Hierarchic Nanostructure for Auto‐Modulation of Material Release: Mesoporous Nanocompartment Films

The preparation of mesoporous nanocompartment films composed of both hollow silica capsules and silica particles by using layer-by-layer (LbL) adsorption is described. The resultant nanocompartment films exhibit stepwise release of encapsulated water molecules without application of external stimuli. The hollow hierarchic pore structure of the silica capsules, including their internal void and mesoporous walls, is a key factor for the regulation and stepwise release of water, and is probably caused by the non-equilibrated concurrent evaporation of material from the mesopore and capillary penetration into the mesopores. The number of release steps and rate of release can be tuned by variation of several parameters including water content, ambient temperature, layer multiplicity, and co-adduct particle size. Application of the mesoporous nanocompartment films for the release of substances, including therapeutic agents and fragrances, indicates that the stepwise material release can be applied for a wide range of liquid substances. The films should lead to a novel material release system useful even for biomedical applications capable of controlled and sustained delivery of drug molecules.

[1]  Hsian-Rong Tseng,et al.  An operational supramolecular nanovalve. , 2004, Journal of the American Chemical Society.

[2]  B. Fang,et al.  Controllable synthesis of hierarchical nanostructured hollow core/mesopore shell carbon for electrochemical hydrogen storage. , 2008, Langmuir : the ACS journal of surfaces and colloids.

[3]  K. Ariga,et al.  Permeability controllable membranes. 11. Polymerized monolayers of single-, double-, and triple-chain silane amphiphiles and permeation control through the monolayer-immobilized porous glass plate in an aqueous solution. , 1989 .

[4]  Cari D. Pentecost,et al.  Construction of a pH-driven supramolecular nanovalve. , 2006, Organic letters.

[5]  K. Hidajat,et al.  pH-Controllable drug release using hydrogel encapsulated mesoporous silica. , 2007, Chemical communications.

[6]  B. Gaber,et al.  Thin film nanofabrication via layer-by-layer adsorption of tubule halloysite, spherical silica, proteins and polycations , 2002 .

[7]  Hsian-Rong Tseng,et al.  A reversible molecular valve. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[8]  María Vallet-Regí,et al.  Mesoporous materials for drug delivery. , 2007, Angewandte Chemie.

[9]  H. Möhwald,et al.  Sustained release properties of polyelectrolyte multilayer capsules. , 2001 .

[10]  Victor S-Y Lin,et al.  Mesoporous silica nanoparticle based controlled release, drug delivery, and biosensor systems. , 2007, Chemical communications.

[11]  Masahiro Fujiwara,et al.  Photocontrolled reversible release of guest molecules from coumarin-modified mesoporous silica , 2003, Nature.

[12]  K. Shakesheff,et al.  Polymeric systems for controlled drug release. , 1999, Chemical reviews.

[13]  G. Kwak,et al.  Nanoporous, Honeycomb-Structured Network Fibers Spun from Semiflexible, Ultrahigh Molecular Weight, Disubstituted Aromatic Polyacetylenes: Superhierarchical Structure and Unique Optical Anisotropy , 2006 .

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

[15]  R. Sijbesma,et al.  Hierarchical self-assembly of columnar aggregates. , 2005, Chemical Society reviews.

[16]  Ying Tian,et al.  Layer-by-layer assembly of magnetic polypeptide nanotubes as a DNA carrier , 2008 .

[17]  Yajun Wang,et al.  Templated synthesis of single-component polymer capsules and their application in drug delivery. , 2008, Nano letters.

[18]  Y. Arntz,et al.  Adenoviral Gene Delivery from Multilayered Polyelectrolyte Architectures , 2007 .

[19]  Janos H. Fendler,et al.  Self-Assembled Nanostructured Materials , 1996 .

[20]  Gero Decher,et al.  Fuzzy Nanoassemblies: Toward Layered Polymeric Multicomposites , 1997 .

[21]  Jayanth Panyam,et al.  Biodegradable nanoparticles for drug and gene delivery to cells and tissue. , 2003, Advanced drug delivery reviews.

[22]  Victor S-Y Lin,et al.  A mesoporous silica nanosphere-based carrier system with chemically removable CdS nanoparticle caps for stimuli-responsive controlled release of neurotransmitters and drug molecules. , 2003, Journal of the American Chemical Society.

[23]  Paula T Hammond,et al.  Electroactive controlled release thin films , 2008, Proceedings of the National Academy of Sciences.

[24]  J. F. Stoddart,et al.  pH-responsive supramolecular nanovalves based on cucurbit[6]uril pseudorotaxanes. , 2008, Angewandte Chemie.

[25]  A. Ajayaghosh,et al.  Organogels as scaffolds for excitation energy transfer and light harvesting. , 2008, Chemical Society reviews.

[26]  Yingchun Zhu,et al.  Installing dynamic molecular photomechanics in mesopores: a multifunctional controlled-release nanosystem. , 2007, Angewandte Chemie.

[27]  S. Rigby,et al.  Engineering silica particles as oral drug delivery vehicles. , 2008, Current pharmaceutical design.

[28]  K. Ariga,et al.  One-pot separation of tea components through selective adsorption on pore-engineered nanocarbon, carbon nanocage. , 2007, Journal of the American Chemical Society.

[29]  Gerhard Hummer,et al.  Osmotic water transport through carbon nanotube membranes , 2003, Proceedings of the National Academy of Sciences of the United States of America.

[30]  K. B. Yoon,et al.  Fabrication of bimodal porous silicate with silicalite-1 core/mesoporous shell structures and synthesis of nonspherical carbon and silica nanocases with hollow core/mesoporous shell structures. , 2005, The journal of physical chemistry. B.

[31]  Vladimir Torchilin,et al.  Stable nanocolloids of poorly soluble drugs with high drug content prepared using the combination of sonication and layer-by-layer technology. , 2008, Journal of controlled release : official journal of the Controlled Release Society.

[32]  K. Ariga.  Silica-supported biomimetic membranes. , 2004, Chemical record.

[33]  A. Loni,et al.  Mesoporous silicon: a platform for the delivery of therapeutics , 2007, Expert opinion on drug delivery.

[34]  K. Ren,et al.  Polyelectrolyte Multilayer Films of Controlled Stiffness Modulate Myoblast Cell Differentiation , 2008, Advanced functional materials.

[35]  P. Schaaf,et al.  Cell apoptosis control using BMP4 and noggin embedded in a polyelectrolyte multilayer film. , 2007, Small.

[36]  J. Salonen,et al.  Mesoporous silicon in drug delivery applications. , 2008, Journal of pharmaceutical sciences.

[37]  Katsuhiko Ariga,et al.  Layer-by-layer assembly as a versatile bottom-up nanofabrication technique for exploratory research and realistic application. , 2007, Physical chemistry chemical physics : PCCP.

[38]  Gleb B. Sukhorukov,et al.  Urease encapsulation in nanoorganized microshells. , 2001 .

[39]  C. Grigoropoulos,et al.  Fast Mass Transport Through Sub-2-Nanometer Carbon Nanotubes , 2006, Science.

[40]  M. Thommes,et al.  Pore condensation and critical-point shift of a fluid in controlled-pore glass , 1994 .

[41]  P. Schaaf,et al.  Polyelectrolyte multilayers with a tunable Young's modulus: influence of film stiffness on cell adhesion. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[42]  P. Hammond.  Form and Function in Multilayer Assembly: New Applications at the Nanoscale , 2004 .

[43]  R. Langer,et al.  Recent advances in pulmonary drug delivery using large, porous inhaled particles. , 1998, Journal of applied physiology.

[44]  Gérard Férey,et al.  Hybrid porous solids: past, present, future. , 2008, Chemical Society reviews.

[45]  X. Zhu,et al.  Polymer microspheres for controlled drug release. , 2004, International journal of pharmaceutics.

[46]  Katsuhiko Ariga,et al.  Biomaterials and biofunctionality in layered macromolecular assemblies. , 2008, Macromolecular bioscience.

[47]  Heinrich M. Jaeger,et al.  Hierarchical self-assembly of metal nanostructures on diblock copolymer scaffolds , 2001, Nature.

[48]  R. Langer,et al.  Drug delivery and targeting. , 1998, Nature.

[49]  K. Kataoka,et al.  Block copolymer micelles for drug delivery: design, characterization and biological significance. , 2001, Advanced drug delivery reviews.

[50]  Y. Lvov,et al.  Nano-engineered microcapsules of tannic acid and chitosan for protein encapsulation. , 2006, Journal of nanoscience and nanotechnology.

[51]  H. Hatori,et al.  Capillary condensation of water in the mesopores of nitrogen-enriched carbon aerogels , 2004 .

[52]  R. Martínez‐Máñez,et al.  New methods for anion recognition and signaling using nanoscopic gatelike scaffoldings. , 2006, Angewandte Chemie.

[53]  Dean-Mo Liu,et al.  Magnetic-sensitive silica nanospheres for controlled drug release. , 2008, Langmuir : the ACS journal of surfaces and colloids.

[54]  G. Chai,et al.  Synthesis of Ordered, Uniform, Macroporous Carbons with Mesoporous Walls Templated by Aggregates of Polystyrene Spheres and Silica Particles for Use as Catalyst Supports in Direct Methanol Fuel Cells , 2004 .

[55]  Y. Arntz,et al.  Composite multilayered biocompatible polyelectrolyte films with intact liposomes: stability and temperature triggered dye release. , 2007, Soft matter.

[56]  Frank Caruso,et al.  Template Synthesis of Nanostructured Materials via Layer-by-Layer Assembly† , 2008 .

[57]  Sang Cheon Lee,et al.  Controlled release of guest molecules from mesoporous silica particles based on a pH-responsive polypseudorotaxane motif. , 2007, Angewandte Chemie.

[58]  H. Möhwald,et al.  Self-assembly of human serum albumin (HSA) and L-alpha-dimyristoylphosphatidic acid (DMPA) microcapsules for controlled drug release. , 2004, Chemistry.

[59]  Michael S. Goldberg,et al.  Nanostructured materials for applications in drug delivery and tissue engineering , 2007, Journal of biomaterials science. Polymer edition.

[60]  George G. Guilbault,et al.  Commercial quartz crystal microbalances-Theory and applications , 1999 .

[61]  K. Ariga,et al.  Coordination chemistry and supramolecular chemistry in mesoporous nanospace , 2007 .

[62]  Jinsheng Zheng,et al.  Molecule-scale controlled-release system based on light-responsive silica nanoparticles. , 2008, Chemical communications.

[63]  Katsuhiko Ariga,et al.  Challenges and breakthroughs in recent research on self-assembly , 2008, Science and technology of advanced materials.

[64]  Gleb B Sukhorukov,et al.  Release mechanisms for polyelectrolyte capsules. , 2007, Chemical Society reviews.

[65]  Victor S-Y Lin,et al.  Stimuli-responsive controlled-release delivery system based on mesoporous silica nanorods capped with magnetic nanoparticles. , 2005, Angewandte Chemie.

[66]  D. M. Lynn,et al.  Ultrathin Multilayered Films Assembled from “Charge‐Shifting” Cationic Polymers: Extended, Long‐Term Release of Plasmid DNA from Surfaces , 2007 .

[67]  F. Xiao,et al.  pH-responsive carrier system based on carboxylic acid modified mesoporous silica and polyelectrolyte for drug delivery , 2005 .

[68]  O. Ikkala,et al.  Functional Materials Based on Self-Assembly of Polymeric Supramolecules , 2002, Science.

[69]  Wim E. Hennink,et al.  In vivo Cellular Uptake, Degradation, and Biocompatibility of Polyelectrolyte Microcapsules† , 2007 .

[70]  Katsuhiko Ariga,et al.  A layered mesoporous carbon sensor based on nanopore-filling cooperative adsorption in the liquid phase. , 2008, Angewandte Chemie.

[71]  K. Ariga,et al.  Permeation control by a phase transition of the dialkylsilane monolayer immobilized on a porous glass plate , 1986 .

[72]  J. Fraser Stoddart,et al.  Supramolecular nanovalves controlled by proton abstraction and competitive binding , 2006 .

[73]  Mauro Ferrari,et al.  Mesoporous silicon particles as a multistage delivery system for imaging and therapeutic applications. , 2008, Nature nanotechnology.

[74]  Brian G. Trewyn,et al.  Mesoporous Silica Nanoparticles for Drug Delivery and Biosensing Applications , 2007 .

[75]  P. Schaaf,et al.  Bioactive coatings based on polyelectrolyte multilayer architectures functionalized by embedded proteins, peptides or drugs. , 2007, Biomolecular engineering.

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

[77]  A. N. Semenov,et al.  Hierarchical self-assembly of chiral rod-like molecules as a model for peptide β-sheet tapes, ribbons, fibrils, and fibers , 2001, Proceedings of the National Academy of Sciences of the United States of America.

[78]  P. Hammond,et al.  Polyelectrolyte multilayers for tunable release of antibiotics. , 2008, Biomacromolecules.

[79]  Katsuhiko Ariga,et al.  Stimuli-free auto-modulated material release from mesoporous nanocompartment films. , 2008, Journal of the American Chemical Society.

[80]  C. Picart.  Polyelectrolyte multilayer films: from physico-chemical properties to the control of cellular processes. , 2008, Current medicinal chemistry.

[81]  K. Akagi.  Synthesis and properties of liquid-crystalline-conjugated polymers , 2007 .

[82]  R. Martínez‐Máñez,et al.  Photochemical and Chemical Two‐Channel Control of Functional Nanogated Hybrid Architectures , 2007 .

[83]  Z. Sideratou,et al.  Multifunctional dendritic drug delivery systems: design, synthesis, controlled and triggered release. , 2008, Current Topics in Medicinal Chemistry.

[84]  F. Caruso,et al.  A general approach for DNA encapsulation in degradable polymer microcapsules. , 2007, ACS nano.

[85]  D. M. Lynn,et al.  Multilayered polyelectrolyte assemblies as platforms for the delivery of DNA and other nucleic acid-based therapeutics. , 2008, Advanced drug delivery reviews.