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Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications

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A special issue of Gels (ISSN 2310-2861). This special issue belongs to the section "Gel Processing and Engineering".

Deadline for manuscript submissions: closed (5 November 2023) | Viewed by 22648

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Prof. Dr. H.P.S. Abdul Khalil

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Cluster of Green Biopolymer, Coatings & Packaging, School of Industrial Technology, Penang 11800, Malaysia
Interests: biopolymers; biocomposite; bioplastic; aerogel; nanofiber
Special Issues, Collections and Topics in MDPI journals

Dr. Esam Bashir Yahya

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Guest Editor

Cluster of Green Biopolymer, Coatings & Packaging, School of Industrial Technology, Universiti Sains Malaysia, Penang 11800, Malaysia
Interests: biopolymers; hydrogels; aerogels; biotechnology

Special Issue Information

Dear Colleagues,

Marine-biopolymer-based materials such as hydrogels, xerogels, and aerogels have been highly attractive research areas in recent decades for different applications in daily life. They are considered as interesting biomaterials for medical applications due to their good biocompatibility, biodegradability, inexpensiveness, stability, abundance, ease of surface modification, and nontoxic nature. They are also interesting materials for nonmedical applications such as food packaging, water treatment, production of bioplastics, cosmetics, etc., as they possess excellent mechanical, thermal, and biological activities. Numerous marine biopolymers such as alginates, agar, carrageenan, and chitosan have been used as bio-ink in the preparation of different forms of gels using conventional and 3D-printing techniques. This Special Issue will present and discuss different approaches for the preparation, modification, and characterizations of hydrogels, xerogels, and aerogels from marine-based biopolymers for different medical and nonmedical applications.

Prof. Dr. H.P.S. Abdul Khalil
Dr. Esam Bashir Yahya
Guest Editors

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Keywords

preparation, modification, characterization, and applications of hydrogels from marine-biopolymer precursors (chitosan, agar, carrageenan, alginate, and others)
preparation, modification, characterization, and applications of marine-based xerogels
preparation, modification, characterization, and applications of hydrogels from marine-biopolymer precursors
marine-based bio-ink and 3D preparation technology
medical and nonmedical applications of marine-biopolymer-based gels or any other related research

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Published Papers (10 papers)

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Research

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17 pages, 4049 KiB

Open AccessArticle

Active Fish Gelatin/Chitosan Blend Film Incorporated with Guava Leaf Powder Carbon Dots: Properties, Release and Antioxidant Activity

by Gokulprasanth Murugan, Krisana Nilsuwan, Thummanoon Prodpran, Arunachalasivamani Ponnusamy, Jong-Whan Rhim, Jun Tae Kim and Soottawat Benjakul

Gels 2024, 10(4), 281; https://doi.org/10.3390/gels10040281 - 21 Apr 2024

Cited by 6 | Viewed by 2496

Abstract

Active packaging is an innovative approach to prolonge the shelf-life of food products while ensuring their quality and safety. Carbon dots (CDs) from biomass as active fillers for biopolymer films have been introduced to improve their bioactivities as well as properties. Gelatin/chitosan (G/C) blend films containing active guava leaf powder carbon dots (GL-CDs) at various levels (0–3%, w/w) were prepared by the solvent casting method and characterized. Thickness of the control increased from 0.033 to 0.041 mm when 3% GL-CDs were added (G/C-CD-3%). Young’s modulus of the resulting films increased (485.67–759.00 MPa), whereas the tensile strength (26.92–17.77 MPa) and elongation at break decreased (14.89–5.48%) as the GL-CDs’ level upsurged (p < 0.05). Water vapor barrier property and water contact angle of the film were enhanced when incorporated with GL-CDs (p < 0.05). GL-CDs had a negligible impact on film microstructure, while GL-CDs interacted with gelatin or chitosan, as determined by FTIR. The release of GL-CDs from blend films was more pronounced in water than in alcoholic solutions (10–95% ethanol). The addition of GL-CDs improved the UV light barrier properties and antioxidant activities of the resultant films in a dose-dependent manner. Thus, GL-CD-added gelatin/chitosan blend films with antioxidant activities could be employed as potential active packaging for the food industry. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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19 pages, 15713 KiB

Open AccessArticle

A Novel Strategy for Topical Administration by Combining Chitosan Hydrogel Beads with Nanostructured Lipid Carriers: Preparation, Characterization, and Evaluation

by Rui Sun, Qiang Xia and Yufeng Sun

Gels 2024, 10(3), 160; https://doi.org/10.3390/gels10030160 - 21 Feb 2024

Cited by 1 | Viewed by 1619

Abstract

The objective of the present study was to develop and evaluate NLC–chitosan hydrogel beads for topical administration. The feasibility of the preparation technology was verified by investigating various formulation factors and the impact of chitosan hydrogel beads on the NLC. The encapsulation efficiency of NLC–chitosan hydrogel beads was above 95% in optimized process conditions. The physical characterization of the NLC–chitosan hydrogel beads showed that the NLC was distributed within the network of the chitosan hydrogel beads. Furthermore, the incorporation of NLC into the chitosan hydrogel beads was related to the electrostatic interaction between the surface of the NLC and chitosan, which influenced the lipid ordering degree of the NLC and contributed to the stability. The stability studies showed that the retention rate of quercetin in the NLC–chitosan hydrogel beads was 88.63 ± 2.57% after 10 months of storage under natural daylight. An in vitro permeation study showed that NLC–chitosan hydrogel beads exhibited superior ability in enhancing skin permeation by hydrophobic active ingredients compared to the NLC and significantly increased skin accumulation. These studies demonstrated that the use of NLC–chitosan hydrogel beads might be a promising strategy for the delivery of hydrophobic active ingredients in topical administration. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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18 pages, 4551 KiB

Open AccessArticle

Nexus Advances Using Marine Biopolymeric Gel Material as a Photocatalyst for the Oxidation of Agricultural Wastewater Containing Insecticides

by Ehssan Ahmed Hassan and Maha A. Tony

Gels 2023, 9(11), 864; https://doi.org/10.3390/gels9110864 - 30 Oct 2023

Viewed by 1280

Abstract

The attention of the research community is focused not only on waste elimination, but also on waste valorization. The natural marine biopolymer gel substance chitosan, which can be derived from the waste substances of marine life, is a polymer-matrix-based nanocomposite. Chitosan attracts special attention due to its potential applications, especially in wastewater treatment. In this regard, magnetite-incorporated chitosan powders of nanometer scale were synthesized by a simple co-precipitation method to attain the dual functions of chitosan gel and magnetite. The synthesized magnetite-incorporated chitosan nanopowders were verified using X-ray diffraction (XRD), Fourier-transform infrared (FTIR) spectroscopy, a vibrating-sample magnetometer (VSM), a scanning electron microscope (SEM), and transmission electron microscopy (TEM) images, which showed that the synthesized magnetite-incorporated chitosan was nanosized. The superior application of such a material to offset the deterioration of the environment caused by insecticides is attained through a photocatalytic reaction. The experimental results verified the function of magnetite-incorporated chitosan, since it increased the composite-specific surface area, resulting in high methomyl molecule oxidation. Methomyl oxidation reached almost complete insecticide removal (99%) within only one hour of irradiance time. The optimal operational conditions were investigated, and the maximal removal rate occurred when the aqueous solution was at an acidic pH of 3.0. The reaction was affected by differing hydrogen peroxide and catalyst doses, and the optimized reagent was recorded at the levels of 40 and 400 mg/L of catalyst and hydrogen peroxide, respectively. Also, catalyst reusability was attained, confirming its sustainability, since it could be used for successive cycles. From the current investigation, it is proposed that magnetite–chitosan nanoparticles could serve as a promising photocatalyst for the elimination of insecticides from wastewater in a green manner. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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14 pages, 2613 KiB

Open AccessArticle

Sodium Salt of Partially Carboxymethylated Sodium Alginate-g-Poly(acrylonitrile): I. Photo-Induced Synthesis, Characterization, and Alkaline Hydrolysis

by Jignesh Trivedi and Arvind Chourasia

Gels 2023, 9(5), 410; https://doi.org/10.3390/gels9050410 - 15 May 2023

Cited by 3 | Viewed by 1425

Abstract

An efficient redox initiating system, ceric ammonium nitrate/nitric acid, has been employed for the first time to carry out photo-induced graft copolymerization of acrylonitrile (AN) onto sodium salt of partially carboxymethylated sodium alginate, having an average degree of substitution value to be 1.10. The photo-grafting reaction conditions for maximum grafting have been systematically optimized by varying the reaction variables such as reaction time, temperature, the concentration of acrylonitrile monomer, ceric ammonium nitrate, and nitric acid, as well as the amount of the backbone. The optimum reaction conditions are obtained with a reaction time of 4 h, reaction temperature of 30 °C, acrylonitrile monomer concentration of 0.152 mol/L, initiator concentration of 5 × 10⁻³ mol/L, nitric acid concentration of 0.20 mol/L, amount of backbone of 0.20 (dry basis) and the total volume of the reaction system of 150 mL. The highest percentage of grafting (%G) and grafting efficiency (%GE) achieved are 316.53% and 99.31%, respectively. The optimally prepared graft copolymer, sodium salt of partially carboxymethylated sodium alginate-g-polyacrylonitrile (%G = 316.53), has been hydrolyzed in an alkaline medium (0.7N NaOH, 90–95 °C for ~2.5 h) to obtain the superabsorbent hydrogel, H–Na–PCMSA–g–PAN. The chemical structure, thermal characteristics, and morphology of the products have also been studied. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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17 pages, 8083 KiB

Open AccessArticle

Sodium Salt of Partially Carboxymethylated Sodium Alginate-Graft-Poly(Acrylonitrile): II Superabsorbency, Salt Sensitivity and Swelling Kinetics of Hydrogel, H-Na-PCMSA-g-PAN

by Jignesh Trivedi and Arvind Chourasia

Gels 2023, 9(5), 407; https://doi.org/10.3390/gels9050407 - 12 May 2023

Cited by 8 | Viewed by 1566

Abstract

The water absorption measurements of a novel superabsorbent anionic hydrogel, H-Na-PCMSA-g-PAN, has been reported first time in water with a poor conductivity, 0.15 M saline (NaCl, CaCl_2, and AlCl₃) solutions, and simulated urine (SU) solutions at various times. The hydrogel has been prepared by the saponification of the graft copolymer, Na-PCMSA-g-PAN (%G = 316.53, %GE = 99.31). Results indicated that as compared to the swelling capacity values evaluated in water with a poor conductivity, the ability of the hydrogel to swell in various saline solutions with the same concentration is significantly reduced at all different durations. The swelling tends to be Na⁺ > Ca²⁺ > Al³⁺ at the same saline concentration in the solution. Studies of the absorbency in various aqueous saline (NaCl) solutions also revealed that the swelling capacity decreased as the ionic strength of the swelling medium rose, which is consistent with the experimental results and Flory’s equation. Furthermore, the experimental results strongly suggested that second-order kinetics governs the swelling process of the hydrogel in various swelling media. The swelling characteristics and equilibrium water contents for the hydrogel in various swelling media have also been researched. The hydrogel samples have been successfully characterized by FTIR to show the change in chemical environment to COO⁻ and CONH₂ groups after swelling in different swelling media. The samples have also been characterized by SEM technique. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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14 pages, 2473 KiB

Open AccessArticle

Effects of Alkaline Solvent Type and pH on Solid Physical Properties of Carrageenan from Eucheuma cottonii

by Rival Ferdiansyah, Marline Abdassah, Achmad Zainuddin, Revika Rachmaniar and Anis Yohana Chaerunisaa

Gels 2023, 9(5), 397; https://doi.org/10.3390/gels9050397 - 10 May 2023

Cited by 8 | Viewed by 2616

Abstract

The effects of alkali type and pH on the physical properties of carrageenan have been extensively studied. However, their effects on certain characteristics of solid-state properties of carrageenan have not been identified. This research aimed to investigate the effect of alkaline solvent type and pH on the solid physical properties of carrageenan isolated from Eucheuma cottonii. Carrageenan was extracted from the algae using NaOH, KOH, and Ca(OH)₂ at pHs of 9, 11, and 13. Based on the results of preliminary characterization, including yield, ash content, pH, sulphate content, viscosity, and gel strength, it was found that all samples followed Food and Agriculture Organization (FAO) specifications. The swelling capacity of carrageenan based on the type of alkali was KOH > NaOH > Ca(OH)₂. The FTIR spectra of all samples were in agreement with that of standard carrageenan. The molecular weight (MW) of carrageenan using KOH as the alkali followed the order pH 13 > pH 9 > pH 11, while using NaOH, the order was pH 9 > pH 13 > pH 11, and while using Ca(OH)₂, the order was pH 13 > pH 9 > pH 11. The results of the solid-state physical characterization of carrageenan with the highest MW in each type of alkali showed that the morphology of carrageenan using Ca(OH)₂ has a cubic shape and is more crystal-like. The order of crystallinity of carrageenan using different types of alkali was Ca(OH)₂ (14.44%) > NaOH (9.80%) > KOH (7.91%), while the order of density was Ca(OH)₂ > KOH > NaOH. The order of solid fraction (SF) of the carrageenan was KOH > Ca(OH)₂ > NaOH, while the tensile strength when using KOH was 1.17, when using NaOH it was 0.08, and while using Ca(OH)₂, it was 0.05. The bonding index (BI) of carrageenan using KOH = 0.04, NaOH = 0.02, and Ca(OH)₂ = 0.02. The brittle fracture index (BFI) of the carrageenan was KOH = 0.67, NaOH = 0.26, and Ca(OH)₂ = 0.04. The order of carrageenan solubility in water was NaOH > KOH > Ca(OH)₂. These data can be used as the basis for the development of carrageenan for excipients in solid dosage forms. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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24 pages, 5622 KiB

Open AccessArticle

Study of Hydroxypropyl β-Cyclodextrin and Puerarin Inclusion Complexes Encapsulated in Sodium Alginate-Grafted 2-Acrylamido-2-Methyl-1-Propane Sulfonic Acid Hydrogels for Oral Controlled Drug Delivery

by Abid Naeem, Chengqun Yu, Weifeng Zhu, Zhenzhong Zang and Yongmei Guan

Gels 2023, 9(3), 246; https://doi.org/10.3390/gels9030246 - 20 Mar 2023

Cited by 6 | Viewed by 2641

Abstract

Puerarin has been reported to have anti-inflammatory, antioxidant, immunity enhancement, neuroprotective, cardioprotective, antitumor, and antimicrobial effects. However, due to its poor pharmacokinetic profile (low oral bioavailability, rapid systemic clearance, and short half-life) and physicochemical properties (e.g., low aqueous solubility and poor stability) its therapeutic efficacy is limited. The hydrophobic nature of puerarin makes it difficult to load into hydrogels. Hence, hydroxypropyl-β-cyclodextrin (HP-βCD)-puerarin inclusion complexes (PIC) were first prepared to enhance solubility and stability; then, they were incorporated into sodium alginate-grafted 2-acrylamido-2-methyl-1-propane sulfonic acid (SA-g-AMPS) hydrogels for controlled drug release in order to increase bioavailability. The puerarin inclusion complexes and hydrogels were evaluated via FTIR, TGA, SEM, XRD, and DSC. Swelling ratio and drug release were both highest at pH 1.2 (36.38% swelling ratio and 86.17% drug release) versus pH 7.4 (27.50% swelling ratio and 73.25% drug release) after 48 h. The hydrogels exhibited high porosity (85%) and biodegradability (10% in 1 week in phosphate buffer saline). In addition, the in vitro antioxidative activity (DPPH (71%), ABTS (75%), and antibacterial activity (Staphylococcus aureus, Escherichia coli, and Pseudomonas aeruginosa) indicated the puerarin inclusion complex-loaded hydrogels had antioxidative and antibacterial capabilities. This study provides a basis for the successful encapsulation of hydrophobic drugs inside hydrogels for controlled drug release and other purposes. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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14 pages, 3359 KiB

Open AccessArticle

An Eco-Friendly Antheraea Pernyi Silk Gland Protein/Sodium Alginate Multiple Network Hydrogel as Potential Drug Release Systems

by Jia Li, Bo-Xiang Wang, De-Hong Cheng, Yue Zhang, Qiang Yao, Xin-bin Ji, Jing Guo and Yan-Hua Lu

Gels 2023, 9(1), 4; https://doi.org/10.3390/gels9010004 - 22 Dec 2022

Cited by 3 | Viewed by 1865

Abstract

To improve the versatility of the sodium alginate-loaded bio-hydrogels, Antheraea pernyi silk gland protein/sodium alginate drug-loaded hydrogels were prepared by using an eco-friendly multiple network cross-link technology. Fourier transform infrared (FT-IR) spectroscopy and UV-Vis spectrophotometer were used separately to evaluate the chemical structure and drug release behavior of drug-loaded hydrogels. The antibacterial drug carrier gels were evaluated by using inhibition zone test against the S. aureus and E. coli. The CCK-8 assay was used to assess the biocompatibility of drug loaded hydrogels. The FT-IR results showed that there was a strong interaction within the drug loaded hydrogels, and the ASGP was beneficial to enhance the interaction within the drug loaded hydrogels. UV-Vis spectrophotometer results indicated the cumulative release reached 80% within 400 min. Antibacterial bio-hydrogels had a good antibacterial property, especially the antibacterial bio-hydrogels with bacitracin exhibits superior to other antibacterial agents. The drug-loaded bio-hydrogels exhibited the adhesion and proliferation of RSC96 cells and perfected biocompatibility. This provides a new idea for further research and development of tissue-friendly drug-loaded biomaterials. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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Review

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21 pages, 4284 KiB

Open AccessReview

Nanostructured Bioaerogels as a Potential Solution for Particulate Matter Pollution

by Wafa Mustafa Saleh, Mardiana Idayu Ahmad, Esam Bashir Yahya and Abdul Khalil H.P.S.

Gels 2023, 9(7), 575; https://doi.org/10.3390/gels9070575 - 14 Jul 2023

Cited by 4 | Viewed by 2355

Abstract

Particulate matter (PM) pollution is a significant environmental and public health issue globally. Exposure to high levels of PM, especially fine particles, can have severe health consequences. These particles can come from a variety of sources, including natural events like dust storms and wildfires, as well as human activities such as industrial processes and transportation. Although an extensive development in air filtration techniques has been made in the past few years, fine particulate matter still poses a serios and dangerous threat to human health and to our environment. Conventional air filters are fabricated from non-biodegradable and non-ecofriendly materials which can cause further environmental pollution as a result of their excessive use. Nanostructured biopolymer aerogels have shown great promise in the field of particulate matter removal. Their unique properties, renewable nature, and potential for customization make them attractive materials for air pollution control. In the present review, we discuss the meaning, properties, and advantages of nanostructured aerogels and their potential in particulate matter removal. Particulate matter pollution, types and sources of particulate matter, health effect, environmental effect, and the challenges facing scientists in particulate matter removal are also discussed in the present review. Finally, we present the most recent advances in using nanostructured bioaerogels in the removal of different types of particulate matter and discuss the challenges that we face in these applications. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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26 pages, 36467 KiB

Open AccessReview

Recent Advances in Nanocellulose Aerogels for Efficient Heavy Metal and Dye Removal

by Azfaralariff Ahmad, Mohamad Anuar Kamaruddin, Abdul Khalil H.P.S., Esam Bashir Yahya, Syaifullah Muhammad, Samsul Rizal, Mardiana Idayu Ahmad, Indra Surya and C. K. Abdullah

Gels 2023, 9(5), 416; https://doi.org/10.3390/gels9050416 - 16 May 2023

Cited by 26 | Viewed by 3621

Abstract

Water pollution is a significant environmental issue that has emerged because of industrial and economic growth. Human activities such as industrial, agricultural, and technological practices have increased the levels of pollutants in the environment, causing harm to both the environment and public health. Dyes and heavy metals are major contributors to water pollution. Organic dyes are a major concern because of their stability in water and their potential to absorb sunlight, increasing the temperature and disrupting the ecological balance. The presence of heavy metals in the production of textile dyes adds to the toxicity of the wastewater. Heavy metals are a global issue that can harm both human health and the environment and are mainly caused by urbanization and industrialization. To address this issue, researchers have focused on developing effective water treatment procedures, including adsorption, precipitation, and filtration. Among these methods, adsorption is a simple, efficient, and cheap method for removing organic dyes from water. Aerogels have shown potential as a promising adsorbent material because of their low density, high porosity, high surface area, low thermal and electrical conductivity, and ability to respond to external stimuli. Biomaterials such as cellulose, starch, chitosan, chitin, carrageenan, and graphene have been extensively studied for the production of sustainable aerogels for water treatment. Cellulose, which is abundant in nature, has received significant attention in recent years. This review highlights the potential of cellulose-based aerogels as a sustainable and efficient material for removing dyes and heavy metals from water during the treatment process. Full article

(This article belongs to the Special Issue Marine Biopolymers-Based Hydrogels, Xerogels and Aerogels: Preparation and Applications)

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