Controlled Annealing in Adaptive Multicomponent Gels

Ravarino, Paolo; Panja, Santanu; Bianco, Simona; Koev, Todor; Wallace, Matthew; Adams, Dave J.

doi:10.1002/anie.202215813

Cited by 3 publications

(2 citation statements)

References 40 publications

(24 reference statements)

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“…For instance, the replacement of HCl with a hydrolysing reagent such as glucono‐δ‐lactone (GdL) 32,33 or 1,3‐propanesultone 34,35 induces gelation by a slow pH change allowing the formation of strong homogeneous hydrogels. The presence of a reagent that slowly triggers the gelation is useful not only to achieve homogeneity through the gelation process, but also to create transient systems, that is, that evolve over time 36–38 . Moreover, several studies have been devoted to the use of salts to form supramolecular polymers by electrostatic interactions 39–42 .…”

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confidence: 99%

“…The presence of a reagent that slowly triggers the gelation is useful not only to achieve homogeneity through the gelation process, but also to create transient systems, that is, that evolve over time. [36][37][38] Moreover, several studies have been devoted to the use of salts to form supramolecular polymers by electrostatic interactions. [39][40][41][42] In particular, divalent cations proved to be a valid method to obtain gels over a wide range of pH, crosslinking the carboxylate groups derived from the dissolution of dipeptides at high pH.…”

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A short oxazolidine‐2‐one containing peptide forms supramolecular hydrogels under controlled conditions

Ravarino

Giuri

Tomasini

2023

Journal of Peptide Science

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Low‐molecular‐weight hydrogels are made of a small percentage of small organic molecules dispersed in an aqueous medium, which may aggregate in several manners using different methods. However, often the organic gelator in water has poor solubility, so the addition of a solubilising agent is required. In the case of acidic gelators, this mainly consists of the addition of a strong base, that is sodium hydroxide, that deprotonates the acidic moiety, so the gelator molecules become more soluble and tend to assemble into micelles, forming a dispersion. Some gelators, however, are sensitive to the harsh pH and get hydrolysed. This is the case of some molecules presenting carbamates in their features, like Fmoc‐protected or oxazolidinone‐containing peptides. In this paper, we present a valid alternative to sodium hydroxide, by dissolving a tripeptide containing an oxazolidinone moiety in a phosphate buffer (PB) medium at pH 7.4. The results obtained with the NaOH dissolution are compared with the ones with PB, as both methods present advantages and drawbacks. The use of NaOH produces transparent but weak hydrogels, as it exposes the gelator to harsh conditions that end up in its partial hydrolysis, which is more pronounced at high concentrations (≥10 mM). Using PB to dissolve the gelator, this problem is completely avoided as no hydrolysis product has been detected in the hydrogels, which are very stiff although more opaque. By tuning the preparation conditions, we can obtain a wide variety of hydrogels, with the properties required by the final application.

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Section: Introductionmentioning

confidence: 99%

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confidence: 99%

A short oxazolidine‐2‐one containing peptide forms supramolecular hydrogels under controlled conditions

Ravarino

Giuri

Tomasini

2023

Journal of Peptide Science

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Controlled Annealing in Adaptive Multicomponent Gels

et al. 2022

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We use a pH-driven annealing process to convert between co-assembled and self-sorted networks in multicomponent gels. The initially formed gels at low pH are co-assembled, with the two components coexisting within the same self-assembled structures. We use an enzymatic approach to increase the pH, resulting in a gel-to-sol transition, followed by a hydrolysis to lower the pH once again. As the pH decreases, a self-sorted network is formed by a two-stage gelation process determined by the pK a of each component. This approach can be expanded to layered systems to generate many varied systems by changing composition and rates of pH change, adapting their microstructure and so allowing access to a far greater range of morphologies and complexity than can be achieved in single component systems.

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Supramolecular dissipative self‐assembly systems: Approaches and applications

Hou,

Chen,

Wei

et al. 2023

Responsive Materials

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Dissipative self‐assembly (DSA) system requires a continuous supply of fuels to maintain the far‐from‐equilibrium assembled state. Living organisms exist and operate far from the thermodynamic equilibrium by continuous consumption of energy taken from the surroundings, so how to realize the construction of the artificial DSA system has attracted much attention by researchers all over the world. Owing to dynamic controllable noncovalent interactions, artificial supramolecular DSA systems have achieved higher functions fueled by various types of energy, such as chemical fuels, light, electric energy, acoustic energy, and mechanical energy. Upon the input of external fuels, nonactive precursors can be activated to form building blocks at higher energy levels and then self‐assemble into transient supramolecular structures. As the proceeding of deactivation reaction, the building blocks with higher energy level dissipate back to the initial precursors, resulting in the disassembly process, to complete a full cycle. In this review, we summarize the recent advances of artificial supramolecular DSA systems on its construction strategies and energy‐fueled regulation approaches. The applications of supramolecular DSA systems in luminescence modulating, information encryption, self‐regulating gels, drug delivery, and catalysis are also discussed. We hope that this review article will facilitate further understanding and development of DSA systems.

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Controlled Annealing in Adaptive Multicomponent Gels

Cited by 3 publications

References 40 publications

A short oxazolidine‐2‐one containing peptide forms supramolecular hydrogels under controlled conditions

A short oxazolidine‐2‐one containing peptide forms supramolecular hydrogels under controlled conditions

Controlled Annealing in Adaptive Multicomponent Gels

Supramolecular dissipative self‐assembly systems: Approaches and applications

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