Concurrent Control over Sequence and Dispersity in Multiblock Copolymers
2020
Controlling
monomer sequence in synthetic macromolecules is a major challenge in polymer
science and the order of building blocks has already been demonstrated to
determine macromolecular folding, self-assembly and fundamental polymer
properties. Dispersity is another key parameter in material design, with both
low and high dispersity polymers displaying complementary properties and
functions. However, synthetic approaches that can simultaneously control both
sequence and dispersity remain experimentally unattainable. Here we report a simple,
one pot, and rapid synthesis of sequence-controlled multiblocks with on demand
control over dispersity while maintaining high livingness, excellent agreement
between theoretical and experimental molecular weights and quantitative yields.
Key to our approach is the regulation in chain transfer agent activity during
controlled radical polymerization that enables the preparation of multiblocks
with gradually ascending (Ɖ=1.16 →1.60),
descending (Ɖ=1.66 →1.22), alternating
low and high dispersity values (Ɖ=1.17
→1.61 →1.24 →1.70 →1.26) or any combination thereof. The enormous potential of
our methodology was further demonstrated through the impressive synthesis of
highly ordered pentablock, octablock and decablock copolymers yielding the first
generation of multiblocks with concurrent control over both sequence and
dispersity.
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