particles. The Zeta potential was higher in accordance with (GNFC/H2SO4 > GNFC/NaOH > GNFC/NaClO), indicating the acid higher effect. Full article
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14 pages, 3334 KiB  
Article
Properties of Biocomposite Film Based on Whey Protein Isolate Filled with Nanocrystalline Cellulose from Pineapple Crown Leaf
by Fitriani Fitriani, Sri Aprilia, Nasrul Arahman, Muhammad Roil Bilad, Hazwani Suhaimi and Nurul Huda
Polymers 2021, 13(24), 4278; https://doi.org/10.3390/polym13244278 - 07 Dec 2021
Cited by 11 | Viewed by 2974
Abstract
Among the main bio-based polymer for food packaging materials, whey protein isolate (WPI) is one of the biopolymers that have excellent film-forming properties and are environmentally friendly. This study was performed to analyse the effect of various concentrations of bio-based nanocrystalline cellulose (NCC) [...] Read more.
Among the main bio-based polymer for food packaging materials, whey protein isolate (WPI) is one of the biopolymers that have excellent film-forming properties and are environmentally friendly. This study was performed to analyse the effect of various concentrations of bio-based nanocrystalline cellulose (NCC) extracted from pineapple crown leaf (PCL) on the properties of whey protein isolate (WPI) films using the solution casting technique. Six WPI films were fabricated with different loadings of NCC from 0 to 10 % w/v. The resulting films were characterised based on their mechanical, physical, chemical, and thermal properties. The results show that NCC loadings increased the thickness of the resulting films. The transparency of the films decreased at higher NCC loadings. The moisture content and moisture absorption of the films decreased with the presence of the NCC, being lower at higher NCC loadings. The water solubility of the films decreased from 92.2% for the pure WPI to 65.5% for the one containing 10 % w/v of NCC. The tensile strength of the films peaked at 7% NCC loading with the value of 5.1 MPa. Conversely, the trend of the elongation at break data was the opposite of the tensile strength. Moreover, the addition of NCC produced a slight effect of NCC in FTIR spectra of the WPI films using principal component analysis. NCC loading enhanced the thermal stability of the WPI films, as shown by an increase in the glass transition temperature at higher NCC loadings. Moreover, the morphology of the films turned rougher and more heterogeneous with small particle aggregates in the presence of the NCC. Overall, the addition of NCC enhanced the water barrier and mechanical properties of the WPI films by incorporating the PCL-based NCC as the filler. Full article
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12 pages, 5147 KiB  
Article
Isolation and Characterization of Nanocrystalline Cellulose Isolated from Pineapple Crown Leaf Fiber Agricultural Wastes Using Acid Hydrolysis
by Fitriani Fitriani, Sri Aprilia, Nasrul Arahman, Muhammad Roil Bilad, Amri Amin, Nurul Huda and Jumardi Roslan
Polymers 2021, 13(23), 4188; https://doi.org/10.3390/polym13234188 - 30 Nov 2021
Cited by 15 | Viewed by 3382
Abstract
Pineapple crown leaf fiber (PCLF) is one of the major biomass wastes from pineapple processing plants. It consists mostly of carbohydrate polymers, such as cellulose, hemicellulose, and lignin. It can be further processed to form a more valuable and widely used nanocrystalline cellulose [...] Read more.
Pineapple crown leaf fiber (PCLF) is one of the major biomass wastes from pineapple processing plants. It consists mostly of carbohydrate polymers, such as cellulose, hemicellulose, and lignin. It can be further processed to form a more valuable and widely used nanocrystalline cellulose (NCC). This study investigates the effect of hydrolysis time on the properties of the produced NCC. The acid hydrolysis was conducted using 1 M of sulfuric acid at hydrolysis times of 1–3 h. The resulting NCCs were then characterized by their morphology, functional groups, crystallinity, thermal stability, elemental composition, and production yield. The results show that the NCC products had a rod-like particle structure and possessed a strong cellulose crystalline structure typically found in agricultural fiber-based cellulose. The highest NCC yield was obtained at 79.37% for one hour of hydrolysis. This NCC also displayed a higher decomposition temperature of 176.98 °C. The overall findings suggest that PCLF-derived NCC has attractive properties for a variety of applications. Full article
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Review

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17 pages, 1534 KiB  
Review
Unlocking the Potential of Lignocellulosic Biomass Dragon Fruit (Hylocereus polyrhizus) in Bioplastics, Biocomposites and Various Commercial Applications
by N. H. Taharuddin, R. Jumaidin, M. R. Mansor, K. Z. Hazrati, J. Tarique, M. R. M. Asyraf and M. R. Razman
Polymers 2023, 15(12), 2654; https://doi.org/10.3390/polym15122654 - 12 Jun 2023
Viewed by 2371
Abstract
Dragon fruit, also called pitaya or pitahaya, is in the family Cactaceae. It is found in two genera: ‘Selenicereus’ and ‘Hylocereus’. The substantial growth in demand intensifies dragon fruit processing operations, and waste materials such as peels and seeds [...] Read more.
Dragon fruit, also called pitaya or pitahaya, is in the family Cactaceae. It is found in two genera: ‘Selenicereus’ and ‘Hylocereus’. The substantial growth in demand intensifies dragon fruit processing operations, and waste materials such as peels and seeds are generated in more significant quantities. The transformation of waste materials into value-added components needs greater focus since managing food waste is an important environmental concern. Two well-known varieties of dragon fruit are pitaya (Stenocereus) and pitahaya (Hylocereus), which are different in their sour and sweet tastes. The flesh of the dragon fruit constitutes about two-thirds (~65%) of the fruit, and the peel is approximately one-third (~22%). Dragon fruit peel is believed to be rich in pectin and dietary fibre. In this regard, extracting pectin from dragon fruit peel can be an innovative technology that minimises waste disposal and adds value to the peel. Dragon fruit are currently used in several applications, such as bioplastics, natural dyes and cosmetics. Further research is recommended for diverging its development in various areas and maturing the innovation of its usage. Full article
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16 pages, 2770 KiB  
Review
Carbonized Leather Waste: A Review and Conductivity Outlook
by Jaroslav Stejskal, Fahanwi Asabuwa Ngwabebhoh, Petr Sáha and Jan Prokeš
Polymers 2023, 15(4), 1028; https://doi.org/10.3390/polym15041028 - 18 Feb 2023
Cited by 5 | Viewed by 2051
Abstract
The carbonization of collagen-based leather waste to nitrogen-containing carbon is reviewed with respect to the preparation, characterization of carbonized products, and applications proposed in the literature. The resulting nitrogen-containing carbons with fibrous morphology have been used as adsorbents in water pollution treatment, in [...] Read more.
The carbonization of collagen-based leather waste to nitrogen-containing carbon is reviewed with respect to the preparation, characterization of carbonized products, and applications proposed in the literature. The resulting nitrogen-containing carbons with fibrous morphology have been used as adsorbents in water pollution treatment, in electrocatalysis, and especially in electrodes of energy-storage devices, such as supercapacitors and batteries. Although electrical conductivity has been implicitly exploited in many cases, the quantitative determination of this parameter has been addressed in the literature only marginally. In this report, attention has been newly paid to the determination of conductivity and its dependence on carbonization temperature. The resulting powders cannot be compressed into pellets for routine conductivity determination. A new method has been used to follow the resistivity of powders as a function of pressure up to 10 MPa. The conductivity at this pressure increased from 9.4 × 10−8 S cm−1 for carbonization at 500 °C to 5.3 S cm−1 at 1000 °C. The conductivity of the last sample was comparable with conducting polymers such as polypyrrole. The carbonized leather thus has the potential to be used in applications requiring electrical conduction. Full article
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