Nanofibrillar Peptide Hydrogels for the Immobilization of Biocatalysts for Chemical Transformations

Hickling, Christopher; Toogood, Helen S.; Saiani, Alberto; Scrutton, Nigel S.; Miller, Aline F.

doi:10.1002/marc.201400027

Cited by 17 publications

(11 citation statements)

References 54 publications

(85 reference statements)

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“…The hydrogel mimics the functions of the pancreas, revealing a concentrationdependent insulin release in response to glucose; an important attribute for glucose management in diabetes. It should be noted that numerous studies addressed the incorporation of enzymes in hydrogels as functional matrices for operating biotechnological applications 56 or sensing, 57 and enzymeloaded hydrogels were used as functional matrices for the biocatalysed, triggered degradation of the matrices and release of loads. 58 Nonetheless, the enzyme-loaded DNA-based hydrogels, where the biocatalysts are retained and caged in the hydrogels within the process of the biocatalytic control over the stiffness of the hydrogels (and the accompanying shape-memory/selfhealing events), are, to the best of our knowledge, unprecedented.…”

Section: Introductionmentioning

confidence: 99%

Biocatalytic reversible control of the stiffness of DNA-modified responsive hydrogels: applications in shape-memory, self-healing and autonomous controlled release of insulin

et al. 2020

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Section: Introductionmentioning

confidence: 99%

Biocatalytic reversible control of the stiffness of DNA-modified responsive hydrogels: applications in shape-memory, self-healing and autonomous controlled release of insulin

et al. 2020

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“…In order to avoid affecting the self-assembling properties of the peptides, their functionalization is usually achieved by linking the functionality to one of the peptide’s chain termini. 3 , 24 − 28 Here we are interested in looking at the possibility to functionalize the peptide fibrils through its hydrophobic face in order to bury the functionality in the hydrophobic core of the peptide fiber.…”

Section: Introductionmentioning

confidence: 99%

Modification of β-Sheet Forming Peptide Hydrophobic Face: Effect on Self-Assembly and Gelation

Elsawy¹,

Smith²,

Hodson³

et al. 2016

Langmuir

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β-Sheet forming peptides have attracted significant interest for the design of hydrogels for biomedical applications. One of the main challenges is the control and understanding of the correlations between peptide molecular structure, the morphology, and topology of the fiber and network formed as well as the macroscopic properties of the hydrogel obtained. In this work, we have investigated the effect that functionalizing these peptides through their hydrophobic face has on their self-assembly and gelation. Our results show that the modification of the hydrophobic face results in a partial loss of the extended β-sheet conformation of the peptide and a significant change in fiber morphology from straight to kinked. As a consequence, the ability of these fibers to associate along their length and form large bundles is reduced. These structural changes (fiber structure and network topology) significantly affect the mechanical properties of the hydrogels (shear modulus and elasticity).

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“…Hydrogel fibers have similar properties to the natural macromolecules in extracellular matrix (ECM) such as large surface area, high porosity, and high content of water. They have been applied in mimicking 3D ECM for tissue engineering, sensors, immobilizing biocatalysts, sustained releasing of proteins and drugs, and wound healing . Among three common ways of synthesizing fibers, self‐assembly, electrospinning and phase separation, electrospinning is the most versatile, simple and cost effective technique.…”

Section: Introductionmentioning

confidence: 99%

Bioinspired Metal Ion Coordinated Polyelectrolyte Fibrous Nanoreactors

Malhotra

Bera

Zhai

2016

Adv Materials Inter

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improve the stability of hydrogel fibers and introduce multiple functionality to hydrogel fibers.Hydrogel fibers have similar properties to the natural macromolecules in extracellular matrix (ECM) such as large surface area, high porosity, and high content of water. They have been applied in mimicking 3D ECM [28][29][30][31][32][33][34][35][36][37] for tissue engineering, sensors, [38,39] immobilizing biocatalysts, [40] sustained releasing of proteins and drugs, [41][42][43] and wound healing. [44][45][46] Among three common ways of synthesizing fibers, self-assembly, electrospinning and phase separation, electrospinning is the most versatile, simple and cost effective technique. However, the application of electrospun hydrogel fibers (EHFs) faces challenges of low stability in aqueous solutions, liability to harsh chemical conditions and limitations in further functionalization.The EHFs of one polyelectrolyte component are water soluble, all subsequent chemical reactions have to be performed under solvent-free conditions or in non-aqueous media. To stabilize fibrous hydrogels in aqueous media, thermal or vaporphase crosslinking is required which impedes their applications. Polyelectrolyte complexes have been used to improve the stability of fibrous hydrogels in aqueous solutions. [32,[47][48][49][50][51][52][53][54] A polyelectrolyte complex is formed by mixing oppositely charged polyelectrolytes such as poly(acrylic acid) (PAA) and poly(allyl amine hydrochloric acid) or PAA and chitosan (CS) in solutions with controlled polymer ratio and pH. The electrostatic interactions between partially charged polymeric chains lead to the formation of a polymer hydrogel network without covalent crosslinkers. [47][48][49][55][56][57] However, when exposed to solutions with high salt concentration and extreme pH, the disruption of the electrostatic interactions between polycations and polyanions results in the dissolution of the fibers.Functionalizing EHFs requires a simpler and more versatile method to introduce a variety of functional materials such as nanoparticles, peptides, polymers onto the fibers for various applications. Current approaches include in situ fabrication where nanoparticles or polymers/peptides are added to polymer solutions before electrospinning, and post fabrication where nanoparticles or polymers/peptides are introduced onto fibers via reactions in solutions. Post fabrication approaches are not sufficient in obtaining uniform and controlled functionalization in large scale while the amount of nanoparticles in fibers is limited by the dispersity of nanoparticles in polymer solutions in preloading fabrication approaches. [58][59][60] Therefore, Inspired by natural metal ion/ligand interactions, stable electrospun hydrogel fibers (EHFs) are produced from polyelectrolyte complexes coordinated with various metal ions. This development provides a novel and promising approach to advance hydrogel fiber applications by creating fibers with high stability in solutions and controlled interfacial reactions. The e...

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Nanofibrillar Peptide Hydrogels for the Immobilization of Biocatalysts for Chemical Transformations

Cited by 17 publications

References 54 publications

Biocatalytic reversible control of the stiffness of DNA-modified responsive hydrogels: applications in shape-memory, self-healing and autonomous controlled release of insulin

Biocatalytic reversible control of the stiffness of DNA-modified responsive hydrogels: applications in shape-memory, self-healing and autonomous controlled release of insulin

Modification of β-Sheet Forming Peptide Hydrophobic Face: Effect on Self-Assembly and Gelation

Bioinspired Metal Ion Coordinated Polyelectrolyte Fibrous Nanoreactors

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