Spatial and Directional Control over Self‐Assembly Using Catalytic Micropatterned Surfaces

Olive, Alexandre G. L.; Abdullah, Nor Hakimin; Ziemecka, Iwona; Mendes, Eduardo; Eelkema, Rienk; Esch, Jan H. van

doi:10.1002/ange.201310776

Cited by 33 publications

(15 citation statements)

References 30 publications

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“… 142 , 143 Recognizing catalyst-assisted self-assembly as a common process in nature to achieve spatial control over structure formation, they developed an ingenious way to generate a spatially controlled supramolecular hydrogel using a micropatterned catalyst on a surface. 144 According to their design, the precursors (cyclohexane-1,3,5-tricarbohydrazide and 3,4-bis[2-(2-methoxyethoxy)ethoxy]benzaldehyde, 3:1) of a gelator (trishydrazone derivative 144 ) react on micropatterned catalytic sites on a surface to form building blocks of self-assembled nanofibers that act as the matrixes of the hydrogels. Unlike homogeneous catalysis, this method apparently can achieve multilevel organization among the nanofibers, which is uniquely promising for further development.…”

Section: Stimuli For Hydrogelationmentioning

confidence: 99%

Supramolecular Hydrogelators and Hydrogels: From Soft Matter to Molecular Biomaterials

et al. 2015

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In this review we intend to provide a relatively comprehensive summary of the work of supramolecular hydrogelators after 2004 and to put emphasis particularly on the applications of supramolecular hydrogels/hydrogelators as molecular biomaterials. After a brief introduction of methods for generating supramolecular hydrogels, we discuss supramolecular hydrogelators on the basis of their categories, such as small organic molecules, coordination complexes, peptides, nucleobases, and saccharides. Following molecular design, we focus on various potential applications of supramolecular hydrogels as molecular biomaterials, classified by their applications in cell cultures, tissue engineering, cell behavior, imaging, and unique applications of hydrogelators. Particularly, we discuss the applications of supramolecular hydrogelators after they form supramolecular assemblies but prior to reaching the critical gelation concentration because this subject is less explored but may hold equally great promise for helping address fundamental questions about the mechanisms or the consequences of the self-assembly of molecules, including low molecular weight ones. Finally, we provide a perspective on supramolecular hydrogelators. We hope that this review will serve as an updated introduction and reference for researchers who are interested in exploring supramolecular hydrogelators as molecular biomaterials for addressing the societal needs at various frontiers.

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Section: Stimuli For Hydrogelationmentioning

confidence: 99%

Supramolecular Hydrogelators and Hydrogels: From Soft Matter to Molecular Biomaterials

et al. 2015

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“…[6] A number of strategies have emerged to shape and structure supramolecular gels, [3] including photopatterning, [7] 3D printing, [8] electrochemistry, [9] and surface-mediated processes. [10] Several reports have used controlled diffusion to achieve spatial resolution. [11] Surprisingly, however, there have been limited reports of a supramolecular gel being formulated as spherical particles.…”

Section: Introductionmentioning

confidence: 99%

Self‐Assembling Supramolecular Hybrid Hydrogel Beads

2019

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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 PdII and reducing it in situ to yield catalytically active Pd0 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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“…[10][11][12][13][14][15] Along this route, spatial localization of (bio)catalysts has recently proven to be an effective process to direct supramolecular self-assemblies in a spatiotemporal way. [16][17][18][19][20] Localization of (bio)catalysts in space allows inducing the chemical switch from non-self-assembling entities into self-assembling ones, leading to a spontaneous self-assembly process occurring exclusively and specifically near the (bio)catalyst localization. Ulijn and co-workers have first shown that the immobilization of thermolysin on a glass substrate followed by the contact with a mixture of Fmoc-L and LL dipeptide (L=Leucine) allows the self-assembly nucleation of Fmoc-Ln spatially controlled from the enzymatically-active surface.…”

Section: Introductionmentioning

confidence: 99%

Phase Separation in Supramolecular Hydrogels Based on Peptide Self-Assembly from Enzyme-Coated Nanoparticles

et al. 2019

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Spatial localization of biocatalysts, such as enzymes, has recently proven to be an effective process to direct supramolecular self-assemblies in a spatiotemporal way. In this work, silica nanoparticles functionalized covalently by alkaline phosphatase (NPs@AP) induce the localized growth of selfassembled peptide nanofibers from NPs by dephosphorylation of Fmoc-FFpY peptides (Fmoc: Fluorenylmethyloxycarbonyl; F: phenylalanine; Y: tyrosine; p: phosphate group). The fibrillary nanoarchitecture around NPs@AP underpins a homogeneous hydrogel which unexpectedly undergoes a macroscopic shape change over time. This macroscopic change is due to a phase separation leading to a dense phase (in NPs and nanofibers) in the center of the vial and surrounded by a dilute one which still contains NPs and peptides self-assemblies. We thus hypothesize that the phase separation is not a syneresis process. Such a change is only observed when the enzymes are localized on the NPs. The dense phase contracts with time until reaching a constant volume after several days. For a given phosphorylated peptide concentration, the dense phase contracts faster when NPs@AP concentration is increased. For a given NPs@AP concentration, it condenses faster when the peptide concentration increases. We hypothesize that the appearance of a dense phase is not only due to attractive interactions between NPs@AP but also to the strong interaction of self-assembled peptide nanofibers with the enzymes, covalently fixed on the NPs.

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Spatial and Directional Control over Self‐Assembly Using Catalytic Micropatterned Surfaces

Cited by 33 publications

References 30 publications

Supramolecular Hydrogelators and Hydrogels: From Soft Matter to Molecular Biomaterials

Supramolecular Hydrogelators and Hydrogels: From Soft Matter to Molecular Biomaterials

Self‐Assembling Supramolecular Hybrid Hydrogel Beads

Phase Separation in Supramolecular Hydrogels Based on Peptide Self-Assembly from Enzyme-Coated Nanoparticles

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