title: Programmed DNAzyme-Triggered Dissolution of DNA-Based Hydrogels: Means for Controlled Release of Biocatalysts and for the Activation of Enzyme Cascades.
abstract: Acrylamide/acrylamide-modified nucleic acid copolymer chains provide building units for the construction of acrylamide-DNA hydrogels. Three different hydrogels are prepared by the cross-linking of the acrylamide-DNA chains with metal ion-dependent DNAzyme sequences and their substrates. The metal ion-dependent DNAzyme sequences used in the study include the Cu(2+)-, Mg(2+)-, and Zn(2+)-dependent DNAzymes. In the presence of the respective metal ions, the substrates of the respective DNAzymes are cleaved, leading to the separation of the cross-linking units and to the dissolution of the hydrogel. The different hydrogels were loaded with a fluorophore-modified dextran or with a fluorophore-functionalized glucose oxidase. Treatment of the different hydrogels with the respective ions led to the release of the loaded dextran or the enzyme, and the rates of releasing of the loaded macromolecules followed the order of Cu(2+) > Mg(2+) > Zn(2+). Also, the different hydrogels were loaded with the enzymes β-galactosidase (β-Gal), glucose oxidase (GOx), or horseradish peroxidase (HRP). In the presence of the appropriate metal ions, the respective hydrogels were dissolved, resulting in the activation of the β-Gal/GOx or GOx/HRP bienzyme cascades and of the β-Gal/GOx/HRP trienzyme cascade.
authors.affiliation: Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
authors.forename: Sivan
authors.initials: S
authors.lastname: Lilienthal
authors.affiliation: Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
authors.forename: Zohar
authors.initials: Z
authors.lastname: Shpilt
authors.affiliation: Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
authors.forename: Fuan
authors.initials: F
authors.lastname: Wang
authors.affiliation: Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
authors.forename: Ron
authors.initials: R
authors.lastname: Orbach
authors.affiliation: Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
authors.forename: Itamar
authors.initials: I
authors.lastname: Willner
mesh_terms: D020106:Acrylamide; D055162:Biocatalysis; D004247:DNA / Q000737:chemistry*; D021881:DNA, Catalytic / Q000378:metabolism*; D003911:Dextrans / Q000737:chemistry; D004789:Enzyme Activation; D005456:Fluorescent Dyes; D005949:Glucose Oxidase / Q000378:metabolism*; D006735:Horseradish Peroxidase / Q000378:metabolism*; D020100:Hydrogels / Q000737:chemistry*; D012212:Rheology; D012235:Rhodamines / Q000737:chemistry; D013997:Time Factors
chemical_list: D021881:DNA, Catalytic; D003911:Dextrans; D005456:Fluorescent Dyes; D020100:Hydrogels; D012235:Rhodamines; D020106:Acrylamide; C005358:tetramethylrhodamine; D004247:DNA; D005949:Glucose Oxidase; D006735:Horseradish Peroxidase
keywords: acrylamide; metal ion; polymer; responsive; switch