Adenosine Triphosphate-Triggered Release of Macromolecular and Nanoparticle Loads from Aptamer/DNA-Cross-Linked Microcapsules.

The synthesis of stimuli-responsive DNA microcapsules acting as carriers for different payloads, and being dissociated through the formation of aptamer-ligand complexes is described. Specifically, stimuli-responsive anti-adenosine triphosphate (ATP) aptamer-cross-linked DNA-stabilized microcapsules loaded with tetramethylrhodamine-modified dextran (TMR-D), CdSe/ZnS quantum dots (QDs), or microperoxidase-11 (MP-11) are presented. In the presence of ATP as trigger, the microcapsules are dissociated through the formation of aptamer-ATP complexes, resulting in the release of the respective loads. Selective unlocking of the capsules is demonstrated, and CTP, GTP, or TTP do not unlock the pores. The ATP-triggered release of MP-11 from the microcapsules enables the MP-11-catalyzed oxidation of Amplex UltraRed by H2O2 to the fluorescent product resorufin.

[1]  Zonghuan Lu,et al.  Magnetic switch of permeability for polyelectrolyte microcapsules embedded with Co@Au nanoparticles. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[2]  W. Parak,et al.  Synthesis and characterization of ratiometric ion-sensitive polyelectrolyte capsules. , 2011, Small.

[3]  Changyou Gao,et al.  Molecular-engineered polymeric microcapsules assembled from Concanavalin A and glycogen with specific responses to carbohydrates , 2011 .

[4]  G. Boyle,et al.  The Oligomycin Axis of Mitochondrial ATP Synthase: OSCP and the Proton Channel , 2000, Journal of bioenergetics and biomembranes.

[5]  Wolfgang J Parak,et al.  Laser-induced release of encapsulated materials inside living cells. , 2006, Angewandte Chemie.

[6]  Wolfgang J. Parak,et al.  Synthesis and evaluation of gold nanoparticle-modified polyelectrolyte capsules under microwave irradiation for remotely controlled release for cargo , 2011 .

[7]  M. DeRosa,et al.  Target-molecule-triggered rupture of aptamer-encapsulated polyelectrolyte microcapsules. , 2013, ACS applied materials & interfaces.

[8]  H. Möhwald,et al.  Polyelectrolyte multilayer capsule permeability control , 2002 .

[9]  Benno Radt,et al.  Optically Addressable Nanostructured Capsules , 2004 .

[10]  Itamar Willner,et al.  DNA switches: from principles to applications. , 2015, Angewandte Chemie.

[11]  F. Caruso,et al.  DNA multilayer films on planar and colloidal supports: sequential assembly of like-charged polyelectrolytes. , 2005, Nano letters.

[12]  F. Caruso,et al.  Biodegradable click capsules with engineered drug-loaded multilayers. , 2010, ACS nano.

[13]  F. Caruso,et al.  Modular assembly of layer-by-layer capsules with tailored degradation profiles. , 2011, Langmuir : the ACS journal of surfaces and colloids.

[14]  Functionalization of Calcium Carbonate Microparticles as a Combined Sensor and Transport System for Active Agents in Cells , 2011, Journal of biomaterials science. Polymer edition.

[15]  Y. Lvov,et al.  Nanoshells for Drug Delivery , 2007 .

[16]  Gleb B. Sukhorukov,et al.  Ultrasound stimulated release and catalysis using polyelectrolyte multilayer capsules , 2007 .

[17]  P. Hammond,et al.  Tuning the Glass Transition of and Ion Transport within Hydrogen-Bonded Layer-by-Layer Assemblies , 2007 .

[18]  Itamar Willner,et al.  Electronic aptamer-based sensors. , 2007, Angewandte Chemie.

[19]  Gleb B. Sukhorukov,et al.  Intracellularly Degradable Polyelectrolyte Microcapsules , 2006 .

[20]  Itamar Willner,et al.  Aptamer-DNAzyme hairpins for amplified biosensing. , 2009, Analytical chemistry.

[21]  Caruso,et al.  Nanoengineering of inorganic and hybrid hollow spheres by colloidal templating , 1998, Science.

[22]  Michael F. Rubner,et al.  pH-Dependent Thickness Behavior of Sequentially Adsorbed Layers of Weak Polyelectrolytes , 2000 .

[23]  Helmuth Möhwald,et al.  Electrostatic Self-Assembly of Silica Nanoparticle−Polyelectrolyte Multilayers on Polystyrene Latex Particles , 1998 .

[24]  I. Willner,et al.  Biocatalytic release of an anticancer drug from nucleic-acids-capped mesoporous SiO2 Using DNA or molecular biomarkers as triggering stimuli. , 2013, ACS nano.

[25]  E. Shchukina,et al.  LbL coated microcapsules for delivering lipid-based drugs. , 2011, Advanced drug delivery reviews.

[26]  Frank Caruso,et al.  Controlled degradation of DNA capsules with engineered restriction-enzyme cut sites. , 2009, Small.

[27]  Dieter Braun,et al.  The role of metal nanoparticles in remote release of encapsulated materials. , 2005, Nano letters.

[28]  A. Duncan,et al.  Overexpression of a transporter gene in a multidrug-resistant human lung cancer cell line. , 1992, Science.

[29]  Michelle Prevot,et al.  Matrix polyelectrolyte microcapsules: new system for macromolecule encapsulation. , 2004, Langmuir : the ACS journal of surfaces and colloids.

[30]  Helmuth Möhwald,et al.  Assembly, structural characterization, and thermal behavior of layer-by-layer deposited ultrathin films of poly(vinyl sulfate) and poly(allylamine) , 1993 .

[31]  F. Caruso,et al.  Redox-active polymer microcapsules for the delivery of a survivin-specific siRNA in prostate cancer cells. , 2011, ACS nano.

[32]  M. Antonietti,et al.  CO2-switchable oligoamine patches based on amino acids and their use to build polyelectrolyte containers with intelligent gating. , 2008, Soft matter.

[33]  F. Caruso,et al.  Tuning the formation and degradation of layer-by-layer assembled polymer hydrogel microcapsules. , 2009, Langmuir : the ACS journal of surfaces and colloids.

[34]  G. Sukhorukov,et al.  Real-time assessment of spatial and temporal coupled catalysis within polyelectrolyte microcapsules containing coimmobilized glucose oxidase and peroxidase. , 2006, Biomacromolecules.

[35]  Xiaoling Zhang,et al.  An aptamer cross-linked hydrogel as a colorimetric platform for visual detection. , 2010, Angewandte Chemie.

[36]  A. Yashchenok,et al.  Encapsulation, Release and Applications of LbL Polyelectrolyte Multilayer Capsules , 2012 .

[37]  F. Caruso,et al.  Compositional and structural engineering of DNA multilayer films. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[38]  Wolfgang J Parak,et al.  Multiplexed sensing of ions with barcoded polyelectrolyte capsules. , 2011, ACS nano.

[39]  P. Bates,et al.  Antiproliferative Activity of G-rich Oligonucleotides Correlates with Protein Binding* , 1999, The Journal of Biological Chemistry.

[40]  Itamar Willner,et al.  Smart mesoporous SiO2 nanoparticles for the DNAzyme-induced multiplexed release of substrates. , 2013, Journal of the American Chemical Society.

[41]  M. Mascini,et al.  Analytical applications of aptamers. , 2005, Biosensors & bioelectronics.

[42]  Ioanis Katakis,et al.  Aptamers: molecular tools for analytical applications , 2008, Analytical and bioanalytical chemistry.

[43]  Qing Zhao,et al.  Cytochrome c acts as a cardiolipin oxygenase required for release of proapoptotic factors , 2005, Nature chemical biology.

[44]  Juewen Liu,et al.  Functional nucleic acid sensors. , 2009, Chemical reviews.

[45]  Raimo Hartmann,et al.  Magnetically triggered release of molecular cargo from iron oxide nanoparticle loaded microcapsules. , 2015, Nanoscale.

[46]  S. Verma,et al.  Sunlight mediated disruption of peptide-based soft structures decorated with gold nanoparticles. , 2010, Chemical communications.

[47]  Hua Ai Layer-by-layer capsules for magnetic resonance imaging and drug delivery. , 2011, Advanced drug delivery reviews.

[48]  F. Caruso,et al.  Stabilization and Functionalization of Polymer Multilayers and Capsules via Thiol-Ene Click Chemistry , 2009 .

[49]  F. Caruso,et al.  Manipulating the salt and thermal stability of DNA multilayer films via oligonucleotide length. , 2008, Biomacromolecules.

[50]  Benno Radt,et al.  Light-responsive polyelectrolyte/gold nanoparticle microcapsules. , 2005, The journal of physical chemistry. B.

[51]  Jennifer I. L. Chen,et al.  Morphology-based plasmonic nanoparticle sensors: controlling etching kinetics with target-responsive permeability gate. , 2013, Journal of the American Chemical Society.

[52]  G. Khomutov,et al.  Nanocomposite Microcontainers with High Ultrasound Sensitivity , 2010 .

[53]  J. Graves,et al.  Controlled protein release from microcapsules with composite shells using high frequency ultrasound—potential for in vivo medical use , 2011 .

[54]  Nicholas A Kotov,et al.  Ultrasound-triggered release from multilayered capsules. , 2007, Small.

[55]  G. Sukhorukov,et al.  Polymer Microcapsules with Carbohydrate‐Sensitive Properties , 2008 .

[56]  G. Sukhorukov,et al.  Polyelectrolyte Multilayer Microspheres as Carriers for Bienzyme System: Preparation and Characterization , 2005 .

[57]  Jiafu Shi,et al.  Design and Synthesis of Organic—Inorganic Hybrid Capsules for Biotechnological Applications , 2014 .

[58]  Wolfgang J Parak,et al.  Intracellular processing of proteins mediated by biodegradable polyelectrolyte capsules. , 2009, Nano letters.

[59]  Changyou Gao,et al.  Layer‐by‐Layer Assembly of Microcapsules and Their Biomedical Applications , 2012 .

[60]  Lars Dähne,et al.  Tailor-made polyelectrolyte microcapsules: from multilayers to smart containers. , 2004, Angewandte Chemie.

[61]  Kevin Braeckmans,et al.  Light-addressable capsules as caged compound matrix for controlled triggering of cytosolic reactions. , 2013, Angewandte Chemie.

[62]  M. DeRosa,et al.  Target binding influences permeability in aptamer-polyelectrolyte microcapsules. , 2011, Small.

[63]  Helmuth Möhwald,et al.  Novel Hollow Polymer Shells by Colloid-Templated Assembly of Polyelectrolytes. , 1998, Angewandte Chemie.

[64]  T. Maruyama,et al.  Cross-linked DNA capsules templated on porous calcium carbonate microparticles , 2010 .

[65]  Sensitive and visual detection of adenosine by a rationally designed FokI-based biosensing strategy. , 2009, Chemistry, an Asian journal.

[66]  F. Caruso,et al.  Degradable polyelectrolyte capsules filled with oligonucleotide sequences. , 2006, Angewandte Chemie.