Programmed DNAzyme-Triggered Dissolution of DNA-Based. Hydrogels: Means for Controlled Release of Biocatalysts and for the Activation of Enzyme Cascades
Programmed DNAzyme-Triggered Dissolution of DNA-Based. Hydrogels: Means for Controlled Release of Biocatalysts and for the Activation of Enzyme Cascades
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DOI：
10.1021/acsami.5b02156
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发表时间：
2015-04-29
影响因子：
9.5
通讯作者：
Willner, Itamar
中科院分区：
文献类型：
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作者：
Lilienthal, Sivan;Shpilt, Zohar;Willner, Itamar
丙烯酰胺/丙烯酰胺修饰的核酸共聚物链为构建丙烯酰胺-DNA水凝胶提供了构建单元。通过将丙烯酰胺-DNA链与金属离子依赖的DNA酶序列及其底物进行交联，制备了三种不同的水凝胶。研究中使用的金属离子依赖的DNAzyme序列包括Cu2+依赖的DNAzyme、Mg2+依赖的DNAzyme和Zn2+依赖的DNAzyme。在各自的金属离子存在下，各自的DNAzyme的底物被切割，导致交联单元的分离和水凝胶的溶解。不同的水凝胶被负载了荧光团修饰的葡聚糖或荧光团功能化的葡萄糖氧化酶。用不同的离子处理不同的水凝胶会导致负载的葡聚糖或酶的释放，并且负载的大分子的释放速度顺序是Cu2+&Gt；Mg2+&Gt；Zn2+。此外，不同的水凝胶中负载了β-半乳糖苷酶(β-Gal)、葡萄糖氧化酶(GOx)或辣根过氧化物酶(HRP)。在适当的金属离子存在下，相应的水凝胶被溶解，导致B-Gal/Gox或Gox/HRP双酶级联和β-Gal/Gox/HRP三酶级联的激活。
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 Cu2+-, Mg2+-, and Zn2+-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 Cu2+ > Mg2+ > Zn2+. Also, the different hydrogels were loaded with the enzymes beta-galactosidase (beta-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 B-Gal/GOx or GOx/HRP bienzyme cascades and of the beta-Gal/GOx/HRP trienzyme cascade.