Self-Assembling Supramolecular Hybrid Hydrogel Beads

Overview

Journal Angew Chem Int Ed Engl

Specialty Chemistry

Date 2019 Nov 8

PMID 31697017

Citations 18

Authors

Carmen C Piras

Petr Slavik

David K Smith

Affiliations

Soon will be listed here.

Abstract

With the goal of imposing shape and structure on supramolecular gels, we combine a low-molecular-weight gelator (LMWG) with the polymer gelator (PG) calcium alginate in a hybrid hydrogel. By imposing thermal and temporal control of the orthogonal gelation methods, the system either forms an extended interpenetrating network or core-shell-structured gel beads-a rare example of a supramolecular gel formulated inside discrete gel spheres. The self-assembled LMWG retains its unique properties within the beads, such as remediating Pd and reducing it in situ to yield catalytically active Pd nanoparticles. A single PdNP-loaded gel bead can catalyse the Suzuki-Miyaura reaction, constituting a simple and easy-to-use reaction-dosing form. These uniquely shaped and structured LMWG-filled gel beads are a versatile platform technology with great potential in a range of applications.

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References

Weiss R . The past, present, and future of molecular gels. What is the status of the field, and where is it going?. J Am Chem Soc. 2014; 136(21):7519-30. DOI: 10.1021/ja503363v. View

Avino F, Matheson A, Adams D, Clegg P . Stabilizing bubble and droplet interfaces using dipeptide hydrogels. Org Biomol Chem. 2017; 15(30):6342-6348. DOI: 10.1039/c7ob01053b. View

Torres-Martinez A, Angulo-Pachon C, Galindo F, Miravet J . In between molecules and self-assembled fibrillar networks: highly stable nanogel particles from a low molecular weight hydrogelator. Soft Matter. 2019; 15(17):3565-3572. DOI: 10.1039/c9sm00252a. View

Cornwell D, Okesola B, Smith D . Multidomain hybrid hydrogels: spatially resolved photopatterned synthetic nanomaterials combining polymer and low-molecular-weight gelators. Angew Chem Int Ed Engl. 2014; 53(46):12461-5. DOI: 10.1002/anie.201405098. View

Hirst A, Escuder B, Miravet J, Smith D . High-tech applications of self-assembling supramolecular nanostructured gel-phase materials: from regenerative medicine to electronic devices. Angew Chem Int Ed Engl. 2008; 47(42):8002-18. DOI: 10.1002/anie.200800022. View

Felip-Leon C, Cejudo-Marin R, Peris M, Galindo F, Miravet J . Sizing Down a Supramolecular Gel into Micro- and Nanoparticles. Langmuir. 2017; 33(39):10322-10328. DOI: 10.1021/acs.langmuir.7b02440. View

Venkatesan J, Anil S, Kim S, Shim M . Seaweed Polysaccharide-Based Nanoparticles: Preparation and Applications for Drug Delivery. Polymers (Basel). 2019; 8(2). PMC: 6432598. DOI: 10.3390/polym8020030. View

Agrawal G, Agrawal R . Functional Microgels: Recent Advances in Their Biomedical Applications. Small. 2018; 14(39):e1801724. DOI: 10.1002/smll.201801724. View

Wei Q, Xu M, Liao C, Wu Q, Liu M, Zhang Y . Printable hybrid hydrogel by dual enzymatic polymerization with superactivity. Chem Sci. 2017; 7(4):2748-2752. PMC: 5477016. DOI: 10.1039/c5sc02234g. View

10.

Vieira V, Lima A, de Jong M, Smith D . Commercially Relevant Orthogonal Multi-Component Supramolecular Hydrogels for Programmed Cell Growth. Chemistry. 2018; 24(56):15112-15118. DOI: 10.1002/chem.201803292. View

11.

Okesola B, Suravaram S, Parkin A, Smith D . Selective Extraction and In Situ Reduction of Precious Metal Salts from Model Waste To Generate Hybrid Gels with Embedded Electrocatalytic Nanoparticles. Angew Chem Int Ed Engl. 2015; 55(1):183-7. DOI: 10.1002/anie.201507684. View

12.

Jain D, Bar-Shalom D . Alginate drug delivery systems: application in context of pharmaceutical and biomedical research. Drug Dev Ind Pharm. 2014; 40(12):1576-84. DOI: 10.3109/03639045.2014.917657. View

13.

Slavik P, Kurka D, Smith D . Palladium-scavenging self-assembled hybrid hydrogels - reusable highly-active green catalysts for Suzuki-Miyaura cross-coupling reactions. Chem Sci. 2019; 9(46):8673-8681. PMC: 6301269. DOI: 10.1039/c8sc04561e. View

14.

Burey P, Bhandari B, Howes T, Gidley M . Hydrocolloid gel particles: formation, characterization, and application. Crit Rev Food Sci Nutr. 2008; 48(5):361-77. DOI: 10.1080/10408390701347801. View

15.

Agrawal G, Agrawal R . Stimuli-Responsive Microgels and Microgel-Based Systems: Advances in the Exploitation of Microgel Colloidal Properties and Their Interfacial Activity. Polymers (Basel). 2019; 10(4). PMC: 6415239. DOI: 10.3390/polym10040418. View

16.

Ruiz-Olles J, Smith D . Diffusion across a gel-gel interface - molecular-scale mobility of self-assembled 'solid-like' gel nanofibres in multi-component supramolecular organogels. Chem Sci. 2018; 9(25):5541-5550. PMC: 6048691. DOI: 10.1039/c8sc01071d. View

17.

Lovrak M, Hendriksen W, Maity C, Mytnyk S, Steijn V, Eelkema R . Free-standing supramolecular hydrogel objects by reaction-diffusion. Nat Commun. 2017; 8:15317. PMC: 5465320. DOI: 10.1038/ncomms15317. View

18.

Fang W, Zhang Y, Wu J, Liu C, Zhu H, Tu T . Recent Advances in Supramolecular Gels and Catalysis. Chem Asian J. 2018; 13(7):712-729. DOI: 10.1002/asia.201800017. View

19.

Howe E, Okesola B, Smith D . Self-assembled sorbitol-derived supramolecular hydrogels for the controlled encapsulation and release of active pharmaceutical ingredients. Chem Commun (Camb). 2015; 51(35):7451-4. DOI: 10.1039/c5cc01868d. View

20.

Slaughter B, Khurshid S, Fisher O, Khademhosseini A, Peppas N . Hydrogels in regenerative medicine. Adv Mater. 2010; 21(32-33):3307-29. PMC: 4494665. DOI: 10.1002/adma.200802106. View