Hierarchical Assembly of Complex Block Copolymer Nanoparticles into Multicompartment Superstructures through Tunable Interparticle Associations

Zhu, Jiahua; Zhang, Shiyi; Zhang, Fuwu; Wooley, Karen L.; Pochan, Darrin J.

doi:10.1002/adfm.201202323

Cited by 69 publications

(63 citation statements)

References 53 publications

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“…The ability to kinetically trap block copolymers into nanoparticles and observe local equilibration within the particles provides an excellent opportunity to construct complex, multi-component nano-objects for multifunctional, hierarchical materials 18,19 . In single diblock copolymer solution suspensions, assemblies with locally mixed geometries, for example, cylinders with sphere end-caps and Y-junctions between cylinders, have been found at relative block compositions that lie between molecular compositions that form traditional spheres and cylinders or cylinders and vesicles 20 .…”

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Disk-cylinder and disk-sphere nanoparticles via a block copolymer blend solution construction

et al. 2013

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Researchers strive to produce nanoparticles with complexity in composition and structure. Although traditional spherical, cylindrical and membranous, or planar, nanostructures are ubiquitous, scientists seek more complicated geometries for potential functionality. Here we report the simple solution construction of multigeometry nanoparticles, disk-sphere and diskcylinder, through a straightforward, molecular-level, blending strategy with binary mixtures of block copolymers. The multigeometry nanoparticles contain disk geometry in the core with either spherical patches along the disk periphery in the case of disk-sphere particles or cylindrical edges and handles in the case of the disk-cylinder particles. The portions of different geometry in the same nanoparticles contain different core block chemistry, thus also defining multicompartments in the nanoparticles. Although the block copolymers chosen for the blends are important for the definition of the final hybrid particles, the control of the kinetic pathway of assembly is critical for successful multigeometry particle construction.

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Disk-cylinder and disk-sphere nanoparticles via a block copolymer blend solution construction

et al. 2013

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“…Laboratory-based synthetic approaches are now beginning to reach similar levels of exquisite control in the creation of nanoscale and mesoscale architectures [1][2][3][4][5] , using well-defined nanomaterials as building blocks. For example, a variety of supramolecular structures have been formed through the secondary association of various organic building blocks 6 including block copolymer (BCP) micelles [7][8][9][10][11][12] . Higher order structures have also been formed by the self-assembly of inorganic nanoparticles (NPs), including particles with different but complementary shapes, and rod-like particles coated at the ends with DNA or synthetic polymers [13][14][15][16][17] .…”

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A design strategy for the hierarchical fabrication of colloidal hybrid mesostructures

et al. 2014

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Advances in nanotechnology depend upon expanding the ability to create new and complex materials with well-defined multidimensional mesoscale structures. The creation of hybrid hierarchical structures by combining colloidal organic and inorganic building blocks remains a challenge due to the difficulty in preparing organic structural units of precise size and shape. Here we describe a design strategy to generate controlled hierarchical organic-inorganic hybrid architectures by multistep bottom-up self-assembly. Starting with a suspension of large inorganic nanoparticles, we anchor uniform block copolymer crystallites onto the nanoparticle surface. These colloidally stable multi-component particles can initiate the living growth of uniform cylindrical micelles from their surface, leading to three-dimensional architectures. Structures of greater complexity can be obtained by extending the micelles via addition of a second core-crystalline block copolymer. This controlled growth of polymer micelles from the surface of inorganic particles opens the door to the construction of previously inaccessible colloidal organic-inorganic hybrid structures.

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“…36,37 In our study, poly(acrylic acid) (PAA) was chosen as the hydrophilic block owing to the susceptibility of COOH groups to chemical modification. Poly ( n -butyl acrylate) (P n BA) was chosen as the hydrophobic block because of its low glass transition (−49 to −55 °C).…”

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Hyaluronic Acid-Based Hydrogels Containing Covalently Integrated Drug Depots: Implication for Controlling Inflammation in Mechanically Stressed Tissues

et al. 2013

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Synthetic hydrogels containing covalently-integrated soft and deformable drug depots capable of releasing therapeutic molecules in response to mechanical forces are attractive candidates for the treatment of degenerated tissues that are normally load bearing. Herein, radically crosslinkable block copolymer micelles (xBCM) assembled from an amphiphilic block copolymer consisting of hydrophilic poly(acrylic acid) (PAA) partially modified with 2-hydroxyethyl acrylate, and hydrophobic poly(n-butyl acryclate) (PnBA) were employed as the drug depots and the microscopic crosslinkers for the preparation of hyaluronic acid (HA)-based, hydrogels. HA hydrogels containing covalently integrated micelles (HAxBCM) were prepared by radical polymerization of glycidyl methacrylate (GMA)-modified HA (HAGMA) in the presence of xBCMs. When micelles prepared from the parent PAA-b-PnBA without any polymerizable double bonds were used, hydrogels containing physically entrapped micelles (HApBCM) were obtained. The addition of xBCMs to a HAGMA precursor solution accelerated the gelation kinetics and altered the hydrogel mechanical properties. The resultant HAxBCM gels exhibit an elastic modulus of 847 ± 43 Pa and a compressive modulus of 9.2 ± 0.7 kPa. Diffusion analysis of Nile Red (NR)-labeled xBCMs employing fluorescence correlation spectroscopy confirmed the covalent immobilization of xBCMs in HA networks. Covalent integration of dexamethasone (DEX)-loaded xBCMs in HA gels significantly reduced the initial burst release and provided sustained release over a prolonged period. Importantly, DEX release from HAxBCM gels was accelerated by intermittently-applied external compression in a strain-dependent manner. Culturing macrophages in the presence of DEX-releasing HAxBCM gels significantly reduced cellular production of inflammatory cytokines. Incorporating mechano-responsive modules in synthetic matrices offers a novel strategy to harvest mechanical stress present in the healing wounds to initiate tissue repair.

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Hierarchical Assembly of Complex Block Copolymer Nanoparticles into Multicompartment Superstructures through Tunable Interparticle Associations

Cited by 69 publications

References 53 publications

Disk-cylinder and disk-sphere nanoparticles via a block copolymer blend solution construction

Disk-cylinder and disk-sphere nanoparticles via a block copolymer blend solution construction

A design strategy for the hierarchical fabrication of colloidal hybrid mesostructures

Hyaluronic Acid-Based Hydrogels Containing Covalently Integrated Drug Depots: Implication for Controlling Inflammation in Mechanically Stressed Tissues

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