Advances in Cellulose-Based Hydrogels

A special issue of Gels (ISSN 2310-2861).

Deadline for manuscript submissions: closed (15 May 2022) | Viewed by 59282

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Guest Editor
Department of Engineering for Innovation, University of Salento, Via per Monteroni, 73100 Lecce, Italy
Interests: biomaterials; scaffold; tissue engineering; material characterization; viscoelasticity; hydrogels; green chemistry; natural polymers
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Guest Editor
Department of Civil Engineering and Architecture (DICAr), Università degli Studi di Pavia, 27100 Pavia, Italy
Interests: hydrogels; gels; natural polymers; biopolymers; biomaterials; responsive polymers; smart polymers; cellulose; cellulose derivatives; materials characterization; rheology; scaffold; biomedical; tissue engineering; regenerative medicine
Special Issues, Collections and Topics in MDPI journals
Department of Chemistry, Materials and Chemical Engineering “G. Natta”, Politecnico di Milano, 20131 Milano, Italy
Interests: cellulose nanofibers; biopolymers; aerogels; advanced cellulose-based systems; applied chemistry
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Cellulose is the most abundant natural biopolymer on Earth. With an estimated annual production of ~1.5 x 1012 tons globally, and the possibility of its extraction even from waste sources, it is considered an almost inexhaustible source of raw material capable to make up for the growing demand for environmentally friendly and biocompatible products.

Within this framework, cellulose-based hydrogels usually combine hydrophilicity, biodegradability, non-toxicity, and biocompatibility together with low costs and massive availability, which make them extremely attractive in both academic and industrial fields. Possible application fields include biomedical engineering (e.g., tissue engineering and regenerative medicine, drug/cell delivery systems, and 3D printing and bioprinting), progress in smart systems (e.g., sensors, actuators, and soft robotics) and stimuli-responsive systems (e.g., pH- or thermo-responsive hydrogels), the agricultural sector (e.g., soil conditioning, nutrient carriers, and water reservoirs), and water purification.

This Special Issue is aimed at collecting the recent progress in cellulose-based hydrogels, including gels prepared from natural cellulose and its derivatives, cellulose graft co-polymers, and composite gels based on cellulose. We encourage submissions covering key aspects of cellulose-based hydrogels, including design, characterization, as well as application-focused research.

As Guest Editors, we would kindly invite you to contribute a research paper or a review on any topic related to this thread.

Dr. Christian Demitri
Dr. Lorenzo Bonetti
Dr. Laura Riva
Guest Editors

Manuscript Submission Information

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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
  • nanocellulose
  • cellulose derivatives
  • cellulose-based composites
  • hydrogels
  • design
  • characterization
  • applications

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Published Papers (16 papers)

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Editorial

Jump to: Research, Review

3 pages, 204 KiB  
Editorial
Editorial on the Special Issue “Advances in Cellulose-Based Hydrogels”
by Lorenzo Bonetti, Christian Demitri and Laura Riva
Gels 2022, 8(12), 790; https://doi.org/10.3390/gels8120790 - 2 Dec 2022
Cited by 3 | Viewed by 1198
Abstract
Cellulose is one of the most ubiquitous and naturally abundant biopolymers found on Earth and is primarily obtained from plants and other biomass sources [...] Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)

Research

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26 pages, 6727 KiB  
Article
Biocompatible Self-Assembled Hydrogen-Bonded Gels Based on Natural Deep Eutectic Solvents and Hydroxypropyl Cellulose with Strong Antimicrobial Activity
by Daniela Filip, Doina Macocinschi, Mihaela Balan-Porcarasu, Cristian-Dragos Varganici, Raluca-Petronela Dumitriu, Dragos Peptanariu, Cristina Gabriela Tuchilus and Mirela-Fernanda Zaltariov
Gels 2022, 8(10), 666; https://doi.org/10.3390/gels8100666 - 17 Oct 2022
Cited by 6 | Viewed by 2690
Abstract
Natural deep eutectic solvents (NADES)-hydroxypropyl cellulose (HPC) self-assembled gels with potential for pharmaceutical applications are prepared. FT-IR, 1HNMR, DSC, TGA and rheology measurements revealed that hydrogen bond acceptor–hydrogen bond donor interactions, concentration of NADES and the water content influence significantly the physico-chemical [...] Read more.
Natural deep eutectic solvents (NADES)-hydroxypropyl cellulose (HPC) self-assembled gels with potential for pharmaceutical applications are prepared. FT-IR, 1HNMR, DSC, TGA and rheology measurements revealed that hydrogen bond acceptor–hydrogen bond donor interactions, concentration of NADES and the water content influence significantly the physico-chemical characteristics of the studied gel systems. HPC-NADES gel compositions have thermal stabilities lower than HPC and higher than NADES components. Thermal transitions reveal multiple glass transitions characteristic of phase separated systems. Flow curves evidence shear thinning (pseudoplastic) behavior. The flow curve shear stress vs. shear rate were assessed by applying Bingham, Herschel–Bulkley, Vocadlo and Casson rheological models. The proposed correlations are in good agreement with experimental data. The studied gels evidence thermothickening behavior due to characteristic LCST (lower critical solution temperature) behavior of HPC in aqueous systems and a good biocompatibility with normal cells (human gingival fibroblasts). The order of antibacterial and antifungal activities (S.aureus, E.coli, P. aeruginosa and C. albicans) is as follows: citric acid >lactic acid > urea > glycerol, revealing the higher antibacterial and antifungal activities of acids. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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24 pages, 9704 KiB  
Article
Cellulose-g-poly(2-(dimethylamino)ethylmethacrylate) Hydrogels: Synthesis, Characterization, Antibacterial Testing and Polymer Electrolyte Application
by Roko Blažic, Dajana Kučić Grgić, Marijana Kraljić Roković and Elvira Vidović
Gels 2022, 8(10), 636; https://doi.org/10.3390/gels8100636 - 7 Oct 2022
Cited by 13 | Viewed by 2105
Abstract
Hydrogels have been investigated due to their unique properties. These include high water content and biocompatibility. Here, hydrogels with different ratios of poly(2-(dimethylamino)ethylmethacrylate) (PDMAEMA) were grafted onto cellulose (Cel-g-PDMAEMA) by the free radical polymerization method and gamma-ray radiation was applied in [...] Read more.
Hydrogels have been investigated due to their unique properties. These include high water content and biocompatibility. Here, hydrogels with different ratios of poly(2-(dimethylamino)ethylmethacrylate) (PDMAEMA) were grafted onto cellulose (Cel-g-PDMAEMA) by the free radical polymerization method and gamma-ray radiation was applied in order to increase crosslinking and content of PDMAEMA. Gamma irradiation enabled an increase of PDMAEMA content in hydrogels in case of higher ratio of 2-(dimethylamino)ethyl methacrylate in the initial reaction mixture. The swelling of synthesized hydrogels was monitored in dependence of pH (3, 5.5 and 10) during up to 60 days. The swelling increased from 270% to 900%. Testing of antimicrobial activity of selected hydrogel films showed weak inhibitory activity against Escherichia coli, Pseudomonas aeruginosa, and Bacillus subtilis. The results obtained by the cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) indicate that chemically synthesized hydrogels have good characteristics for the supercapacitor application. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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9 pages, 7110 KiB  
Article
Use of Carbotrace 480 as a Probe for Cellulose and Hydrogel Formation from Defibrillated Microalgae
by Frederik L. Zitzmann, Ewan Ward and Avtar S. Matharu
Gels 2022, 8(6), 383; https://doi.org/10.3390/gels8060383 - 16 Jun 2022
Cited by 2 | Viewed by 2467
Abstract
Carbotrace 480 is a commercially available fluorescent optotracer that specifically binds to cellulose’s glycosidic linkages. Herein, the use of Carbotrace 480 is reported as an analytical tool for linking cellulose content to hydrogel formation capability in defibrillated celluloses obtained from proprietary microalgae. Defibrillated [...] Read more.
Carbotrace 480 is a commercially available fluorescent optotracer that specifically binds to cellulose’s glycosidic linkages. Herein, the use of Carbotrace 480 is reported as an analytical tool for linking cellulose content to hydrogel formation capability in defibrillated celluloses obtained from proprietary microalgae. Defibrillated celluloses obtained from acid-free hydrothermal microwave processing at low temperature (160 °C) showed poor hydrogel formation attributed to a low cellulose concentration as evidenced through the lack of Carbotrace fluorescence. High temperature (220 °C) processing afforded reasonable gels commensurate with a higher cellulose loading and stronger response to Carbotrace. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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15 pages, 4861 KiB  
Article
Electrospun Core (HPMC–Acetaminophen)–Shell (PVP–Sucralose) Nanohybrids for Rapid Drug Delivery
by Xinkuan Liu, Mingxin Zhang, Wenliang Song, Yu Zhang, Deng-Guang Yu and Yanbo Liu
Gels 2022, 8(6), 357; https://doi.org/10.3390/gels8060357 - 7 Jun 2022
Cited by 37 | Viewed by 4161
Abstract
The gels of cellulose and its derivatives have a broad and deep application in pharmaceutics; however, limited attention has been paid to the influences of other additives on the gelation processes and their functional performances. In this study, a new type of electrospun [...] Read more.
The gels of cellulose and its derivatives have a broad and deep application in pharmaceutics; however, limited attention has been paid to the influences of other additives on the gelation processes and their functional performances. In this study, a new type of electrospun core–shell nanohybrid was fabricated using modified, coaxial electrospinning which contained composites of hydroxypropyl methyl cellulose (HPMC) and acetaminophen (AAP) in the core sections and composites of PVP and sucralose in the shell sections. A series of characterizations demonstrated that the core–shell hybrids had linear morphology with clear core–shell nanostructures, and AAP and sucralose distributed in the core and shell section in an amorphous state separately due to favorable secondary interactions such as hydrogen bonding. Compared with the electrospun HPMC–AAP nanocomposites from single-fluid electrospinning of the core fluid, the core–shell nanohybrids were able to promote the water absorbance and HMPC gelation formation processes, which, in turn, ensured a faster release of AAP for potential orodispersible drug delivery applications. The mechanisms of the drug released from these nanofibers were demonstrated to be a combination of erosion and diffusion mechanisms. The presented protocols pave a way to adjust the properties of electrospun, cellulose-based, fibrous gels for better functional applications. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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14 pages, 3918 KiB  
Article
Tissue Adhesive, Conductive, and Injectable Cellulose Hydrogel Ink for On-Skin Direct Writing of Electronics
by Subin Jin, Yewon Kim, Donghee Son and Mikyung Shin
Gels 2022, 8(6), 336; https://doi.org/10.3390/gels8060336 - 30 May 2022
Cited by 22 | Viewed by 4611
Abstract
Flexible and soft bioelectronics used on skin tissue have attracted attention for the monitoring of human health. In addition to typical metal-based rigid electronics, soft polymeric materials, particularly conductive hydrogels, have been actively developed to fabricate biocompatible electrical circuits with a mechanical modulus [...] Read more.
Flexible and soft bioelectronics used on skin tissue have attracted attention for the monitoring of human health. In addition to typical metal-based rigid electronics, soft polymeric materials, particularly conductive hydrogels, have been actively developed to fabricate biocompatible electrical circuits with a mechanical modulus similar to biological tissues. Although such conductive hydrogels can be wearable or implantable in vivo without any tissue damage, there are still challenges to directly writing complex circuits on the skin due to its low tissue adhesion and heterogeneous mechanical properties. Herein, we report cellulose-based conductive hydrogel inks exhibiting strong tissue adhesion and injectability for further on-skin direct printing. The hydrogels consisting of carboxymethyl cellulose, tannic acid, and metal ions (e.g., HAuCl4) were crosslinked via multiple hydrogen bonds between the cellulose backbone and tannic acid and metal-phenol coordinate network. Owing to this reversible non-covalent crosslinking, the hydrogels showed self-healing properties and reversible conductivity under cyclic strain from 0 to 400%, as well as printability on the skin tissue. In particular, the on-skin electronic circuit printed using the hydrogel ink maintained a continuous electrical flow under skin deformation, such as bending and twisting, and at high relative humidity of 90%. These printable and conductive hydrogels are promising for implementing structurally complicated bioelectronics and wearable textiles. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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15 pages, 5217 KiB  
Article
Development of Bigels Based on Date Palm-Derived Cellulose Nanocrystal-Reinforced Guar Gum Hydrogel and Sesame Oil/Candelilla Wax Oleogel as Delivery Vehicles for Moxifloxacin
by Hamid M. Shaikh, Arfat Anis, Anesh Manjaly Poulose, Niyaz Ahamad Madhar and Saeed M. Al-Zahrani
Gels 2022, 8(6), 330; https://doi.org/10.3390/gels8060330 - 24 May 2022
Cited by 12 | Viewed by 3441
Abstract
Bigels are biphasic semisolid systems that have been explored as delivery vehicles in the food and pharmaceutical industries. These formulations are highly stable and have a longer shelf-life than emulsions. Similarly, cellulose-based hydrogels are considered to be ideal for these formulations due to [...] Read more.
Bigels are biphasic semisolid systems that have been explored as delivery vehicles in the food and pharmaceutical industries. These formulations are highly stable and have a longer shelf-life than emulsions. Similarly, cellulose-based hydrogels are considered to be ideal for these formulations due to their biocompatibility and flexibility to mold into various shapes. Accordingly, in the present study, the properties of an optimized guar gum hydrogel and sesame oil/candelilla wax oleogel-based bigel were tailored using date palm-derived cellulose nanocrystals (dp-CNC). These bigels were then explored as carriers for the bioactive molecule moxifloxacin hydrochloride (MH). The preparation of the bigels was achieved by mixing guar gum hydrogel and sesame oil/candelilla wax oleogel. Polarizing microscopy suggested the formation of the hydrogel-in-oleogel type of bigels. An alteration in the dp-CNC content affected the size distribution of the hydrogel phase within the oleogel phase. The colorimetry studies revealed the yellowish-white color of the samples. There were no significant changes in the FTIR functional group positions even after the addition of dp-CNC. In general, the incorporation of dp-CNC resulted in a decrease in the impedance values, except BG3 that had 15 mg dp-CNC in 20 g bigel. The BG3 formulation showed the highest firmness and fluidity. The release of MH from the bigels was quasi-Fickian diffusion mediated. BG3 showed the highest release of the drug. In summary, dp-CNC can be used as a novel reinforcing agent for bigels. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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15 pages, 3500 KiB  
Article
Preparation and Enzyme Degradability of Spherical and Water-Absorbent Gels from Sodium Carboxymethyl Cellulose
by Sayaka Fujita, Toshiaki Tazawa and Hiroyuki Kono
Gels 2022, 8(5), 321; https://doi.org/10.3390/gels8050321 - 20 May 2022
Cited by 12 | Viewed by 3402
Abstract
To synthesize a biodegradable alternative to spherical polyacrylic acid absorbent resin, spherical hydrogel particles were prepared from carboxymethyl cellulose (CMC) dissolved in an aqueous solution, using ethylene glycol diglycidyl ether (EGDE) as a crosslinking agent. The effect of varying the initial CMC concentration [...] Read more.
To synthesize a biodegradable alternative to spherical polyacrylic acid absorbent resin, spherical hydrogel particles were prepared from carboxymethyl cellulose (CMC) dissolved in an aqueous solution, using ethylene glycol diglycidyl ether (EGDE) as a crosslinking agent. The effect of varying the initial CMC concentration and feed amount of EGDE on the shape, water absorbency, water-holding capacity, and enzyme degradability of the resultant CMC hydrogels was determined. The reaction solution was poured into fluid paraffin, and spherical hydrogel particles were obtained via the shear force from stirring. The shape and diameter of the spherical hydrogel particles in the swollen state depended on the CMC concentration. The spherical hydrogel particles obtained by increasing the amount of EGDE resulted in a decrease in absorbency. Additionally, all the spherical hydrogel particles were degraded by cellulase. Thus, spherical biodegradable hydrogel particles were prepared from CMC, and the particle size and water absorption of the hydrogel could be controlled in the range of 5–18 mm and 30–90 g·g−1 in the swollen state, respectively. As an alternative to conventional superabsorbent polymers, the spherical CMC hydrogels are likely to be useful in industrial and agricultural applications. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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16 pages, 2122 KiB  
Article
Smart Methylcellulose Hydrogels for pH-Triggered Delivery of Silver Nanoparticles
by Lorenzo Bonetti, Andrea Fiorati, Agnese D’Agostino, Carlo Maria Pelacani, Roberto Chiesa, Silvia Farè and Luigi De Nardo
Gels 2022, 8(5), 298; https://doi.org/10.3390/gels8050298 - 12 May 2022
Cited by 20 | Viewed by 3267
Abstract
Infection is a severe complication in chronic wounds, often leading to morbidity or mortality. Current treatments rely on dressings, which frequently contain silver as a broad-spectrum antibacterial agent, although improper dosing can result in severe side effects. This work proposes a novel methylcellulose [...] Read more.
Infection is a severe complication in chronic wounds, often leading to morbidity or mortality. Current treatments rely on dressings, which frequently contain silver as a broad-spectrum antibacterial agent, although improper dosing can result in severe side effects. This work proposes a novel methylcellulose (MC)-based hydrogel designed for the topical release of silver nanoparticles (AgNPs) via an intelligent mechanism activated by the pH variations in infected wounds. A preliminary optimization of the physicochemical and rheological properties of MC hydrogels allowed defining the optimal processing conditions in terms of crosslinker (citric acid) concentration, crosslinking time, and temperature. MC/AgNPs nanocomposite hydrogels were obtained via an in situ synthesis process, exploiting MC both as a capping and reducing agent. AgNPs with a 12.2 ± 2.8 nm diameter were obtained. MC hydrogels showed a dependence of the swelling and degradation behavior on both pH and temperature and a noteworthy pH-triggered release of AgNPs (release ~10 times higher at pH 12 than pH 4). 1H-NMR analysis revealed the role of alkaline hydrolysis of the ester bonds (i.e., crosslinks) in governing the pH-responsive behavior. Overall, MC/AgNPs hydrogels represent an innovative platform for the pH-triggered release of AgNPs in an alkaline milieu. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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15 pages, 4463 KiB  
Article
In Situ Growth of Zeolitic Imidazolate Framework-L in Macroporous PVA/CMC/PEG Composite Hydrogels with Synergistic Antibacterial and Rapid Hemostatic Functions for Wound Dressing
by Hang Yang, Xianyu Lan and Yuzhu Xiong
Gels 2022, 8(5), 279; https://doi.org/10.3390/gels8050279 - 1 May 2022
Cited by 18 | Viewed by 3683
Abstract
Although many advances have been made in medicine, traumatic bleeding and wound infection are two of the most serious threats to human health. To achieve rapid hemostasis and prevent infection by pathogenic microbes, the development of new hemostatic and antibacterial materials has recently [...] Read more.
Although many advances have been made in medicine, traumatic bleeding and wound infection are two of the most serious threats to human health. To achieve rapid hemostasis and prevent infection by pathogenic microbes, the development of new hemostatic and antibacterial materials has recently gained significant attention. In this paper, safe, non-toxic, and biocompatible polyvinyl alcohol (PVA); carboxymethyl cellulose (CMC), which contains several carboxyl and hydroxyl groups; and polyethylene glycol (PEG), which functions as a pore-forming agent, were used to prepare a novel PVA/CMC/PEG-based composite hydrogel with a macroporous structure by the freeze-thaw method and the phase separation technique. In addition, a PVA/CMC/PEG@ZIF-L composite hydrogel was prepared by the in situ growth of zeolitic imidazolate framework-L (ZIF-L). ZIF-L grown in situ on hydrogels released Zn2+ and imidazolyl groups. They elicited a synergistic antibacterial effect in hemostasis with PVA and CMC, rendering the PVA/CMC/PEG@ZIF-L hydrogel with a good antibacterial effect against Staphylococcus aureus. At the same time, the macroporous structure enabled the rapid release of Zn2+ and imidazolyl groups in ZIF-L and promoted cell proliferation at an early stage, enhancing the coagulation efficiency. A rat liver injury model was used to confirm its rapid hemostasis capacity. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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14 pages, 2524 KiB  
Article
Properties of Cellulose Pulp and Polyurethane Composite Films Fabricated with Curcumin by Using NMMO Ionic Liquid
by Chaehyun Jo, Sam Soo Kim, Balasubramanian Rukmanikrishnan, Srinivasan Ramalingam, Prabakaran D. S. and Jaewoong Lee
Gels 2022, 8(4), 248; https://doi.org/10.3390/gels8040248 - 18 Apr 2022
Cited by 7 | Viewed by 2539
Abstract
Cellulose pulp (CP), polyurethane (PU), and curcumin-based biocompatible composite films were prepared using a simple cost-effective method. Significant structural and microstructural changes were studied using FT-IR spectroscopy, XRD, and SEM. The 5% and 10% gravimetric losses of the CP/PU/curcumin composite were found to [...] Read more.
Cellulose pulp (CP), polyurethane (PU), and curcumin-based biocompatible composite films were prepared using a simple cost-effective method. Significant structural and microstructural changes were studied using FT-IR spectroscopy, XRD, and SEM. The 5% and 10% gravimetric losses of the CP/PU/curcumin composite were found to be in the range 87.2–182.3 °C and 166.7–249.8 °C, respectively. All the composites exhibited single Tg values in the range 147.4–154.2 °C. The tensile strength of CP was measured to be 93.2 MPa, which dropped to 14.1 MPa for the 1:0.5 CP/PU composite and then steadily increased to 30.5 MPa with further addition of PU. The elongation at the break of the composites decreased from 8.1 to 3.7% with the addition of PU. The addition of PU also improved the water vapor permeability (3.96 × 10−9 to 1.75 × 10−9 g m−1 s−1 Pa−1) and swelling ratio (285 to 202%) of the CP composite films. The CP/PU/curcumin composite exhibited good antioxidant activity and no cytotoxicity when tested on the HaCat cell line. The visual appearance and UV transmittance (86.2–32.9% at 600 nm) of the CP composite films were significantly altered by the incorporation of PU and curcumin. This study demonstrates that CP/PU/curcumin composites can be used for various packaging and biomedical applications. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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12 pages, 3519 KiB  
Article
Soft Stretchable Conductive Carboxymethylcellulose Hydrogels for Wearable Sensors
by Kyuha Park, Heewon Choi, Kyumin Kang, Mikyung Shin and Donghee Son
Gels 2022, 8(2), 92; https://doi.org/10.3390/gels8020092 - 4 Feb 2022
Cited by 17 | Viewed by 4465
Abstract
Hydrogels that have a capability to provide mechanical modulus matching between time-dynamic curvilinear tissues and bioelectronic devices have been considered tissue-interfacing ionic materials for stably sensing physiological signals and delivering feedback actuation in skin-inspired healthcare systems. These functionalities are totally different from those [...] Read more.
Hydrogels that have a capability to provide mechanical modulus matching between time-dynamic curvilinear tissues and bioelectronic devices have been considered tissue-interfacing ionic materials for stably sensing physiological signals and delivering feedback actuation in skin-inspired healthcare systems. These functionalities are totally different from those of elastomers with low ionic conductivity and higher stiffness. Despite such remarkable progress, their low conductivity remains limited in transporting electrical charges to internal or external terminals without undesired information loss, potentially leading to an unstable biotic–abiotic interfaces in the wearable electronics. Here, we report a soft stretchable conductive hydrogel composite consisting of alginate, carboxymethyl cellulose, polyacrylamide, and silver flakes. This composite was fabricated via sol–gel transition. In particular, the phase stability and low dynamic modulus rates of the conductive hydrogel were confirmed through an oscillatory rheological characterization. In addition, our conductive hydrogel showed maximal tensile strain (≈400%), a low deformations of cyclic loading (over 100 times), low resistance (≈8.4 Ω), and a high gauge factor (≈241). These stable electrical and mechanical properties allowed our composite hydrogel to fully support the operation of a light-emitting diode demonstration under mechanical deformation. Based on such durable performance, we successfully measured the electromyogram signals without electrical malfunction even in various motions. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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15 pages, 4583 KiB  
Article
Zinc- and Copper-Loaded Nanosponges from Cellulose Nanofibers Hydrogels: New Heterogeneous Catalysts for the Synthesis of Aromatic Acetals
by Laura Riva, Angelo Davide Lotito, Carlo Punta and Alessandro Sacchetti
Gels 2022, 8(1), 54; https://doi.org/10.3390/gels8010054 - 12 Jan 2022
Cited by 17 | Viewed by 3028
Abstract
Herein we report the synthesis of cellulose-based metal-loaded nano-sponges and their application as heterogeneous catalysts in organic synthesis. First, the combination in water solution of TEMPO-oxidized cellulose nanofibers (TOCNF) with branched polyethyleneimine (bPEI) and citric acid (CA), and the thermal treatment of the [...] Read more.
Herein we report the synthesis of cellulose-based metal-loaded nano-sponges and their application as heterogeneous catalysts in organic synthesis. First, the combination in water solution of TEMPO-oxidized cellulose nanofibers (TOCNF) with branched polyethyleneimine (bPEI) and citric acid (CA), and the thermal treatment of the resulting hydrogel, leads to the synthesis of an eco-safe micro- and nano-porous cellulose nano-sponge (CNS). Subsequently, by exploiting the metal chelation characteristics of CNS, already extensively investigated in the field of environmental decontamination, this material is successfully loaded with Cu (II) or Zn (II) metal ions. Efficiency and homogeneity of metal-loading is confirmed by scanning electron microscopy (SEM) analysis with an energy dispersive X-ray spectroscopy (EDS) detector and by inductively coupled plasma-optical emission spectrometry (ICP-OES) analysis. The resulting materials perform superbly as heterogeneous catalysts for promoting the reaction between aromatic aldehydes and alcohols in the synthesis of aromatic acetals, which play a fundamental role as intermediates in organic synthesis. Optimized conditions allow one to obtain conversions higher than 90% and almost complete selectivity toward acetal products, minimizing, and in some cases eliminating, the formation of carboxylic acid by-products. ICP-OES analysis of the reaction medium allows one to exclude any possible metal-ion release, confirming that catalysis undergoes under heterogeneous conditions. The new metal-loaded CNS can be re-used and recycled five times without losing their catalytic activity. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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Review

Jump to: Editorial, Research

29 pages, 5239 KiB  
Review
Advances in Cellulose-Based Hydrogels for Biomedical Engineering: A Review Summary
by Pengfei Zou, Jiaxin Yao, Ya-Nan Cui, Te Zhao, Junwei Che, Meiyan Yang, Zhiping Li and Chunsheng Gao
Gels 2022, 8(6), 364; https://doi.org/10.3390/gels8060364 - 8 Jun 2022
Cited by 32 | Viewed by 5725
Abstract
In recent years, hydrogel-based research in biomedical engineering has attracted more attention. Cellulose-based hydrogels have become a research hotspot in the field of functional materials because of their outstanding characteristics such as excellent flexibility, stimulus-response, biocompatibility, and degradability. In addition, cellulose-based hydrogel materials [...] Read more.
In recent years, hydrogel-based research in biomedical engineering has attracted more attention. Cellulose-based hydrogels have become a research hotspot in the field of functional materials because of their outstanding characteristics such as excellent flexibility, stimulus-response, biocompatibility, and degradability. In addition, cellulose-based hydrogel materials exhibit excellent mechanical properties and designable functions through different preparation methods and structure designs, demonstrating huge development potential. In this review, we have systematically summarized sources and types of cellulose and the formation mechanism of the hydrogel. We have reviewed and discussed the recent progress in the development of cellulose-based hydrogels and introduced their applications such as ionic conduction, thermal insulation, and drug delivery. Also, we analyzed and highlighted the trends and opportunities for the further development of cellulose-based hydrogels as emerging materials in the future. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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16 pages, 2441 KiB  
Review
Recent Progress of Cellulose-Based Hydrogel Photocatalysts and Their Applications
by Jinyu Yang, Dongliang Liu, Xiaofang Song, Yuan Zhao, Yayang Wang, Lu Rao, Lili Fu, Zhijun Wang, Xiaojie Yang, Yuesheng Li and Yi Liu
Gels 2022, 8(5), 270; https://doi.org/10.3390/gels8050270 - 26 Apr 2022
Cited by 19 | Viewed by 4736
Abstract
With the development of science and technology, photocatalytic technology is of great interest. Nanosized photocatalysts are easy to agglomerate in an aqueous solution, which is unfavorable for recycling. Therefore, hydrogel-based photocatalytic composites were born. Compared with other photocatalytic carriers, hydrogels have a three-dimensional [...] Read more.
With the development of science and technology, photocatalytic technology is of great interest. Nanosized photocatalysts are easy to agglomerate in an aqueous solution, which is unfavorable for recycling. Therefore, hydrogel-based photocatalytic composites were born. Compared with other photocatalytic carriers, hydrogels have a three-dimensional network structure, high water absorption, and a controllable shape. Meanwhile, the high permeability of these composites is an effective way to promote photocatalysis technology by inhibiting nanoparticle photo corrosion, while significantly ensuring the catalytic activity of the photocatalysts. With the growing energy crisis and limited reserves of traditional energy sources such as oil, the attention of researchers was drawn to natural polymers. Like almost all abundant natural polymer compounds in the world, cellulose has the advantages of non-toxicity, degradability, and biocompatibility. It is used as a class of reproducible crude material for the preparation of hydrogel photocatalytic composites. The network structure and high hydroxyl active sites of cellulose-based hydrogels improve the adsorption performance of catalysts and avoid nanoparticle collisions, indirectly enhancing their photocatalytic performance. In this paper, we sum up the current research progress of cellulose-based hydrogels. After briefly discussing the properties and preparation methods of cellulose and its descendant hydrogels, we explore the effects of hydrogels on photocatalytic properties. Next, the cellulose-based hydrogel photocatalytic composites are classified according to the type of catalyst, and the research progress in different fields is reviewed. Finally, the challenges they will face are summarized, and the development trends are prospected. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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18 pages, 1968 KiB  
Review
Cellulosic-Based Conductive Hydrogels for Electro-Active Tissues: A Review Summary
by Esubalew Kasaw Gebeyehu, Xiaofeng Sui, Biruk Fentahun Adamu, Kura Alemayehu Beyene and Melkie Getnet Tadesse
Gels 2022, 8(3), 140; https://doi.org/10.3390/gels8030140 - 23 Feb 2022
Cited by 18 | Viewed by 4830
Abstract
The use of hydrogel in tissue engineering is not entirely new. In the last six decades, researchers have used hydrogel to develop artificial organs and tissue for the diagnosis of real-life problems and research purposes. Trial and error dominated the first forty years [...] Read more.
The use of hydrogel in tissue engineering is not entirely new. In the last six decades, researchers have used hydrogel to develop artificial organs and tissue for the diagnosis of real-life problems and research purposes. Trial and error dominated the first forty years of tissue generation. Nowadays, biomaterials research is constantly progressing in the direction of new materials with expanded capabilities to better meet the current needs. Knowing the biological phenomenon at the interaction among materials and the human body has promoted the development of smart bio-inert and bio-active polymeric materials or devices as a result of vigorous and consistent research. Hydrogels can be tailored to contain properties such as softness, porosity, adequate strength, biodegradability, and a suitable surface for adhesion; they are ideal for use as a scaffold to provide support for cellular attachment and control tissue shapes. Perhaps electrical conductivity in hydrogel polymers promotes the interaction of electrical signals among artificial neurons and simulates the physiological microenvironment of electro-active tissues. This paper presents a review of the current state-of-the-art related to the complete process of conductive hydrogel manufacturing for tissue engineering from cellulosic materials. The essential properties required by hydrogel for electro-active-tissue regeneration are explored after a short overview of hydrogel classification and manufacturing methods. To prepare hydrogel from cellulose, the base material, cellulose, is first synthesized from plant fibers or generated from bacteria, fungi, or animals. The natural chemistry of cellulose and its derivatives in the fabrication of hydrogels is briefly discussed. Thereafter, the current scenario and latest developments of cellulose-based conductive hydrogels for tissue engineering are reviewed with an illustration from the literature. Finally, the pro and cons of conductive hydrogels for tissue engineering are indicated. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Hydrogels)
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