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Controlling hydrogel properties by tuning non-covalent interactions in a charge complementary multicomponent system.

ABSTRACT: Mixing small molecule gelators is a promising route to prepare useful and exciting materials that cannot be accessed from any of the individual components. Here, we describe pH-triggered hydrogelation by mixing of two non-gelling amphiphiles. The intermolecular interactions among the molecules can be tuned either by controlling the degree of ionization of the components or by a preparative pathway, which enables us to control material properties such as gel strength, gel stiffness, thermal stability, and an unusual shrinking/swelling behaviour.

SUBMITTER: Panja S

PROVIDER: S-EPMC8386653 | biostudies-literature | 2021 Aug

REPOSITORIES: biostudies-literature

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Controlling hydrogel properties by tuning non-covalent interactions in a charge complementary multicomponent system.

Panja Santanu S Seddon Annela A Adams Dave J DJ

Chemical science 20210722 33

Mixing small molecule gelators is a promising route to prepare useful and exciting materials that cannot be accessed from any of the individual components. Here, we describe pH-triggered hydrogelation by mixing of two non-gelling amphiphiles. The intermolecular interactions among the molecules can be tuned either by controlling the degree of ionization of the components or by a preparative pathway, which enables us to control material properties such as gel strength, gel stiffness, thermal stabi ...[more]

PMID: 34522317

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Project description:Hydrogels are versatile materials that have emerged in the last few decades as promising candidates for a range of applications in the biomedical field, from tissue engineering and regenerative medicine to controlled drug delivery. In the drug delivery field, in particular, they have been the subject of significant interest for the spatially and temporally controlled delivery of anticancer drugs and therapeutics. Self-assembling peptide-based hydrogels, in particular, have recently come to the fore as potential candidate vehicles for the delivery of a range of drugs. In order to explore how drug-peptide interactions influence doxorubicin (Dox) release, five β-sheet-forming self-assembling peptides with different physicochemical properties were used for the purpose of this study, namely: FEFKFEFK (F8), FKFEFKFK (FK), FEFEFKFE (FE), FEFKFEFKK (F8K), and KFEFKFEFKK (KF8K) (F: phenylalanine; E: glutamic acid; K: lysine). First, Dox-loaded hydrogels were characterized to ensure that the incorporation of the drug did not significantly affect the hydrogel properties. Subsequently, Dox diffusion out of the hydrogels was investigated using UV absorbance. The amount of drug retained in F8/FE composite hydrogels was found to be directly proportional to the amount of charge carried by the peptide fibers. When cation-π interactions were used, the position and number of end-lysine were found to play a key role in the retention of Dox. In this case, the amount of Dox retained in F8/KF8K composite hydrogels was linked to the amount of end-lysine introduced, and an end-lysine/Dox interaction stoichiometry of 3/1 was obtained. For pure FE and KF8K hydrogels, the maximum amount of Dox retained was also found to be related to the overall concentration of the hydrogels and, therefore, to the overall fiber surface area available for interaction with the drug. For 14 mM hydrogel, ∼170-200 μM Dox could be retained after 24 h. This set of peptides also showed a broad range of susceptibilities to enzymatic degradation opening the prospect of being able to control also the rate of degradation of these hydrogels. Finally, the Dox released from the hydrogel was shown to be active and affect 3T3 mouse fibroblasts viability in vitro. Our study clearly shows the potential of this peptide design as a platform for the formulation of injectable or sprayable hydrogels for controlled drug delivery.

Project description:Surface chemical composition is fundamental to determining properties on the nanoscale, making precise control over surface chemistry critical to being able to optimise nanomaterials for virtually any application. Surface-engineering independent of the preparation of the underlying nanomaterial is particularly attractive for efficient, divergent synthetic strategies, and for the potential to create reactive, responsive and smart nanodevices. For monolayer-stabilised nanoparticles, established methods include ligand exchange to replace the ligand shell in its entirety, encapsulation with amphiphilic (macro)molecules, noncovalent interactions with surface-bound biomolecules, or a relatively limited number of covalent bond forming reactions. Yet, each of these approaches has considerable drawbacks. Here we show that dynamic covalent exchange at the periphery of the nanoparticle-stabilizing monolayer allows surface-bound ligand molecular structure to be substantially modified in mild and reversible processes that are independent of the nanoparticle-molecule interface. Simple stoichiometric variation allows the extent of exchange to be controlled, generating a range of kinetically stable mixed-monolayer compositions across an otherwise identical, self-consistent series of nanoparticles. This approach can be used to modulate nanoparticle properties that are defined by the monolayer composition. We demonstrate switching of nanoparticle solvent compatibility between widely differing solvents - spanning hexane to water - and the ability to tune solubility across the entire continuum between these extremes, all from a single nanoparticle starting point. We also demonstrate that fine control over mixed-monolayer composition influences the assembly of discrete, colloidally stable nanoparticle clusters. By carefully assessing monolayer composition in each state, using both in situ and ex situ methods, we are able to correlate the molecular-level details of the nanoparticle-bound monolayer with system-level properties and behaviour. These empirically determined relationships contribute fundamental insights on nanoscale structure-function relationships, which are currently beyond the capabilities of ab initio prediction.

Dataset Information

Controlling hydrogel properties by tuning non-covalent interactions in a charge complementary multicomponent system.

Publications

Controlling hydrogel properties by tuning non-covalent interactions in a charge complementary multicomponent system.

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