Self-assembled low-molecular-weight gelator injectable microgel beads for delivery of bioactive agents

Piras, Carmen C.; Kay, Alasdair G.; Genever, Paul G.; Smith, David K.

doi:10.1039/d0sc06296k

Cited by 31 publications

(24 citation statements)

References 64 publications

(28 reference statements)

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“…Work to explore this is currently in progress. Given the ability to scale these beads down to the microscale, as we recently reported [5c] and the ability of this LMWG to control the release of bio‐active agents, [25] these mobile systems might also have applications in spatially resolved nanomedicine.…”

Section: Discussionmentioning

confidence: 99%

Self‐Propelling Hybrid Gels Incorporating an Active Self‐Assembled, Low‐Molecular‐Weight Gelator

Piras

Smith

2021

Chemistry A European J

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Hybrid gel beads based on combining a low‐molecular‐weight gelator (LMWG) with a polymer gelator (PG) demonstrate an enhanced ability to self‐propel in water, with the LMWG playing an active role. Hybrid gel beads were loaded with ethanol and shown to move in water owing to the Marangoni effect changes in surface tension caused by the expulsion of ethanol – smaller beads move farther and faster than larger beads. Flat shapes of the hybrid gel were cut using a “stamp” – circles moved the furthest, whereas stars showed more rotation on their own axes. Comparing hybrid LMWG/PG gel beads with PG‐only beads demonstrated that the LMWG speeds up the beads, enhancing the rate of self‐propulsion. Self‐assembly of the LMWG into a “solid‐like” network prevents its leaching from the gel. The LMWG also retains its own unique function – specifically, remediating methylene blue pollutant dye from basic water as a result of noncovalent interactions. The mobile hybrid beads accumulate this dye more effectively than PG‐only beads. Self‐propelling gel beads have potential applications in removal/delivery of active agents in environmental or biological settings. The ability of self‐assembling LMWGs to enhance mobility and control removal/delivery suggests that adding them to self‐propelling systems can add significant value.

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Section: Discussionmentioning

confidence: 99%

Self‐Propelling Hybrid Gels Incorporating an Active Self‐Assembled, Low‐Molecular‐Weight Gelator

Piras

Smith

2021

Chemistry A European J

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“…We note that, with approximately 3 mm diameter, the beads reported here are too large for most local/systemic applications, which would better make use of injection as a delivery mode. However, we have recently demonstrated the potential to develop injectable microgels from this type of system, [9] and we therefore reason that statin‐loaded injectable microgel beads might be achievable. Such systems would be potentially transformative in injectable local and systemic delivery, and work towards this goal is currently a key target in our laboratory.…”

Section: Discussionmentioning

confidence: 99%

“…We have also recently used this approach to generate smaller injectable microgel beads with diameters of about 800 nm, and shown that such microgels can release bioactive agents to enhance tissue growth. [9] With the goal of controlled drug delivery, we have previously been interested in multicomponent hydrogels. [10] As a result, we decided to develop gel beads with stimulus responsiveness.…”

Section: Introductionmentioning

confidence: 99%

“…By loading these gel beads with metal nanoparticles, we demonstrated their potential both in catalysis [8a] and antibacterial [8b] applications. We have also recently used this approach to generate smaller injectable microgel beads with diameters of about 800 nm, and shown that such microgels can release bioactive agents to enhance tissue growth [9] . With the goal of controlled drug delivery, we have previously been interested in multicomponent hydrogels [10] .…”

Section: Introductionmentioning

confidence: 99%

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Hybrid Self‐Assembled Gel Beads for Tuneable pH‐Controlled Rosuvastatin Delivery

Piras

Patterson

Smith

2021

Chemistry A European J

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This article describes the fabrication of new pHresponsive hybrid gel beads combining the polymer gelator calcium alginate with two different low-molecular-weight gelators (LMWGs) based on 1,3 : 2,4-dibenzylidene-d-sorbitol: pH-responsive DBS-COOH and thermally responsive DBS-CONHNH 2 , thus clearly demonstrating that different classes of LMWG can be fabricated into gel beads by using this approach. We also demonstrate that self-assembled multicomponent gel beads can be formed by using different combinations of these gelators. The different gel bead formulations exhibit different responsiveness -the DBS-COOH network can disassemble within those beads in which it is present upon raising the pH. To exemplify preliminary data for a potential application for these hybrid gel beads, we explored aspects of the delivery of the lipid-lowering active pharmaceutical ingredient (API) rosuvastatin. The release profile of this statin from the hybrid gel beads is pHdependent, with greater release at pH 7.4 than at pH 4.0primary control of this process results from the pK a of the API. The extent of pH-mediated API release is also significantly further modified according to gel bead composition. The DBS-COOH/alginate beads show rapid, highly effective drug release at pH 7.4, whereas the three-component DBS-COOH/ DBS-CONHNH 2 /alginate system shows controlled slow release of the API under the same conditions. These initial results indicate that such gel beads constitute a promising, versatile and easily tuned platform suitable for further development for controlled drug-delivery applications.

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“…These various polymers establish complex 3D networks of intermolecular interactions between building blocks to form macroscopic objects. Besides polymers, low-molecular-weight gelators (LMWGs) (generally <2000 Da) are of great interest because the associated gelators have intrinsic self-assembly ability to form different morphologies of fibers, rods, ribbons, and nanotubes, which could be used to build attractive tools for various biomedical applications on account of their high biocompatibility and low toxicity ( Nolan et al, 2017 ; Ramin et al, 2017 ; Piras et al, 2021 ). Among the LMWGs, self-assembly peptide-based hydrogels are well known and have been the subject of many studies because the peptides are the most attractive building blocks, which can be readily controlled by changing the amino acid sequence of the peptides and by modifying the side chains of the peptides ( Frick et al, 2017 ; Fu et al, 2021 ; Zhang et al, 2021 ).…”

Section: Introductionmentioning

confidence: 99%

Self-Assembly Dipeptide Hydrogel: The Structures and Properties

Zheng

et al. 2021

Front. Chem.

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Self-assembly peptide-based hydrogels are well known and popular in biomedical applications due to the fact that they are readily controllable and have biocompatibility properties. A dipeptide is the shortest self-assembling motif of peptides. Due to its small size and simple synthesis method, dipeptide can provide a simple and easy-to-use method to study the mechanism of peptides’ self-assembly. This review describes the design and structures of self-assembly linear dipeptide hydrogels. The strategies for preparing the new generation of linear dipeptide hydrogels can be divided into three categories based on the modification site of dipeptide: 1) COOH-terminal and N-terminal modified dipeptide, 2) C-terminal modified dipeptide, and 3) uncapped dipeptide. With a deeper understanding of the relationship between the structures and properties of dipeptides, we believe that dipeptide hydrogels have great potential application in preparing minimal biocompatible materials.

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Self-assembled low-molecular-weight gelator injectable microgel beads for delivery of bioactive agents

Abstract: We report microgel beads with diameters of ca. 800 nm based on interpenetrating networks of a low-molecular-weight gelator and a polymer gelator, and demonstrate their use as heparin delivery vehicles to enhance stem cell growth.

Cited by 31 publications

References 64 publications

Self‐Propelling Hybrid Gels Incorporating an Active Self‐Assembled, Low‐Molecular‐Weight Gelator

Self‐Propelling Hybrid Gels Incorporating an Active Self‐Assembled, Low‐Molecular‐Weight Gelator

Hybrid Self‐Assembled Gel Beads for Tuneable pH‐Controlled Rosuvastatin Delivery

Self-Assembly Dipeptide Hydrogel: The Structures and Properties

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