Construction of supramolecular hydrogels using photo-generated nitric oxide radicals

Mulvee, Matthew T.; Vasiljević, Nataša; Mann, Stephen; Patil, Avinash J.

doi:10.1039/c8sm00651b

Cited by 6 publications

(9 citation statements)

References 62 publications

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“…Supramolecular hydrogels have continued to gain support, highlighting their ability for fast recovery times after disruption. [138][139][140][141][142][143] An interesting material was proposed by Shao et al [144] in which supramolecular hydrogels based on DNA selfassembly were created forming a hydrogel from complimentary base pairing. In another approach, Yavvari et al [145] evaluated catechol-modified chitosan and Fe(III) selfassembling hydrogels, in which a naturally forming ligand interaction was formed between the catechol group and the iron.…”

Section: Physically Crosslinked Hydrogelsmentioning

confidence: 99%

Flow behavior prior to crosslinking: The need for precursor rheology for placement of hydrogels in medical applications and for 3D bioprinting

Townsend

Beck

Gehrke

et al. 2019

Progress in Polymer Science

148

102

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Hydrogels-water swollen cross-linked networks-have demonstrated considerable promise in tissue engineering and regenerative medicine applications. However, ambiguity over which rheological properties are needed to characterize these gels before crosslinking still exists. Most hydrogel research focuses on the performance of the hydrogel construct after implantation, but for clinical practice, and for related applications such as bioinks for 3D bioprinting, the behavior of the pre-gelled state is also critical. Therefore, the goal of this review is to emphasize the need for better rheological characterization of hydrogel precursor formulations, and standardized testing for surgical placement or 3D bioprinting. In particular, we consider engineering paste or putty precursor solutions (i.e., suspensions with a yield stress), and distinguish between these differences to ease the path to clinical translation. The connection between rheology and surgical application as well as how the use of paste and putty nomenclature can help to qualitatively identify material properties are explained. Quantitative rheological properties for defining materials as either pastes or putties are proposed to enable easier adoption to current methods. Specifically, the three-parameter Herschel-Bulkley model is proposed as a suitable model to correlate experimental data and provide a basis for meaningful comparison between different materials. This model combines a yield stress, the critical parameter distinguishing solutions from pastes (100-2000 Pa) and from putties (>2000 Pa), with power law fluid behavior once the yield stress is exceeded. Overall, successful implementation of paste or putty handling properties to the hydrogel precursor may minimize the surgeon-technology learning time and ultimately ease

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Section: Physically Crosslinked Hydrogelsmentioning

confidence: 99%

Flow behavior prior to crosslinking: The need for precursor rheology for placement of hydrogels in medical applications and for 3D bioprinting

Townsend

Beck

Gehrke

et al. 2019

Progress in Polymer Science

148

102

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show abstract

“…The consequences of the aforementioned non-orthogonal assembly on the macroscopic properties of the hydrogels were studied using differential scanning calorimetry (DSC) and oscillatory rheology ( Figure 5 ). The DSC thermograms displayed a broad endothermic peak for all samples, corresponding to the disruption of the non-covalent crosslinked matrix of the supramolecular hydrogel system, which facilitates the gel-to-sol transition [ 25 , 70 , 71 , 72 ]. The single-component FY gel showed a broad minimum at 40.1 °C with a broad shoulder in the region of 48–60 °C.…”

Section: Resultsmentioning

confidence: 99%

“…Oscillatory amplitude sweeps at a constant frequency (1 Hz) demonstrated a linear viscoelastic region (LVR) for all the hydrogels, in which the storage (elastic) G’ moduli were roughly an order of magnitude higher than the loss (viscous) G” moduli. This indicated that an elastic solid-like nanofilament network permeated throughout a viscous solvent [ 25 , 27 , 34 , 70 , 74 ]. All samples showed crossover points with a sharp decrease in storage moduli (G’) compared to viscous moduli (G”), which were assigned to the transition from an elastic gel to a viscous fluid [ 25 , 71 , 75 , 76 ].…”

Section: Resultsmentioning

confidence: 99%

Stimuli-Responsive Nucleotide–Amino Acid Hybrid Supramolecular Hydrogels

Mulvee

Vasiljević

Mann

et al. 2021

Gels

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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.

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“…12 Generally, bis(urea) gels are thermally reversible as they are formed through reversible non-covalent interactions and their gelation behavior can be manipulated by altering the experimental conditions. 2,[13][14][15] Furthermore, the prevention of convection effects, reduced solvent evaporation rate and the possibility of designing drug-specific binding functionality, means that supramolecular gels are emerging as effective media for pharmaceutical crystallization. 11,16,17 Drug solid form screening, solid form control and crystal morphology are of key industrial significance.…”

Section: Introductionmentioning

confidence: 99%

Drug Mimetic Organogelators for the Control of Concomitant Crystallization of Barbital and Thalidomide

Saikia

Mulvee

Torres‐Moya

et al. 2020

Crystal Growth & Design

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A strategic approach to control the polymorphism of two related drugs by introducing a drugmimetic imide functional group into the molecular weight organogelator structure is presented. This was achieved with novel aminoglutethimide-derived bis(urea) organogelators designed to form gels that act as targeted crystallization media for (±)-thalidomide and barbital. The organogelators prevent concomitant crystallization, a serious issue for drug formulation and development. This work demonstrates the potential to control concomitant crystallization with rationally designed supramolecular gelators.

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Construction of supramolecular hydrogels using photo-generated nitric oxide radicals

Cited by 6 publications

References 62 publications

Flow behavior prior to crosslinking: The need for precursor rheology for placement of hydrogels in medical applications and for 3D bioprinting

Flow behavior prior to crosslinking: The need for precursor rheology for placement of hydrogels in medical applications and for 3D bioprinting

Stimuli-Responsive Nucleotide–Amino Acid Hybrid Supramolecular Hydrogels

Drug Mimetic Organogelators for the Control of Concomitant Crystallization of Barbital and Thalidomide

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