Sol-gel Transition Research Articles

Detection of H2O2 and catalase on a paper-based flow sensor constructed with borate cross-linked PVA hydrogel

The detections of H2O2 and catalase play an important role in daily life. This study introduces a paper-based flow sensor that is specifically designed to detect H2O2 and catalase. The sensor utilizes a hydrogel composed of cross-linked 4-carboxyphenylboronic acid and polyvinyl alcohol. When H2O2 is in contact with the hydrogel, the B–C bonds of the hydrogel undergo a reactive process, causing decomposition of the hydrogel. The pH indicator strip enables the visual monitoring of the viscosity change that occurs during the gel-sol transition. The quantification of H2O2 is accomplished by assessing the proportion of water coverage on the pH indicator strip. The sensor shows a detection limit of 0.077 wt% and is applicable for the quantitative measurement of H2O2 in routinely used disinfectants. Furthermore, the presence of catalase is effectively identified and the detection of catalase in milk is successfully fulfilled. In summary, this work proposes a simple, user-friendly, label-free, and cost-effective method for constructing a paper-based flow sensor using borate cross-linked polyvinyl alcohol hydrogel, showing great potential for detecting H2O2 and catalase in various practical scenarios.

Fluoride-Ion-Responsive Sol-Gel Transition in an L-Cysteine/AgNO3 System: Self-Assembly Peculiarities and Anticancer Activity.

Supramolecular hydrogels based on low-molecular-weight compounds are a unique class of so-called "soft" materials, formed by weak non-covalent interactions between precursors at their millimolar concentrations. Due to the variety of structures that can be formed using different low-molecular-weight gelators, they are widely used in various fields of technology and medicine. In this study, we report for the first time an unusual self-assembly process of mixing a hydrosol obtained from L-cysteine and silver nitrate (cysteine-silver sol-CSS) with sodium halides. Modern instrumental techniques such as viscosimetry, UV spectroscopy, dynamic light scattering, zeta potential measurements, SEM and EDS identified that adding fluoride anions to CSS is able to form stable hydrogels of a thixotropic nature, while Cl-, Br- and I- lead to precipitation. The self-assembly process proceeds using a narrow concentration range of F-. An increase in the fluoride anion content in the system leads to a change in the gel network morphology from elongated structures to spherical ones. This fact is reflected in a decrease in the gel viscosity and a number of gel-sol-gel transition cycles. The mechanism of F-'s interaction with hydrosol includes the condensation of anions on the positive surface of the CSS nanoparticles, their binding via electrostatic forces and the formation of a resulting gel carcass. In vitro analysis showed that the hydrogels suppressed human squamous carcinoma cells at a micromolar sample concentration. The obtained soft gels could have potential applications against cutaneous malignancy and as carriers for fluoride anion and other bioactive substance delivery.

Tannic acid and silicate-functionalized polyvinyl alcohol-hyaluronic acid hydrogel for infected diabetic wound healing.

Healing of chronic diabetic wounds is challenging due to complications of severe inflammatory microenvironment, bacterial infection and poor vascular formation. Herein, a novel injectable polyvinyl alcohol-hyaluronic acid-based composite hydrogel was developed, with tannic acid (TA) and silicate functionalization to fabricate an 'all-in-one' hydrogel PTKH. On one hand, after being locally injected into the wound site, the hydrogel underwent a gradual sol-gel transition in situ, forming an adhesive and protective dressing for the wound. Manipulations of rheological characteristics, mechanical properties and swelling ability of PTKH could be performed via regulating TA and silicate content in hydrogel. On the other hand, PTKH was capable of eliminating reactive oxygen species overexpression, combating infection and generating a cell-favored microenvironment for wound healing acceleration in vitro. Subsequent animal studies demonstrated that PTKH could greatly stimulate angiogenesis and epithelization, accompanied with inflammation and infection risk reduction. Therefore, in consideration of its impressive in vitro and in vivo outcomes, this 'all-in-one' multifunctional hydrogel may hold promise for chronic diabetic wound treatment.

Cryoprotective Polysaccharides with Ordered Gel Structures Induce Ice Growth Anticipation and Survival Enhancement during Cell Cryopreservation.

This work cross-correlated rheological, thermodynamic, and conformational features of several natural polysaccharides to their cryoprotective performance. The basis of cryoprotection of FucoPol, pectin, and agar revealed a causal combination of (i) an emerging sol-gel transition (p = 0.014) at near-hypothermia (4 °C), (ii) noncolligative attenuated supercooling of the kinetic freezing point of water (p = 0.026) supporting ice growth anticipation, and (iii) increased conformational order (p < 0.0001), where helix-/sheet-like features boost cryoprotection. FucoPol, of highest cryoprotective performance, revealed a predominantly helical structure (α/β = 1.5) capable of forming a gel state at 4 °C and the highest degree of supercooling attenuation (TH = 6.2 °C). Ice growth anticipation with gel-like polysaccharides suggests that the gel matrix neutralizes elastic deformations and lethal cell volumetric fluctuations during freezing, thus preventing the loss of homeostasis and increasing post-thaw viability. Ultimately, structured gels capable of attenuated supercooling enable cryoprotective action at the polymer-cell interface, in addition to polymer-ice interactions. This rationale potentiates implementing alternative, biobased, noncytotoxic polymers in cryobiology.

Surfactant-mediated gelation by 12-hydroxyoctadecanoic acid in a nonionic surfactant system

In this study, we present a hydrogel fabrication utilizing a water-insoluble, low-molecular-weight organogelator by the surfactant-mediated gelation (SMG). Specifically, we employed a nonionic surfactant (poly(oxyethylene) sorbitan monooleate, Tween 80) and an organogelator (12-hydroxyoctadecanoic acid, 12-HOA) to produce hydrogels. Gelation experiments conducted at varying concentrations of surfactant and gelator demonstrated successful hydrogel formation in the water/Tween 80/12-HOA system. Moreover, we observed a significant dependence of surfactant concentration on gelation ability. The sol-gel transition temperature was found to be influenced by both the gelator and surfactant concentrations. Optical and electron microscopy analyses revealed that the SMG hydrogels comprised an entangled network of fibers with micrometer-scale widths, formed as bundles of submicron-wide fibers, and further composed of fine fibers measuring several tens of nanometers in width. These fine fibers exhibited a left-handed helical structure. Small- and wide-angle X-ray scattering corroborated the presence of a lamellar structure within the fine fibers, displaying a triclinic subcell morphology. The coexistence of micelles with the fiber network was confirmed through small-angle neutron scattering and UV–vis spectroscopy. Furthermore, dynamic viscoelasticity tests demonstrated that the SMG hydrogels exhibited typical solid-like properties indicative of gel behavior.

Reverse mode LCPG films with self-assembly support of gel networks

ABSTRACT Liquid crystal physical gels (LCPG) with a 3D network structure show considerable promise as novel functional materials with a great impact on scientific and practical applications. LCPGs are not characterised by high hardness and high strength, but this mild nature is capable of forming dynamic supramolecular structures with the self-assembly ability of various non-covalent bonds such as hydrogen bonding, π-π stacking, and van der Waals forces. In addition to anisotropic changes under optical and electrical stimulation, it enables to be one of the candidates for display devices. When the isotropic-anisotropic transition temperature of LCPG solution (TIA) is higher than the sol-gel transition temperature of gel molecules (TSG), the gelation can anchor the orientation of liquid crystal molecules to achieve the alteration of transparency and scattering of the film. In this paper, reverse mode LCPG films with high contrast, low driving voltage, and excellent cycle life were prepared using oriented liquid crystal cassettes and LCPG solutions, it also focused on the effects of chiral compounds (S)-octan-2-yl 4-((4-(hexyloxy)benzoyl)oxy)benzoate (S811) and gel 1,3:2,4-bis-0-(3,4-dimethylbenzylidene)sorbitol (DMDBS) content on electro-optical properties of LCPG films as well as the different functions of TIA and TSG on film orientation.

Radiofrequency induced UCST-type gel-sol transition of metformin-conjugated nanogels for precisely synergizing thermal ablation and blood-vessel embolization

Transcatheter arterial chemoembolization (TACE) exhibits an important role in the treatment of some solid tumors. However, incomplete embolization and angiogenesis-induced tumor relapse and metastasis remain the biggest challenges for TACE. Here, we synthesized metformin-conjugated poly(N-acryloyl glycinamide) (pMet) nanogels for precisely synergizing TACE with radiofrequency ablation (RFA) to improve antitumor efficacy. pMet nanogels exhibited RF-heating effect and UCST-type gel-sol phase transition, with high performance of sol syringeability, gel strength and thermal stability. Meanwhile, pMet nanogels showed distinct cytotoxicity and suppression of CD24. By the synergistic efficacy with RF-heating, pMet nanogels exhibited significant tumor regression (0.37 ± 0.5) over 36 d in H22-bearing mice. pMet nanogels further down-regulated the levels of PD-1 and Tim-3 of CD8+ T cells and CD25 and CD38 of CD4+ T cells, suggesting their improvement on tumor immunosuppressive microenvironment. The blood-vessel embolization of pMet nanogels was well validated on rabbit ear vessel model. pMet nanogels provide a new paradigm for constructing RF responsive embolic platform.

Thermoreversible oleogelation of fatty acid monoglyceride-containing sunflower oil from a rheological approach

Nowadays, there is a growing concern among consumers about the impact of diet on health. In this regard, oleogelation has been proposed as a promising strategy to replace unhealthy fats, as well as to encapsulate water-insoluble bioactive compounds in food matrices. Consequently, the development of thermoreversible oleogels may play an important role in the bioavailability and biostability of functional foods and the beneficial effects associated with them. The aim of this work was to evaluate the viscoelastic behavior of oleogels using a commercial food additive (E471) composed of fatty acid monoglycerides (MG). Furthermore, the study of sol-gel transitions of these thermoreversible oleogels allowed to obtain the optimum concentration of gelling agent required. Refined sunflower oil containing 2–5 wt% of E471 were characterized by means of SAOS tests, as a function of temperature. All these systems were liquids above 48 °C, forming stable oleogels below 20 °C. An improvement of the elastic component of them was observed as gelling agent concentration was higher. Oleogels containing 4 and 5 wt% MG showed very similar viscoelastic properties and high stability at body temperature (ca. 37 °C). Conversely, systems containing 2% or 3% led to the formation of weaker gels exhibiting thermo-reversibility but only the latter was stable at body temperature. Therefore, sunflower oleogels containing MG above 3 wt% could be regarded as potential carrier food matrices for lipid-soluble active ingredients. To this end, the modulation of the oleogel network consistency should play a key role in maintaining the integrity of the active principle during gastrointestinal transit.

Synthesis and thermally-induced gelation of interpenetrating nanogels

Thermally-induced in-situ gelation of polymers and nanogels is of significant importance for injectable non-invasive tissue engineering and delivery systems of drug delivery system. In this study, we for the first time demonstrated that the interpenetrating (IPN) nanogel with two networks of poly (N-isopropylacrylamide) (PNIPAM) and poly (N-Acryloyl-l-phenylalanine) (PAphe) underwent a reversible temperature-triggered sol-gel transition and formed a structural color gel above the phase transition temperature (Tp). Dynamic light scattering (DLS) studies confirmed that the Tp of IPN nanogels are the same as that of PNIPAM, independent of Aphe content of the IPN nanogels at pH of 6.5 ∼ 7.4. The rheological and optical properties of IPN nanogels during sol-gel transition were studied by rheometer and optical fiber spectroscopy. The results showed that the gelation time of the hydrogel photonic crystals assembled by IPN nanogel was affected by temperature, PAphe composition, concentration, and sequence of interpenetration. As the temperature rose above the Tp, the Bragg reflection peak of IPN nanogels exhibited blue shift due to the shrinkage of IPN nanogels. In addition, these colored IPN nanogels demonstrated good injectability and had no obvious cytotoxicity. These IPN nanogels will open an avenue to the preparation and thermally-induced in-situ gelation of novel NIPAM-based nanogel system.

Biodegradable chitin nanofiber-alginate dialdehyde hydrogel: An injectable, self-healing scaffold for anti-tumor drug delivery

Injectable hydrogels fabricated from natural polymers have attracted increasing attentions for their potential in biomedical application owing to the biocompatibility and biodegradability. A new class of natural polymer based self-healing hydrogel is constructed through dynamic covalent bonds. The injectable self-healing hydrogels are fabricated by introducing alginate aldehyde to form Schiff base bonds with the chitin nanofibers. These hydrogels demonstrate excellent self-healing properties, injectability, and pH-responsive sol-gel transition behaviors. As a result, they can serve as carriers to allow an effective encapsulation of doxorubicin (DOX) for drug delivery. Furthermore, these hydrogels exhibit excellent biocompatibility and degradability in vitro and in vivo. The sustained release of DOX from the hydrogels effectively suppresses tumor growth in animal models without causing significant systemic toxicity, suggesting their potential application in anti-tumor therapies.

Embedded Bioprinting of Tissue-like Structures Using κ-Carrageenan Sub-Microgel Medium.

Embedded three-dimensional (3D) bioprinting utilizing a granular hydrogel supporting bath has emerged as a critical technique for creating biomimetic scaffolds. However, engineering a suitable gel suspension medium that balances precise bioink deposition with cell viability and function presents multiple challenges, particularly in achieving the desired viscoelastic properties. Here, a novel κ-carrageenan gel supporting bath is fabricated through an easy-to-operate mechanical grinding process, producing homogeneous sub-microscale particles. These sub-microgels exhibit typical Bingham flow behavior with small yield stress and rapid shear-thinning properties, which facilitate the smooth deposition of bioinks. Moreover, the reversible gel-sol transition and self-healing capabilities of the κ-carrageenan microgel network ensure the structural integrity of printed constructs, enabling the creation of complex, multi-layered tissue structures with defined architectural features. Post-printing, the κ-carrageenan sub-microgels can be easily removed by a simple phosphate-buffered saline wash. Further bioprinting with cell-laden bioinks demonstrates that cells within the biomimetic constructs have a high viability of 92% and quickly extend pseudopodia, as well as maintain robust proliferation, indicating the potential of this bioprinting strategy for tissue and organ fabrication. In summary, this novel κ-carrageenan sub-microgel medium emerges as a promising avenue for embedded bioprinting of exceptional quality, bearing profound implications for the in vitro development of engineered tissues and organs.

The Time-Temperature Superposition of Polymeric Rubber Gels Treated by Means of the Mode-Coupling Theory.

Viscoelastic relaxation measurements on styrene-butadiene rubbers (SBRs) doped with carbon nanotube (CNT) at different concentrations around the sol-gel transition show the time-temperature superposition (TTS). This process is described in terms of the mode coupling theory (MCT) approach to viscoelasticity by considering the frequency behavior of the loss modulus E″(ω) and showing that the corresponding TTS is linked to ω1/2 decay. From the analysis of the obtained data, we observe that the interaction between SBRs and CNT determines different levels of decay according to their concentration. Systems with the lowest CNT concentration are only characterized in the studied T-range by their fragile glass-forming behavior. However, at a specific temperature TL, those with the highest CNT concentration show a crossover towards pure Arrhenius that, according to the MCT, indicates the presence of kinetic glass transition (KGT), where system response functions are characterized by scaling behaviors.

3D-printed scaffolds for tissue engineering applications using thermosensitive hydrogels based on biopolymer blends

Three-dimensional (3D) printing is an emerging technology for the construction of complex 3D constructs used for tissue engineering applications. In this study, we are proposing the preparation of 3D printing hydrogel inks consisting of the synthetic polymers poly(caprolactone) and poly(lactic acid), the biopolymer chitosan, and naturally derived gelatin. In addition, pluronic F-127 was used to improve the miscibility between the hydrophobic and hydrophilic components due to its amphiphilic character, as well as for its good 3D printability. The printability of the hydrogel inks was optimized by varying the composition, the extrusion nozzle, and the temperature, while the integrity of the 3D scaffolds was secured via sol–gel transition. The produced hydrogels with PCL-pluronic-chitosan-gelatin/15-20-4-2 wt% (PC3.75-Pl5-CG) and PLA-pluronic-chitosan-gelatin/10-20-4-2 wt% (PL2.5-Pl5-CG) presented the best printability, producing smooth and uniform porous scaffolds. The prepared hydrogels were formed via the interactions between the polymers through hydrogen bonding. Additionally, the produced hydrogels exhibited temperature-dependent swelling behavior, and the scaffolds with PCL presented lower swelling capacity than the scaffolds with PLA. The produced scaffolds presented slower hydrolyzation rate in simulated body fluid (SBF) at 25 °C compared to 37 °C. Biological studies proved that the 3D-printed porous scaffolds were non-cytotoxic and promoted human adipose-derived mesenchymal stem cell adhesion.Graphical abstract

Rheological and Injectability Evaluation of Sterilized Poloxamer-407-Based Hydrogels Containing Docetaxel-Loaded Lipid Nanoparticles.

Nanostructured lipid carriers (NLCs) have the potential to increase the bioavailability and reduce the side effects of docetaxel (DTX). However, only a small fraction of nanoparticles given intravenously can reach a solid tumor. In situ-forming gels combined with nanoparticles facilitate local administration and promote drug retention at the tumor site. Injectable hydrogels based on poloxamer 407 are excellent candidates for this hybrid nanoparticle-hydrogel system because of their thermoresponsive behavior and biocompatibility. Therefore, this work aimed to develop injectable poloxamer hydrogels containing NLCs for intratumoral delivery of DTX. To ensure sterility, the obtained hydrogels were autoclaved (121 °C for 15 min) after preparation. Then, the incorporation of NLCs into the poloxamer hydrogels and the impact of steam sterilization on the nanocomposite hydrogels were evaluated concerning sol-gel transition, injectability, and physicochemical stability. All formulations were extruded through the tested syringe-needle systems with acceptable force (2.2-13.4 N) and work (49.5-317.7 N·mm) of injection. Following steam sterilization, injection became easier in most cases, and the physicochemical properties of all hydrogels remained practically unchanged according to the spectroscopical and thermal analysis. The rheological evaluation revealed that the nanocomposite hydrogels were liquid at 25 °C and underwent rapid gelation at 37 °C. However, their sterilized counterparts gelled at 1-2 °C above body temperature, suggesting that the autoclaving conditions employed had rendered these nanocomposite hydrogels unsuitable for local drug delivery.

Disaggregation and fibrillation during sol-gel transition of alginate hydrogels

The rheological and morphological characteristics of Ca-crosslinked alginate hydrogels with two different M/G ratios, α-L-guluronate (G)-rich and β-D-mannuronate (M)-rich, each with one alginic acid concentration, were investigated. It was found that the stiffness and elasticity of alginate hydrogels are derived from the thickness and density of the fibril network structures. In aqueous alginate solution, ball-like aggregates of alginates are present. Time-resolved small-angle X-ray scattering and time-domain nuclear magnetic resonance measurements suggest that the disaggregation of alginate aggregates and loose fibrillation occur in the early stage of the sol-gel transition. After these induction stage, direct gelation is finally caused by the formation of the egg-box junction. G-rich alginate hydrogel has a higher stiffness and a thicker and denser fibril network structure than M-rich alginate hydrogel. The former also exhibits faster and more significant changes in physical properties during the sol-gel transition.

Thermosensitive injectable polysaccharide-based hydrogels: Gelation mechanisms, synthetic strategies, biomedical applications, and challenges

In recent years, thermosensitive polysaccharide-based injectable hydrogels have gained increasing attention in biomedical applications, including wound healing, drug delivery, and cartilage repair. These hydrogels have favorable biocompatibility, biodegradability, and tunable physical and chemical properties. Thermosensitive polysaccharide-based injectable hydrogels are a class of intelligent soft matter material. They can undergo a reversible liquid-solid transition when exposed to temperature stimuli. Therefore, their precursor solutions can be accurately inserted into target sites with irregular geometries in a minimally invasive way and then transformed into gels in situ by the organism’s temperature stimulation to deliver biologically active molecules. This review summarizes the recent developments of thermosensitive injectable polysaccharide-based hydrogels. The focus is on the mechanism of sol-gel phase transition, as well as the design and preparation of thermosensitive polysaccharides and their applications in biomedical fields. In addition, the outlook of the challenges in biomedical applications is provided at the end of the paper.

An injectable, chitosan-based hydrogel prepared by Schiff base reaction for anti-bacterial and sustained release applications

Injectable hydrogels, providing sustained release as implanted materials, have received tremendous attention. In this study, chitosan-based hydrogels were prepared via Schiff base reaction of the aldehyde groups on Poly(NIPAM-co-FBEMA) and the amine groups on chitosan. Owing to the dynamic covalent linkage, the SC/PNF hydrogels exhibit pH-responsive, reversible sol-gel transition, injectable, and self-healing capacity. The mechanical strength of SC/PNF hydrogels can be operated simply by switching the composition or solid content of Poly(NIPAM-co-FBEMA) copolymers. Rheological analyses, including frequency sweeps, strain sweep scanning, and dynamic time sweeps, were employed to demonstrate the relationship between storage modulus (G′), loss modulus (G″), and composition of the SC/PNF hydrogels. In vitro release behaviors reveal that vancomycin-loaded SC/PNF hydrogel could contribute to both the initial burst release (over 1000 ppm within 4 h) and the sustained release (3000 ppm for at least 30 days). Pristine SC/PNF hydrogel holds good biocompatibility toward L929 cells and S. aureus that it degrades as incubated with S. aureus. However, vancomycin-wrapped SC/PNF hydrogel possesses a rapid bacterial-killing effect with a clear inhibition zone. In short, the SC/PNF hydrogels deliver not only sustainable release ability but also tunable physical properties, which are expected to be an outstanding candidate for non-invasive, anti-infection applications.

Cationic Azobenzenes as Light-Responsive Crosslinkers for Alginate-Based Supramolecular Hydrogels.

Azobenzene photoswitches are fundamental components in contemporary approaches aimed at light-driven control of intelligent materials. Significant endeavors are directed towards enhancing the light-triggered reactivity of azobenzenes for such applications and obtaining water-soluble molecules able to act as crosslinkers in a hydrogel. Here, we report the rational design and the synthesis of azobenzene/alginate photoresponsive hydrogels endowed with fast reversible sol-gel transition. We started with the synthesis of three cationic azobenzenes (AZOs A, B, and C) and then incorporated them in sodium alginate (SA) to obtain photoresponsive supramolecular hydrogels (SMHGs). The photoresponsive properties of the azobenzenes were investigated by UV-Vis and 1H NMR spectroscopy. Upon irradiation with 365 nm UV light, the azobenzenes demonstrated efficient trans-to-cis isomerization, with complete isomerization occurring within seconds. The return to the trans form took several hours, with AZO C exhibiting the fastest return, possibly due to higher trans isomer stability. In the photoresponsive SMHGs, the minimum gelation concentration (MGC) of azobenzenes was determined for different compositions, indicating that small amounts of azobenzenes could induce gel formation, particularly in 5 wt% SA. Upon exposure to 365 nm UV light, the SMHGs exhibited reversible gel-sol transitions, underscoring their photoresponsive nature. This research offers valuable insights into the synthesis and photoresponsive properties of cationic, water-soluble azobenzenes, as well as their potential application in the development of photoresponsive hydrogels.

Injectable Thermo-Responsive Peptide Hydrogels and Its Enzyme Triggered Dynamic Self-Assembly.

Endogenous stimuli-responsive injectable hydrogels hold significant promise for practical applications due to their spatio-temporal controllable drug delivery. Herein, we report a facile strategy to construct a series of in situ formation polypeptide hydrogels with thermal responsiveness and enzyme-triggered dynamic self-assembly. The thermo-responsive hydrogels are from the diblock random copolymer mPEG-b-P(Glu-co-Tyr). The L-glutamic acid (Glu) segments with different γ-alkyl groups, including methyl, ethyl, and n-butyl, offer specific secondary structure, facilitating the formation of hydrogel. The L-tyrosine (Tyr) residues not only provide hydrogen-bond interactions and thus adjust the sol-gel transition temperatures, but also endow polypeptide enzyme-responsive properties. The PTyr segments could be phosphorylated, and the phosphotyrosine copolymers were amphiphilies, which could readily self-assemble into spherical aggregates and transform into sheet-like structures upon dephosphorylation by alkaline phosphatase (ALP). P(MGlu-co-Tyr/P) and P(MGlu-co-Tyr) copolymers showed good compatibility with both MC3T3-E1 and Hela cells, with cell viability above 80% at concentrations up to 1000 μg/mL. The prepared injectable polypeptide hydrogel and its enzyme-triggered self-assemblies show particular potential for biomedical applications.

UCST-Type Thermoresponsive Sol-Gel Transition Triblock Copolymer Containing Zwitterionic Polymer Blocks.

Thermoresponsive sol-gel transition polymers are of significant interest because of their fascinating biomedical applications, including as drug reservoirs for drug delivery systems and scaffolds for tissue engineering. Although extensive research has been conducted on lower critical solution temperature (LCST)-type sol-gel transition polymers, there have been few reports on upper critical solution temperature (UCST)-type sol-gel transition polymers. In this study, we designed an ABA-type triblock copolymer composed of a poly(ethylene glycol) (PEG) block and zwitterionic polymer blocks that exhibit UCST-type thermoresponsive phase transitions. A sulfobetaine (SB) monomer with both ammonium and sulfonate (-SO3) groups in its side chain or a sulfabetaine (SaB) monomer with both ammonium and sulfate (-OSO3) groups in its side chain was polymerized from both ends of the PEG block via reversible addition-fragmentation chain-transfer (RAFT) polymerization to obtain PSB-PEG-PSB and PSaB-PEG-PSaB triblock copolymers, respectively. Although an aqueous solution containing the PSB-PEG-PSB triblock copolymer showed an increase in viscosity upon cooling, it did not undergo a sol-to-gel transition. In contrast, a sol-to-gel transition was observed when a phosphate-buffered saline containing PSaB-PEG-PSaB was cooled from 80 °C to 25 °C. The PSaB blocks with -OSO3 groups exhibited a stronger dipole-dipole interaction than conventional SB with -SO3 groups, leading to intermolecular association and the formation of a gel network composed of PSaB assemblies bridged with PEG. The fascinating UCST-type thermoresponsive sol-gel transition properties of the PSaB-PEG-PSaB triblock copolymer suggest that it can provide a useful platform for designing smart biomaterials, such as drug delivery reservoirs and cell culture scaffolds.