The commercially available 1,2-polybutadiene
(1,2-PB)
contains
highly reactive CC bonds and has excellent machinability,
which is an ideal raw material for preparing thermoplastic elastomers.
The preparation of supramolecular cross-linked 1,2-PB thermoplastic
elastomer with good recyclability and excellent mechanical properties
has promising applications. Here, the 1,2-PB elastomers (UPB elastomers)
were prepared by conjugating a few percent 2-ureido-4[1H]-pyrimidinone (UPy) self-complementary quadruple hydrogen bonding
units onto the high molecular weight (M
n) 1,2-PB chains via the thiol-ene click reaction. The used 2-(mercaptoethyl-ureido)-pyrimidinone
derivative (UPy-SH) with a branched alkyl group had good compatibility
with 1,2-PB in organic solvent contributing to a high transparency
of recyclable UPB elastomers. The cross-linking density of UPB elastomers
can be conveniently adjusted by varying the UPy content, which ultimately
determined the mechanical properties of resulting supramolecular elastomers.
Abundant chain entanglements formed by 1,2-PB chains with a high M
n of 455 kDa and strong quadruple hydrogen bonding
networks formed by side UPy units endowed UPB elastomers with excellent
mechanical properties and damping properties. It was found that sample
UPB-2 containing 2 mol % UPy units showed a tensile strength of 13.4
MPa, a high elongation at break of 1167%, a high elastic recovery
of 89% (under large tensile deformation of 400%), a high peak tan
δ value (tan δmax) of 1.4, and an effective
damping temperature range width of 30.6 °C. Moreover, UPB elastomers
have good recyclability given the noncovalent cross-linking networks.
This effective and universal strategy provides some insights into
the design of physically cross-linked high-performance 1,2-polybutadiene
elastomers.