We report the self‐assembly and characterization of mesoporous silica thin films with a 3D ordered arrangement of isolated spherical pores. The preparation method was based on solvent‐evaporation induced self‐assembly (EISA), with MTES (CH3–Si(OCH2CH3)3) as the silica precursor and a polystyrene‐block‐poly(ethylene oxide) (PS‐b‐PEO) diblock copolymer as the structure‐directing agent. The synthetic approach was designed to suppress the siloxane condensation rate of the siloxane network, allowing co‐self‐assembly of the silica and the amphiphile, followed by retraction of the PEO chains from the silica matrix and matrix consolidation, to occur unimpeded. The calcined films retained the methyl ligands and exhibited no measurable microporosity, thereby indicating that the 3D‐ordered spherical mesopores are not interconnected. A solvent‐mediated formation mechanism is proposed for the absence of microporosity. Due to their closed porosity and hydrophobicity, the MTES‐based films and MTES‐TEOS (Si(OCH2CH3)4)‐based hybrid films we describe should be promising for applications such as low‐k dielectrics.
Scalable
synthesis of multicompartment polyion complex (PIC) systems has been
achieved via visible light-initiated RAFT polymerization of cationic
monomer in the presence of anionic diblock copolymer micelles in water
at 25 °C. This polymerization-induced hierarchical electrostatic
self-assembly (hierarchical PIESA) implements structural hierarchy
via programmable self-assembly to form multicompartment PIC micelles
and their monolayer colloidal nanosheets and nanocages. The anionic
micelles play decisive roles in such a hierarchical PIESA to access
biologically relevant yet otherwise inaccessible multicompartment
PIC systems.
We present a template strategy for precision synthesis of “complex coacervates-in-dodecyl atmosphere” ultrathin lamellae possessing exceptional shape-preservation and charge-tolerance properties.
Macromolecular crowding plays a key
role in liquid-phase condensation
of proteins and membraneless organelles yet is largely unexplored
for artificial liquid materials. Herein, we present a strategy for
direct access to multiphase liquid condensates with individual charged/neutral
subdomains, by introducing macromolecular crowding to our previous
protocol of liquid–liquid phase-separation-driven polymerization-induced
electrostatic self-assembly (LLPS-PIESA). We show that reversible
addition fragmentation chain transfer (RAFT) aqueous dispersion photo-copolymerization
of a charged monomer with a specific neutral monomer, in the presence
of a polar macrochain transfer agent (CTA) and an oppositely charged
polyion, can induce self-sorting and macromolecular crowding. LLPS-PIESA
proceeds via liquid-phase condensation of as-assembled nascent clusters
up to biologically important nanostructured multiphase condensates
with individual charged/neutral subdomains.
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