Recent Advances and Future Perspectives in Stimuli-Responsive Gels

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Collection Editor
Organic and Macromolecular Chemistry, Department of Chemistry, University of Paderborn, Warburger Str. 100, D-33098 Paderborn, Germany
Interests: controlled polymer synthesis; polymer characterization; smart polymers; hydrolgels; actuators and sensors
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Collection Editor
Polymer Chemistry & Biomaterials Research Group, Centre of Macromolecular Chemistry, Ghent University, Krijgslaan 281, S4 Bis, 9000 Ghent, Belgium
Interests: hydrogels; 3D printing; electrospinning; two-photon polymerization; proteins; polysaccharides; tissue engineering; hydrogel functionalization
Special Issues, Collections and Topics in MDPI journals

Topical Collection Information

Dear Colleagues,

Although the technological and scientific importances of functional polymers have been well established over the last few decades, the most recent focus that has attracted much attention concerns stimuli-responsive polymer gels. These materials are of particular interest due to their abilities to respond to internal and/or external chemico-physical stimuli; such responses are often large and macroscopic. Aside from the scientific challenges of designing stimuli-responsive polymer gels, the main technological interests concern numerous applications, ranging from catalysis in microsystem technology and chemomechanical actuators to sensors. Since the phase transition phenomenon of hydrogels is theoretically well understood, advanced materials based on predictions can be prepared. Since the volume phase transition of hydrogels is a diffusion-limited process, the size of the synthesized hydrogels is an important factor. Consistent downscaling of the gel size will result in fast smart gels with sufficient response times.

To apply smart gels in microsystems and sensors, new preparation techniques for hydrogels have to be developed. For upcoming nanotechnology, nano-sized gels as actuating materials would be of great interest. Finally, new design concepts for tough polymer gels are of interest for overcoming the mechanical shortcomings of conventional gels.

This Topical Collection will provide an international forum for researchers to discuss the most recent studies concerning the preparation, characterization, and applications of such Stimuli-Responsive Gels.  Research and review articles focusing on these topics are welcome.

Prof. Dr. Dirk Kuckling
Prof. Dr. Sandra Van Vlierberghe
Collection Editors

Manuscript Submission Information

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Keywords

  • stimuli-responsiveness
  • cross-linking
  • response time
  • mechanical properties
  • applications
  • pH-sensitive
  • redox-sensitive
  • temperature sensitive
  • mechanical stress sensitive
  • multi-stimuli responsiveness
  • engineering

Related Special Issue

Published Papers (5 papers)

2023

Jump to: 2022, 2021

16 pages, 2651 KiB  
Article
Mechanism for the Magnetorheological Effect of Nanocomposite Hydrogels with Magnetite Microparticles
by Lukas Selzer and Stefan Odenbach
Gels 2023, 9(3), 218; https://doi.org/10.3390/gels9030218 - 14 Mar 2023
Cited by 2 | Viewed by 880
Abstract
In a previous study, we presented an empirical law for the magnetorheological effect of nanocomposite hydrogels with magnetite microparticles derived from rheological data. In order to understand the underlying processes, we employ computed tomography for structure analysis. This allows the evaluation of the [...] Read more.
In a previous study, we presented an empirical law for the magnetorheological effect of nanocomposite hydrogels with magnetite microparticles derived from rheological data. In order to understand the underlying processes, we employ computed tomography for structure analysis. This allows the evaluation of the translational and rotational movement of the magnetic particles. Gels with 10% and 3.0% magnetic particle mass content are investigated at three degrees of swelling and at different magnetic flux densities in steady states by means of computed tomography. Since a temperature-controlled sample-chamber is difficult to implement in a tomographic setup, salt is used to deswell the gels instead. Based on the findings of the particle movement, we propose a mechanism using an energy-based approach. This leads to a theoretical law that shows the same scaling behavior as the previously found empirical law. Full article
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16 pages, 2221 KiB  
Article
Empirical Law for the Magnetorheological Effect of Nanocomposite Hydrogels with Magnetite Microparticles
by Lukas Selzer and Stefan Odenbach
Gels 2023, 9(3), 182; https://doi.org/10.3390/gels9030182 - 25 Feb 2023
Cited by 3 | Viewed by 926
Abstract
Hydrogels are functional smart materials which can be tailored by modifying their chemical composition. Further functionalization can be achieved by incorporating magnetic particles into the gel matrix. In this study, a hydrogel with magnetite micro-particles is synthesized and characterized by rheological measurements. Inorganic [...] Read more.
Hydrogels are functional smart materials which can be tailored by modifying their chemical composition. Further functionalization can be achieved by incorporating magnetic particles into the gel matrix. In this study, a hydrogel with magnetite micro-particles is synthesized and characterized by rheological measurements. Inorganic clay is used as the crosslinking agent, which additionally prevents the sedimentation of the micro-particles during the synthesis of the gel. The mass fractions for the magnetite particles in the synthesized gels range from 10% to 60% in the initial state. Rheological measurements are performed in different degrees of swelling using temperature as a stimulus. The influence of a homogeneous magnetic field is analyzed by a step-wise activation and deactivation during dynamic mechanical analysis. For the evaluation of the magnetorheological effect in the steady states a procedure is developed, which takes occurring drift effects into account. Using the magnetic flux density, the particle volume fraction and the storage modulus as independent parameters, a general product approach is deployed for a regression analysis of the dataset. In the end, an empirical law for the magnetorheological effect in nanocomposite hydrogels can be found. Full article
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2022

Jump to: 2023, 2021

20 pages, 1522 KiB  
Review
Thermosensitive In Situ Gels for Joint Disorders: Pharmaceutical Considerations in Intra-Articular Delivery
by Marina Koland, Anoop Narayanan Vadakkepushpakath, Anish John, Arunraj Tharamelveliyil Rajendran and Indu Raghunath
Gels 2022, 8(11), 723; https://doi.org/10.3390/gels8110723 - 08 Nov 2022
Cited by 5 | Viewed by 3117
Abstract
The intra-articular administration of conventional drug solutions or dispersions in joint diseases such as osteoarthritis has a relatively short retention time and, therefore, limited therapeutic effect. Thermosensitive polymer solutions that exhibit a sol–gel phase transition near body temperature after injection can prolong drug [...] Read more.
The intra-articular administration of conventional drug solutions or dispersions in joint diseases such as osteoarthritis has a relatively short retention time and, therefore, limited therapeutic effect. Thermosensitive polymer solutions that exhibit a sol–gel phase transition near body temperature after injection can prolong drug retention by providing a depot from which the drug release is sustained while relieving inflammation and preventing degradation of the joint complex. Thermosensitive hydrogels have in recent times garnered considerable attention in the intra-articular therapeutics of joint diseases such as osteoarthritis. Among the stimuli-responsive gelling systems, most research has focused on thermosensitive hydrogels. These gels are preferred over other stimuli-sensitive hydrogels since they have well-controlled in situ gelling properties and are also easier to load with drugs. Temperature-sensitive polymers, such as block copolymers or poloxamers, are frequently used to modify their gelation properties, usually in combination with other polymers. They are compatible with most drugs but may pose formulation challenges in terms of their low-response time, highly fragile nature, and low biocompatibility. The stability and biodegradability of implant hydrogels can control the drug release rate and treatment efficacy. This review stresses the application of thermosensitive gels in joint disorders and summarizes recent developments for intra-articular application, including the incorporation of nanoparticles. The hydrogel composition, drug release mechanisms, and the challenges involved in their formulation and storage are also discussed. Full article
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29 pages, 2635 KiB  
Review
Peptide-Based Supramolecular Hydrogels as Drug Delivery Agents: Recent Advances
by Carlos B. P. Oliveira, Valéria Gomes, Paula M. T. Ferreira, José A. Martins and Peter J. Jervis
Gels 2022, 8(11), 706; https://doi.org/10.3390/gels8110706 - 01 Nov 2022
Cited by 19 | Viewed by 4228
Abstract
Supramolecular peptide hydrogels have many important applications in biomedicine, including drug delivery applications for the sustained release of therapeutic molecules. Targeted and selective drug administration is often preferential to systemic drug delivery, as it can allow reduced doses and can avoid the toxicity [...] Read more.
Supramolecular peptide hydrogels have many important applications in biomedicine, including drug delivery applications for the sustained release of therapeutic molecules. Targeted and selective drug administration is often preferential to systemic drug delivery, as it can allow reduced doses and can avoid the toxicity and side-effects caused by off-target binding. New discoveries are continually being reported in this rapidly developing field. In this review, we report the latest developments in supramolecular peptide-based hydrogels for drug delivery, focusing primarily on discoveries that have been reported in the last four years (2018–present). We address clinical points, such as peptide self-assembly and drug release, mechanical properties in drug delivery, peptide functionalization, bioadhesive properties and drug delivery enhancement strategies, drug release profiles, and different hydrogel matrices for anticancer drug loading and release. Full article
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2021

Jump to: 2023, 2022

15 pages, 5161 KiB  
Article
Stimuli-Responsive Nucleotide–Amino Acid Hybrid Supramolecular Hydrogels
by Matthew Mulvee, Natasa Vasiljevic, Stephen Mann and Avinash J. Patil
Gels 2021, 7(3), 146; https://doi.org/10.3390/gels7030146 - 17 Sep 2021
Cited by 2 | Viewed by 2631
Abstract
The ability to assemble chemically different gelator molecules into complex supramolecular hydrogels provides excellent opportunities to construct functional soft materials. Herein, we demonstrate the formation of hybrid nucleotide–amino acid supramolecular hydrogels. These are generated by the silver ion (Ag+)-triggered formation of [...] Read more.
The ability to assemble chemically different gelator molecules into complex supramolecular hydrogels provides excellent opportunities to construct functional soft materials. Herein, we demonstrate the formation of hybrid nucleotide–amino acid supramolecular hydrogels. These are generated by the silver ion (Ag+)-triggered formation of silver–guanosine monophosphate (GMP) dimers, which undergo self-assembly through non-covalent interactions to produce nanofilaments. This process results in a concomitant pH reduction due to the abstraction of a proton from the guanine residue, which triggers the in situ gelation of a pH-sensitive amino acid, N-fluorenylmethyloxycarbonyl tyrosine (FY), to form nucleotide–amino acid hybrid hydrogels. Alterations in the supramolecular structures due to changes in the assembly process are observed, with the molar ratio of Ag:GMP:FY affecting the assembly kinetics, and the resulting supramolecular organisation and mechanical properties of the hydrogels. Higher Ag:GMP stoichiometries result in almost instantaneous gelation with non-orthogonal assembly of the gelators, while at lower molar ratios, orthogonal assembly is observed. Significantly, by increasing the pH as an external stimulus, nanofilaments comprising FY can be selectively disassembled from the hybrid hydrogels. Our results demonstrate a simple approach for the construction of multicomponent stimuli-responsive supramolecular hydrogels with adaptable network and mechanical properties. Full article
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