Oberflächenunterstützte Selbstorganisationsstrategien für supramolekulare Hydrogele

Vigier‐Carrière, Cécile; Boulmedais, Fouzia; Schaaf, Pierre; Jierry, Loı̈c

doi:10.1002/ange.201708629

Cited by 12 publications

(4 citation statements)

References 60 publications

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“…267 One way to help increase the local concentrations of the products is to provide a binding site for the products, as shown by the elegant work of Schaaf and Boulmedais. 338 They generated a seed layer composed of poly(acrylic acid) that carried Fmoc-FFC as the pendants. After confirming that PAA-CFF-Fmoc ( 53) interacted with Fmoc-FF p Y (54) to promote ALP catalyzed enzymatic hydrogelation, they embedded ALP in a polyelectrolyte multilayer, which had 53 as the top layer (Figure 41A).…”

Section: 14mentioning

confidence: 99%

“…Based on their innovative approach of surface immobilized ALP for supramolecular hydrogelation, Schaaf and Boulmedais used proteases for localized enzyme-assisted selfassembly (LEASA). 375 As shown in Figure 48C, the enzyme is α-chymotrypsin and the substrate is KL-OEt (104, K: lysine; L: leucine; OEt ethyl ester). After the absorption of αchymotrypsin and bovine serum albumin (BSA) on a surface made of poly(ethylene imine) and tannic acid, the authors allowed the surface to contact the solution of 104 so that αchymotrypsin catalytically converted 104 to (KL) n OEt oligopeptides (105).…”

Section: Proteasesmentioning

confidence: 99%

“…(A) The structures of polyelectrolytes(53) and the peptides(54 and 55) and the illustration of the surface-localized ENS. Adapted from Ref 338. .…”

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confidence: 99%

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Enzymatic Noncovalent Synthesis

et al. 2020

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Enzymatic reactions and noncovalent (i.e., supramolecular) interactions are two fundamental nongenetic attributes of life. Enzymatic noncovalent synthesis (ENS) refers to a process where enzymatic reactions control intermolecular noncovalent interactions for spatial organization of higher-order molecular assemblies that exhibit emergent properties and functions. Like enzymatic covalent synthesis (ECS), in which an enzyme catalyzes the formation of covalent bonds to generate individual molecules, ENS is a unifying theme for understanding the functions, morphologies, and locations of molecular ensembles in cellular environments. This review intends to provide a summary of the works of ENS within the last decade and emphasize ENS for functions. After comparing ECS and ENS, we describe a few representative examples where nature uses ENS, as a rule of life, to create the ensembles of biomacromolecules for emergent properties/functions in a myriad of cellular processes. Then, we focus on ENS of man-made (synthetic) molecules in cell-free conditions, classified by the types of enzymes. After that, we introduce the exploration of ENS of man-made molecules in the context of cells by discussing intercellular, peri/intracellular, and subcellular ENS for cell morphogenesis, molecular imaging, cancer therapy, and other applications. Finally, we provide a perspective on the promises of ENS for developing molecular assemblies/processes for functions. This review aims to be an updated introduction for researchers who are interested in exploring noncovalent synthesis for developing molecular science and technologies to address societal needs.

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Section: 14mentioning

confidence: 99%

Section: Proteasesmentioning

confidence: 99%

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Enzymatic Noncovalent Synthesis

et al. 2020

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“…In the case of peptide‐based hydrogels, a first technological issue that needs to be resolved is the spatial localization of the hydrogel growth from the surface of the polymer foam in order to link the hydrogel and the polymer material. This can be achieved by immobilizing a (bio)catalyst on a planar surface . We immobilized an enzyme that is able to transform non‐self‐assembling precursors present in solution into self‐assembling building blocks on the surface .…”

Section: Figurementioning

confidence: 99%

Supported Catalytically Active Supramolecular Hydrogels for Continuous Flow Chemistry

et al. 2019

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Inspired by biology, one current goal in supramolecular chemistry is to control the emergence of new functionalities arising from the self‐assembly of molecules. In particular, some peptides can self‐assemble and generate exceptionally catalytically active fibrous networks able to underpin hydrogels. Unfortunately, the mechanical fragility of these materials is incompatible with process developments, relaying this exciting field to academic curiosity. Here, we show that this drawback can be circumvented by enzyme‐assisted self‐assembly of peptides initiated at the walls of a supporting porous material. We applied this strategy to grow an esterase‐like catalytically active supramolecular hydrogel (CASH) in an open‐cell polymer foam, filling the whole interior space. Our supported CASH material is highly efficient towards inactivated esters and enables the kinetic resolution of racemates. This hybrid material is robust enough to be used in continuous flow reactors, and is reusable and stable over months.

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Surface‐Assisted Self‐Assembly of a Hydrogel by Proton Diffusion

et al. 2018

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Controlling supramolecular growth at solid surfaces is of great importance to expand the scope of supramolecular materials. A dendritic benzene‐1,3,5‐tricarboxamide peptide conjugate is described in which assembly can be triggered by a pH jump. Stopped‐flow kinetics and mathematical modeling provide a quantitative understanding of the nucleation, elongation, and fragmentation behavior in solution. To assemble the molecule at a solid–liquid interface, we use proton diffusion from the bulk. The latter needs to be slower than the lag phase of nucleation to progressively grow a hydrogel outwards from the surface. Our method of surface‐assisted self‐assembly is generally applicable to other gelators, and can be used to create structured supramolecular materials.

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Oberflächenunterstützte Selbstorganisationsstrategien für supramolekulare Hydrogele

Cited by 12 publications

References 60 publications

Enzymatic Noncovalent Synthesis

Enzymatic Noncovalent Synthesis

Supported Catalytically Active Supramolecular Hydrogels for Continuous Flow Chemistry

Surface‐Assisted Self‐Assembly of a Hydrogel by Proton Diffusion

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