Stimuli-responsive graphene-based hydrogel driven by disruption of triazine hydrophobic interactions

Leganés, Jorge; Sánchez-Migallón, Ana; Merino, Sonia; Vázquez, Éster

doi:10.1039/c9nr10588c

Cited by 13 publications

(22 citation statements)

References 35 publications

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“…Althought he diaminotriazine molecule protonates at low pH (pK a = 5.15), the SGF buffer was chosen as an acidic mediumi no rder to mimic physiological environments. As expected, DATh ydrogels were shown to increase their swelling degree up to 10-foldi nS GF buffer (Figure 2b), [27] proving their pH-responset oa cidic media. Under these conditions, DATm oieties are protonated and repel each other,t husi ncreasing the water content inside the polymer network.…”

Section: Characterizationo Ft He Hydrogelssupporting

confidence: 78%

“…This narrowing of the pore size is attributed to the effect that graphene exerts in the hydrogel:D AT molecules align into extended 2D hydrogen-bondedf ilms on top of the graphene surface and this event reorganizes the porous structure of the hybrids. [27] In SGF media, rather similar pore size distributions were observed for DATand 0.5 G-DATh ydrogels (Figure 2c red and black, respectively). It is logical that in their protonated state, where the DATm olecules are distant from each other, the DATm olecules are not available for aligning on top of graphene sheets,t herefore no significant rearrangemento nt he porosityi so bserved when graphene is incorporated in the hydrogels.…”

Section: Characterizationo Ft He Hydrogelssupporting

confidence: 63%

“…In previouss tudies, we reportedt hat G-DATh ybrid hydrogels enhanced the delivery of ah ydrophobic drug through selective disruption of DAT-DATh ydrophobic interactions. [27] This enhancement was caused by the loosening of hydrophobic DATd omains that entrapped the drug, whichi nt urn was caused by the presenceo fg raphene as wella si nr esponse to an external acidic medium. The structure of the hydrogels is depicted in Figure 1.…”

Section: Resultsmentioning

confidence: 99%

“…When graphene is introduced, the nanomaterial disrupts the DATa ggregates through p-p and graphene-NH 2 interactions between DATand graphene layers, and this fact consequently increases the swelling degree (SD). [27] Pore size distributions of the hydrogels in their maximum swollens tate show polydisperse average sizes for DATh ydrogels in PBS media( 15 AE 14.5 mm) (Figure 2c,b lue). Since DAT molecules tend to aggregate into amorphous domains, porous distributions in DAT-based hydrogels tend to be heterogeneous.…”

Section: Characterizationo Ft He Hydrogelsmentioning

confidence: 95%

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On‐Demand Hydrophobic Drug Release Based on Microwave‐Responsive Graphene Hydrogel Scaffolds

Bayón

Sánchez-Migallón

Díaz‐Ortiz

et al. 2020

Chemistry A European J

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Electromagnetically driven drug delivery systems stand out among stimulus-responsive materials due to their ability to release cargo on demand by remote stimulation, such as light, near infrared (NIR) or microwave (MW) radiation. MW-responsive soft materials, such as hydrogels, generally operate at 2.45 GHz frequencies, which usually involves rapid overheating of the scaffold and may affect tissue surrounding the target location. In contrast, 915 MHz MW penetrate deeper tissues and are less prone to induce rapid overheating. In order to circumvent these limitations, we present here for the first time a graphene-based hydrogel that is responsive to MW irradiation of ν = 915 MHz. This system is a candidate soft scaffold to deliver a model hydrophobic drug. The graphene present in the hydrogel acts as a heat-sink and avoids overheating of the scaffold upon MW irradiation. In addition, the microwave trigger stimulates the in vitro delivery of the model drug, thus suggesting a remote and deeppenetrating means to deliver a drug from a delivery reservoir. Moreover, the MW-triggered release of drug was observed to be enhanced under acidic conditions, where the swelling state is maximum due to the swelling-induced pH-responsiveness of the hydrogel. The hybrid composite described here is a harmless means to deliver remotely a hydrophobic drug on demand with a MW source of 915 MHz. Potential uses in biomedical applications were evaluated by cytotoxicity tests.

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Section: Characterizationo Ft He Hydrogelssupporting

confidence: 78%

Section: Characterizationo Ft He Hydrogelssupporting

confidence: 63%

Section: Resultsmentioning

confidence: 99%

Section: Characterizationo Ft He Hydrogelsmentioning

confidence: 95%

See 2 more Smart Citations

On‐Demand Hydrophobic Drug Release Based on Microwave‐Responsive Graphene Hydrogel Scaffolds

Bayón

Sánchez-Migallón

Díaz‐Ortiz

et al. 2020

Chemistry A European J

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“…Thus, the fact that the semi-IPN presented worse self-healing results in comparison to SHAP can be explained by the interruption of the strong hydrogen bonds present between the water molecules by the free poly(methacrylic acid) chains. In this context, self-healing ability is also influenced by FLG, which would interrupt hydrogen bond formation, as observed previously by our group[67].A different experiment to confirm the role of water and hydrogen bonding in the selfhealing mechanism involved the replacement of water by DMSO. For this purpose, DMSO was added to a dried SHAP hydrogel in the same molar amount as the water remaining after equilibration of SHAP under ambient conditions.…”

supporting

confidence: 68%

Autonomous self-healing hydrogel with anti-drying properties and applications in soft robotics

Naranjo

Martín

Lopez-Diaz

et al. 2020

Applied Materials Today

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Mimicking nature's self-healing ability has always been desired in science, especially when devices accumulate damage over time with performance, including the loss of function due to deterioration. SHAP (Self-Healing AETA([2-(acryloyloxy)ethyl]trimethylammonium chloride)based Polymer), a hydrogel with autonomous self-healing ability that can be applied for the development of a pneumatic artificial muscle, is presented here. Unlike other self-healing hydrogels, SHAP does not require any external stimulus to self-heal and it presents outstanding anti-drying properties. Few-layer graphene is also incorporated into the polymer network of the hydrogel in order to study the possible influence that the nanomaterial has on the properties of the scaffolds. The mechanical behavior and the self-healing abilities of the resulting hydrogels are analyzed. Moreover, the mechanism of self-healing is discussed in terms of experimental results and theoretical calculations. The data suggest a mechanism based on strong hydrogen-bonding interactions between the water molecules that remain inside SHAP, which keeps the material wet and soft under ambient conditions. Finally, the development of a SHAP-based artificial muscle is presented. The results show good performance of the healed artificial muscles after damage, even with healing periods as short as 10 minutes.

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A Biomimetic Follicle‐Based Design for Engineering Reproductive Technologies

Sánchez‐Ajofrín,

Andreu,

Galindo

et al. 2023

Adv Funct Materials

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In the field of assisted reproductive technologies, oocyte in vitro maturation (IVM) has emerged as a potential alternative to overcome the limitations associated with standard ovarian stimulation treatments. However, current IVM protocols lack standardization and yield oocytes of inferior quality compared to those matured in vivo. To address this issue, novel biomaterials like hydrogels offer distinct advantages in cell culture by providing a 3D cellular environment and facilitating easy adjustment and characterization of mechanical properties, such as hydrogel stiffness. Herein, a novel and reusable bilayer hydrogel system is presented that accurately mimics the mechanical properties of the microenvironment surrounding oocyte maturation. The system comprises an outer layer fabricated from either a 3D‐printed synthetic polymer (2‐vinyl‐4,6‐diamino‐1,3,5‐triazine, (VDT)) or a natural polymer (chitosan), along with an inner layer composed of alginate. By faithfully replicating the mechanical properties of native tissue within a 3D culture environment, this system significantly improves the quality and developmental capacity of oocytes, thus resulting in successful embryo development. Overall, this innovative system holds great potential for future medical research and applications in cell culture, thus representing a significant advancement in assisted reproductive technologies.

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Stimuli-responsive graphene-based hydrogel driven by disruption of triazine hydrophobic interactions

Abstract: The study reported here concerns the preparation of a novel graphene-diaminotriazine (G-DAT) nanocomposite hydrogel for application in the drug delivery field.

Cited by 13 publications

References 35 publications

On‐Demand Hydrophobic Drug Release Based on Microwave‐Responsive Graphene Hydrogel Scaffolds

On‐Demand Hydrophobic Drug Release Based on Microwave‐Responsive Graphene Hydrogel Scaffolds

Autonomous self-healing hydrogel with anti-drying properties and applications in soft robotics

A Biomimetic Follicle‐Based Design for Engineering Reproductive Technologies

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