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

Wang, Chen; Fischer, Amit; Ehrlich, Avner; Nahmias, Yaakov; Willner, Itamar

doi:10.1039/d0sc01319f

Cited by 38 publications

(37 citation statements)

References 64 publications

(70 reference statements)

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“…[10][11][12][13][14][15] Indeed, the co-immobilization of cascade enzymes on a platform is one of the most straightforward protocols to mimic sequential enzyme reactions. [16][17][18][19] However, random enzyme distribution in traditional approaches brought many challenges such as the overlap of enzyme active sites, mismatch of the optimal enzyme ratio and inappropriate interenzyme distances, thereby leading to an inferior mass transport of reactants and intermediates among enzymes with signicantly reduced catalytic efficiency. Accordingly, besides the inherent catalytic activity, cascade enzymes with a rational spatial arrangement (e.g., enzyme spacing and ratio) are crucial to achieve highly efficient cascade catalysis, which has been the focus of researchers in recent years but remains challenging.…”

Section: Introductionmentioning

confidence: 99%

A DNA nanopillar as a scaffold to regulate the ratio and distance of mimic enzymes for an efficient cascade catalytic platform

Kou

Yuan

2021

Chem. Sci.

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Section: Introductionmentioning

confidence: 99%

A DNA nanopillar as a scaffold to regulate the ratio and distance of mimic enzymes for an efficient cascade catalytic platform

Kou

Yuan

2021

Chem. Sci.

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“…An ideal self-modulated insulin drug delivery system requires glucose-sensing ability and an automatic shut-off mechanism. The biocatalytic transformations of glucose oxidase included within the pH-responsive DNA containing hydrogels provides a glucose-triggered matrix for the controlled release of insulin and therefore behaves as an artificial pancreas [ 37 ]. The cationic natural polymer oligochitosan and Ca 2+ were allowed to cross-link with pectin to form hydrogel microcarriers to deliver the drug slowly in the upper gastrointestinal tract and rapid release of drug simulated physiological conditions of the colon [ 38 ].…”

Section: Stimuli-sensitive Hydrogelsmentioning

confidence: 99%

Emerging Role of Hydrogels in Drug Delivery Systems, Tissue Engineering and Wound Management

et al. 2021

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The popularity of hydrogels as biomaterials lies in their tunable physical properties, ability to encapsulate small molecules and macromolecular drugs, water holding capacity, flexibility, and controllable degradability. Functionalization strategies to overcome the deficiencies of conventional hydrogels and expand the role of advanced hydrogels such as DNA hydrogels are extensively discussed in this review. Different types of cross-linking techniques, materials utilized, procedures, advantages, and disadvantages covering hydrogels are tabulated. The application of hydrogels, particularly in buccal, oral, vaginal, and transdermal drug delivery systems, are described. The review also focuses on composite hydrogels with enhanced properties that are being developed to meet the diverse demand of wound dressing materials. The unique advantages of hydrogel nanoparticles in targeted and intracellular delivery of various therapeutic agents are explained. Furthermore, different types of hydrogel-based materials utilized for tissue engineering applications and fabrication of contact lens are discussed. The article also provides an overview of selected examples of commercial products launched particularly in the area of oral and ocular drug delivery systems and wound dressing materials. Hydrogels can be prepared with a wide variety of properties, achieving biostable, bioresorbable, and biodegradable polymer matrices, whose mechanical properties and degree of swelling are tailored with a specific application. These unique features give them a promising future in the fields of drug delivery systems and applied biomedicine.

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“…[23][24][25][26][27] The precise implementation of such functionalities is pivotal to designing the next generation of adaptive and interactive materials capable of autonomous and life-like behavior. 28 Indeed, current materials with DNA connecting motifs show increasingly advanced properties for applications as soft robotics, [29][30] therapeutic and cell culture hydrogels, [31][32][33][34] programmable fluorescent mechanosensing, 35 and materials responding to biological inputs. 36 However, a lack of large-scale synthetic access to oligonucleotide building blocks currently prevents widespread application of DNA materials.…”

Section: Introductionmentioning

confidence: 99%

Scalable One-Pot-Liquid-Phase Oligonucleotide Synthesis for Model Network Hydrogels

et al. 2020

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Solid-phase oligonucleotide synthesis (SPOS) based on phosphoramidite chemistry is currently the most widespread technique for DNA and RNA synthesis, but suffers from scalability limitations and high reagent consumption. Liquid-phase oligonucleotide synthesis (LPOS) uses soluble polymer supports and has the potential of being scalable. However, at present, LPOS requires 3 separate reaction steps and 4-5 precipitation steps per nucleotide addition. Moreover, long acid exposure times during the deprotection step degrade sequences with high A-content (adenine) due to depurination and chain cleavage. In this work, we present the first one-pot liquid-phase DNA synthesis technique, which allows the addition of one nucleotide in a one-pot reaction of sequential coupling, oxidation and deprotection, followed by a single precipitation step. Furthermore, we demonstrate how to suppress depurination during the addition of adenine nucleotides. We showcase the potential of this technique to prepare high-purity 4-arm PEG-T 20 (T = thymine) and 4-arm PEG-A 20 building blocks in multi-gram scale. Such complementary 4-arm PEG-DNA building blocks reversibly self-assemble into supramolecular model network hydrogels, and facilitate the elucidation of bond lifetimes. These model network hydrogels exhibit new levels of mechanical properties, high stability at room temperature (melting at 44 °C), and thus open up pathways to next-generation, scalable DNA-materials programmable through sequence recognition and available for macroscale applications. File list (2) download file view on ChemRxiv MS final.pdf (7.23 MiB) download file view on ChemRxiv ESI final.pdf (12.53 MiB)

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

Abstract: Biocatalytic control over the stiffness of pH-responsive hydrogels is applied to develop shape-memory, self-healing and controlled release matrices.

Cited by 38 publications

References 64 publications

A DNA nanopillar as a scaffold to regulate the ratio and distance of mimic enzymes for an efficient cascade catalytic platform

A DNA nanopillar as a scaffold to regulate the ratio and distance of mimic enzymes for an efficient cascade catalytic platform

Emerging Role of Hydrogels in Drug Delivery Systems, Tissue Engineering and Wound Management

Scalable One-Pot-Liquid-Phase Oligonucleotide Synthesis for Model Network Hydrogels

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