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Cellulose-Based Gels: Synthesis, Properties, and Applications
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Cellulose-Based Gels: Synthesis, Properties, and Applications

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

Deadline for manuscript submissions: closed (30 April 2025) | Viewed by 8842

Special Issue Editors

Dr. Alessandro Torchio

E-Mail Website
Guest Editor
Department of Mechanical and Aerospace Engineering, Politecnico di Torino, 10129 Torino, Italy
Interests: hydrogels; supramolecular hydrogels; cyclodextrins; drug delivery; tissue engineering
Dr. Monica Boffito

E-Mail Website
Guest Editor
Department of Mechanical and Aerospace Engineering, Politecnico di Torino, 10129 Torino, Italy
Interests: hydrogels; physical and chemical hydrogels; drug delivery; tissue engineering; polymer synthesis; polymeric scaffolds
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Cellulose-based gels offer exceptional advantages, including biocompatibility, biodegradability, and sustainability. Such features make them promising candidates for diverse applications, ranging from medicine (e.g., tissue engineering and drug delivery) to material science and engineering (e.g., environmental science). These gels can be designed using various chemical and physical crosslinking strategies involving cellulose and its derivatives, possibly other blended polymers or composite systems. The resulting cellulose-based gels exhibit a wide spectrum of properties, including tunable mechanical strength, swelling behavior, and responsiveness to environmental stimuli.

This Special Issue aims to highlight the latest research and innovations in cellulose-based gels, and invites researchers from around the globe to submit their original research articles, reviews, as well as case studies. Topics of interest include novel synthesis techniques, characterization of structural and mechanical properties, exploration of unique functionalities, and investigations into their applications in drug delivery, tissue engineering (e.g., 3D bioprinting), food science, and beyond.

We look forward to receiving your contributions which will irrefutably foster collaboration and knowledge exchange in this rapidly evolving field.

Dr. Alessandro Torchio
Dr. Monica Boffito
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Gels is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2100 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • cellulose
  • cellulose-based gels
  • cellulose derivatives
  • physico-chemical characterization
  • biomedical applications
  • drug delivery
  • tissue engineering
  • 3D bioprinting
  • environmental science
  • food science
  • cellulose synthesis

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Related Special Issue

Published Papers (7 papers)

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Research

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22 pages, 5233 KiB  
Article
A Novel Green In Situ Amine-Functionalized Aerogel UiO-66-NH2/TOCNF for the Removal of Azo Anionic Dyes
by Rabia Amen, Islam Elsayed, Yunsang Kim, Gregory T. Schueneman, Emad M. El-Giar and El Barbary Hassan
Gels 2025, 11(5), 365; https://doi.org/10.3390/gels11050365 - 15 May 2025
Viewed by 255
Abstract
UiO-66-NH2 is a metal–organic framework (MOF) with open metal sites, making it a promising candidate for adsorption and catalysis. However, the powdery texture of MOFs and the use of toxic solvents during synthesis limit their application. A novel solution to this issue [...] Read more.
UiO-66-NH2 is a metal–organic framework (MOF) with open metal sites, making it a promising candidate for adsorption and catalysis. However, the powdery texture of MOFs and the use of toxic solvents during synthesis limit their application. A novel solution to this issue is to create a layered porous composite by encasing the MOF within a flexible and structurally robust aerogel substrate using safe, eco-friendly, and green solvents such as ethanol. The fibrous MOF aerogels, characterized by a desirable macroscopic shape of cylindrical block and hierarchical porosity, were synthesized by two approaches: in situ growth of amine-functionalized UiO-66-NH2 crystals on a TEMPO-oxidized cellulose nanofiber (TOCNF) and ex situ crosslinking of UiO-66-NH2 crystals onto a TOCNF network to form UiO-66-NH2/TOCNF. The incorporation of MOF into the cellulose nanofibrils via the in situ method reduces their aggregation potential, alters the nucleation/growth balance to produce smaller MOF crystals, and enhances mechanical flexibility, as evidenced by SEM images. The three adsorbents, including UiO-66-NH2, ex situ UiO-66-NH2/TOCNF, and in situ UiO-66-NH2/TOCNF, were synthesized and used in this study. The effects of pH, time, temperature, and initial concentration were studied. A maximum adsorption capacity (Qmax) of 549.45 mg/g for Congo Red (CR) and 171.23 mg/g for Orange II (ORII) was observed at pH 6, using 10 mg of in situ UiO-66-NH2/TOCNF at 40 °C with a contact time of 75 min for CR and 2 h for ORII. The adsorption of both dyes primarily occurs through monolayer chemisorption on the in situ UiO-66-NH2/TOCNF. The main removal mechanisms were hydrogen bonding and surface complexation. The noteworthy adsorption capacity of in situ UiO-66-NH2/TOCNF coupled with environment-friendly fabrication techniques indicates its potential applications on a large scale in real wastewater systems. Full article
(This article belongs to the Special Issue Cellulose-Based Gels: Synthesis, Properties, and Applications)
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16 pages, 4034 KiB  
Article
Ibuprofen-Loaded, Nanocellulose-Based Buccal Films: The Development and Evaluation of Promising Drug Delivery Systems for Special Populations
by Katarina Bolko Seljak, Blaž Grilc, Mirjana Gašperlin and Mirjam Gosenca Matjaž
Gels 2025, 11(3), 163; https://doi.org/10.3390/gels11030163 - 24 Feb 2025
Viewed by 446
Abstract
The objective of this work was to investigate the use of nanocrystalline cellulose (NCC) as a drug-delivery excipient for buccal films. Gel-like dispersions were created by blending either gel or powder NCC (gNCC or pNCC) with natural polymers (alginate, pectin, or chitosan) in [...] Read more.
The objective of this work was to investigate the use of nanocrystalline cellulose (NCC) as a drug-delivery excipient for buccal films. Gel-like dispersions were created by blending either gel or powder NCC (gNCC or pNCC) with natural polymers (alginate, pectin, or chitosan) in water, with glycerol serving as a plasticiser. Ibuprofen (IBU) as an active pharmaceutical ingredient (API) was dissolved in a self-microemulsifying drug delivery system (SMEDDS) to improve its solubility prior to its addition to gel-like dispersions. Dispersions were dried, and resulting films were cut to 3 cm × 1.5 cm size, appropriate for buccal delivery. Rheological measurements revealed that shorter, thinner, and less crystalline nanocellulose fibres are more favourable for stronger gel properties. While overall, weaker gel structure prior to film casting also resulted in shorter disintegration time, this was not the case for NCC–chitosan films; here, the low solubility of chitosan in neutral media proved to be the main obstacle. Nevertheless, the prolonged disintegration of NCC–chitosan films did not impact the dissolution of IBU, as these films exhibited the fastest dissolution rate, followed by NCC–pectin and NCC–alginate. Furthermore, NCC properties significantly influenced the dissolution behaviour of the chitosan formulations, with gNCC favouring faster IBU release due to weaker gel formation prior to film casting. Full article
(This article belongs to the Special Issue Cellulose-Based Gels: Synthesis, Properties, and Applications)
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18 pages, 5766 KiB  
Article
Physicochemical Characterization and Antioxidant Properties of Cellulose-Rich Extracts Obtained from Carob (Ceratonia siliqua L.) Pulp for Preparation of Cellulose-Rich Gels
by Bernat Llompart, Esperanza Dalmau, Mónica Umaña and Antoni Femenia
Gels 2025, 11(2), 145; https://doi.org/10.3390/gels11020145 - 18 Feb 2025
Viewed by 550
Abstract
The carob tree (Ceratonia siliqua L.) is a defining species of the Mediterranean region, and its fruit, the carob pod, has seen a notable increase in economic interest in recent years, primarily due to the production of locust bean gum (E410), a [...] Read more.
The carob tree (Ceratonia siliqua L.) is a defining species of the Mediterranean region, and its fruit, the carob pod, has seen a notable increase in economic interest in recent years, primarily due to the production of locust bean gum (E410), a widely used food additive derived from the seeds. The remainder of the fruit, the carob pulp, comprises 80–90% of the fruit’s weight and is typically considered a by-product, with its primary application being in animal feed. This study focused on obtaining cellulose-rich extracts from selected carob varieties cultivated in the Mediterranean region. A comprehensive physicochemical characterization of these cellulose-rich fractions was conducted, including the assessment of their antioxidant properties, specifically total phenolics and antioxidant capacity measured by the FRAP, ABTS, and CUPRAC methods. The findings reveal that carob pulp is an excellent source of carbohydrates, including soluble sugars, which constitute 33–45% of the pulp’s fresh weight, depending on the variety, and cell wall polysaccharides. The cell wall polymers, with cellulose as the predominant component, account for approximately 45% of the fresh pulp weight. Notable amounts of other polysaccharides, such as pectins and hemicelluloses, were also identified. Among the studied varieties, Bugadera and Rotjal stood out as exceptional sources of cellulose-rich extracts. Carob pulp was also found to be rich in antioxidant compounds, reflected in its high antioxidant capacity. In particular, the Bugadera variety, grown under irrigated conditions, exhibited a significant concentration of phenolic compounds (24.4 mg gallic acid equivalents per gram of pulp) and high antioxidant activity across all methods used, with ABTS measurements reaching up to 391.5 mg Trolox equivalents per gram of pulp. In conclusion, these results underscore the significant potential of carob pulp as a source of valuable cellulose-rich extracts, offering applications beyond its traditional use as animal feed. By exploring these new possibilities, the economic and environmental sustainability of carob cultivation could be greatly enhanced, contributing to the broader valorization of this iconic Mediterranean fruit. Full article
(This article belongs to the Special Issue Cellulose-Based Gels: Synthesis, Properties, and Applications)
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18 pages, 4984 KiB  
Article
Development of Extrudable Hydrogels Based on Carboxymethyl Cellulose–Gelatin Complex Coacervates
by Hamid Gharanjig, Hossein Najaf Zadeh, Campbell Stevens, Pram Abhayawardhana, Tim Huber and Ali Reza Nazmi
Gels 2025, 11(1), 51; https://doi.org/10.3390/gels11010051 - 8 Jan 2025
Viewed by 1202
Abstract
This study investigates the 3D extrusion printing of a carboxymethyl cellulose (CMC)–gelatin complex coacervate system. Various CMC–gelatin coacervate hydrogels were prepared and analyzed to achieve this goal. The impact of the CMC–gelatin ratio, pH, and total biopolymer concentration on coacervation formation and rheological [...] Read more.
This study investigates the 3D extrusion printing of a carboxymethyl cellulose (CMC)–gelatin complex coacervate system. Various CMC–gelatin coacervate hydrogels were prepared and analyzed to achieve this goal. The impact of the CMC–gelatin ratio, pH, and total biopolymer concentration on coacervation formation and rheological properties was evaluated to characterize the printability of the samples. Turbidity results indicated that the molecular interactions between gelatin and CMC biopolymers are significantly pH-dependent, occurring within the range of pH 3.7 to pH 5.6 for the tested compositions. Confocal Laser Scanning Microscopy (CLSM) confirmed the presence of coacervates as spherical particles within the optimal coacervation range. Scanning electron microscopy micrographs supported the CLSM findings, revealing greater porosity within this optimal pH range. Rheological characterization demonstrated that all CMC–gelatin hydrogels exhibited pseudoplastic behavior, with an inverse correlation between increased coacervation and decreased shear viscosity. Additionally, the coacervates displayed lower tackiness compared to gelatin hydrogels, with the maximum tackiness normal force for various CMC–gelatin ratios ranging from 1 to 15 N, notably lower than the 29 N observed for gelatin hydrogels. Mixtures with CMC–gelatin ratios of 1:15 and 1:20 exhibited the best shear recovery behavior, maintaining higher strength after shear load. The maximum strength of the CMC–gelatin coacervate system was found at a biopolymer concentration of 6%. However, lower biopolymer content allowed for consistent extrusion. Importantly, all tested samples were successfully extruded at 22 ± 2 °C, with the 1:15 biopolymer ratio yielding the most consistent printed quality. Our research highlights the promise of the CMC–gelatin coacervate system for 3D printing applications, particularly in areas that demand precise material deposition and adjustable properties. Full article
(This article belongs to the Special Issue Cellulose-Based Gels: Synthesis, Properties, and Applications)
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17 pages, 11736 KiB  
Article
3D Printing of New Foods Using Cellulose-Based Gels Obtained from Cerotonia siliqua L. Byproducts
by Antoni Capellà, Mónica Umaña, Esperanza Dalmau, Juan A. Cárcel and Antoni Femenia
Gels 2024, 10(12), 759; https://doi.org/10.3390/gels10120759 - 23 Nov 2024
Viewed by 939
Abstract
Carob pulp is a valuable source of cellulose-rich fraction (CRF) for many food applications. This study aimed to obtain and characterize a CRF derived from carob pulp waste after sugar removal and to evaluate its potential use in the 3D printing of cellulose-rich [...] Read more.
Carob pulp is a valuable source of cellulose-rich fraction (CRF) for many food applications. This study aimed to obtain and characterize a CRF derived from carob pulp waste after sugar removal and to evaluate its potential use in the 3D printing of cellulose-rich foods. Thus, the extraction of the CRF present in carob pulp (by obtaining the alcohol-insoluble residue) was carried out, accounting for nearly 45% dm (dry matter) of this byproduct. The CRF contained about 24% dm of cellulose. The functional properties (swelling capacity, water retention, and fat adsorption) related to this fraction were determined, showing a value of 5.9 mL/g of CRF and 4.0 and 6.5 g/g of CRF, respectively. Different gels were formulated with a total solids content of 15% wm (wet matter), using potato peel flour as a base and partially substituting with CRF (0% to 8% wm). The cellulose-based gels were characterized in terms of viscosity, water distribution (low-field Nuclear Magnetic Resonance), and printability, while the 3D printed samples were assessed for their textural properties. As the percentage of added CRF increased, the viscosity decreased while the water retention increased. Printability improved when small proportions of CRF (2% to 4%) were used, while it deteriorated for higher percentages (6% to 8%). The textural properties (hardness, adhesiveness, cohesiveness, and gumminess) showed significant changes caused by the addition of CRF, with gels containing 3% to 4% CRF exhibiting the most suitable printing values. In summary, this study demonstrates the significant potential of carob cellulose-based gel as an ingredient in the 3D printing of novel fiber-rich foods, contributing to reducing food waste and promoting sustainable practices within the framework of the circular economy. Full article
(This article belongs to the Special Issue Cellulose-Based Gels: Synthesis, Properties, and Applications)
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14 pages, 3603 KiB  
Article
Xyloglucan–Cellulose Nanocrystals Mixtures: A Case Study of Nanocolloidal Hydrogels and Levers for Tuning Functional Properties
by Géraldine Rangel, Céline Moreau, Ana Villares, Christophe Chassenieux and Bernard Cathala
Gels 2024, 10(5), 334; https://doi.org/10.3390/gels10050334 - 15 May 2024
Viewed by 1417
Abstract
The development of fully biobased hydrogels obtained by simple routes and in the absence of toxic or environmentally harmful reagents is a major challenge in meeting new societal demands. In this work, we discuss the development of hydrogels made from cellulose nanocrystals (CNCs) [...] Read more.
The development of fully biobased hydrogels obtained by simple routes and in the absence of toxic or environmentally harmful reagents is a major challenge in meeting new societal demands. In this work, we discuss the development of hydrogels made from cellulose nanocrystals (CNCs) and xyloglucan (XG), two non-toxic, renewable, and biobased components. We present three strategies to fine-tune the functional properties. The first one consists in varying the XG/CNC ratio that leads to the modulation of the mechanical properties of hydrogels as well as a better comprehension of the gel mechanism formation. The second relies on tuning the XG chains’ interaction by enzymatic modification to achieve thermoresponsive systems. Finally, the third one is based on the increase in the hydrogel solid content by osmotic concentration. The high-solid-content gels were found to have very high mechanical properties and self-healing properties that can be used for molding materials. Overall, these approaches are a case study of potential modifications and properties offered by biobased nanocolloidal hydrogels. Full article
(This article belongs to the Special Issue Cellulose-Based Gels: Synthesis, Properties, and Applications)
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Review

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27 pages, 1421 KiB  
Review
Advances in Cellulose-Based Hydrogels: Current Trends and Challenges
by Bogdan-Marian Tofanica, Aleksandra Mikhailidi, Costel Samuil, Ovidiu C. Ungureanu, Maria E. Fortună and Elena Ungureanu
Gels 2024, 10(12), 842; https://doi.org/10.3390/gels10120842 - 20 Dec 2024
Cited by 2 | Viewed by 3074
Abstract
This paper provides a solid foundation for understanding the synthesis, properties, and applications of cellulose-based gels. It effectively showcases the potential of these gels in diverse applications, particularly in biomedicine, and highlights key synthesis methods and properties. However, to push the field forward, [...] Read more.
This paper provides a solid foundation for understanding the synthesis, properties, and applications of cellulose-based gels. It effectively showcases the potential of these gels in diverse applications, particularly in biomedicine, and highlights key synthesis methods and properties. However, to push the field forward, future research should address the gaps in understanding the environmental impact, mechanical stability, and scalability of cellulose-based gels, while also considering how to overcome barriers to their industrial use. This will ultimately allow for the realization of cellulose-based gels in large-scale, sustainable applications. Full article
(This article belongs to the Special Issue Cellulose-Based Gels: Synthesis, Properties, and Applications)
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