Abstract
A facile fabrication of spherical vesicles and micelles by acyclic diene metathesis (ADMET) polymerization and alternative metathesis polymerization (ALTMET) was investigated. We utilize fluorine (FL) and perylene diimide-based (PDI) α,ω-dienes and α,ω-diacrylates to provide a series of homopolymers and alternating copolymers. When using α,ω-dienes as model monomers, TEM measurement indicates that the aromatic FL and PDI building block induced polymers to generate medium-sized (30–50 nm and 90–120 nm, respectively) micelles and vesicles. It was amazing that alternating copolymers derived from PDI α,ω-dienes and FL α,ω-diacrylates spontaneously form giant vesicles with sizes in the range of 0.7 μm to 2.5 μm. The controlled self-assembly of the organic polymer mediated by ADMET and ALTMET techniques avoided extremely annoying post treatment. Therefore, this work establishes a new, versatile synthetic strategy to create nanoparticles having tunable morphologies with potential application as molecular payload delivery vehicles.
Highlights
During the past decades, advances in polymer synthesis and macromolecular conjugation reactions have led to progressively complex polymer compositions and architectures being accessible and versatile self-assembly techniques have emerged
We propose a facile one-pot approach to nanoparticle synthesis, acyclic diene metathesis (ADMET) and alternative metathesis polymerization (ALTMET) polymerizationinduced self-assembly using chemically and topologically de ned patterned monomers as shown in Scheme 1
In order to compare the effects of different aromatic groups on the assembly morphology, and consider the repeatability of the functionalization-induced self-assembly behavior, the perylene diimide-based (PDI)-functionalized a,u-diene monomer, M1 was resynthesized according to literature.[17]
Summary
Advances in polymer synthesis and macromolecular conjugation reactions have led to progressively complex polymer compositions and architectures being accessible and versatile self-assembly techniques have emerged. Polymerization induced self-assembly (PISA) is an emerging area that couples control of chain-growth and dynamic self-assembly morphological versatility, e.g., spherical, cylindrical, and vesicular nanomaterials.[1] for access to highly tailorable and readily available nanomaterials, complementary approaches to self-assembly are needed which offer broadened structural versatility to solvophobic blocks and which are value-added for the self-assembly of existing block copolymer substrates.[2,3,4,5] PISA is mostly constructed from polymers bearing amphiphilic AB diblocks or ABC triblocks, which requires tedious multistep syntheses and sometimes require the preparations of elaborately designed small molecules and solvent selectivity, and so forth.[6,7,8]. Acyclic diene metathesis (ADMET) polymerization, on the other hand, has been considered to be an efficient route for the construction of nanomaterials.
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